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VOLUME 48
Editors
BENJAMIN BEDERSON
New York University
New York, New York
HERBERT WALTHER
Max-Plank-Institut j~ir Quantenoptik
Garching bei Miinchen
Germany
Editorial Board
ER. BERMAN
University of Michigan
Ann Arbor, Michigan
M. GAVRILA
EO.M. Instituut voor Atoom- en Molecuulfysica
Amsterdam, The Netherlands
M. INOKUTI
Argonne National Laboratory
Argonne, Illinois
CHUN C. LIN
University of Wisconsin
Madison, Wisconsin
Founding Editor
SIR DAVID BATES
Supplements
1. Atoms in Intense Laser Fields, Mihai Gavrila, Ed.
2. Cavity Quantum Electrodynamics, Paul R. Berman, Ed.
3. Cross Section Data, Mitio Inokuti, Ed.
A D VANCES IN
ATOMIC
MOLECOLAR
AND OPTICAL
PHYSICS
Edited by
Benjamin Bederson
DEPARTMENT OF PHYSICS
NEW YORK UNIVERSITY
NEW YORK, NEW YORK
Herbert Walther
UNIVERSITY OF MUNICH AND
MAX-PLANK INSTITUT FOR QUANTENOPTIK
MUNICH, GERMANY
Volume 4 8
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Contents
CONTRIBUTORS . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ix
INDEX . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 391
Numbers in parentheses indicate the pages on which the authors' contributions begin.
L.W. ANDERSON(357), Department of Physics, University of Wisconsin, Madi-
son, Wisconsin 53706
W. BECI~R (35), Max-Born-Institut, Max-Born-Str. 2A, 12489 Berlin, Germany
J.B. BOFFARD(357), Department of Physics, University of Wisconsin, Madison,
Wisconsin 53706
ROBERT N. COMPTON (219), Department of Chemistry, and Department of
Physics, University of Tennessee, Knoxville, Tennessee 37996
NIR DAVIDSON(99), Weizmann Institute of Science, Department of Physics of
Complex Systems, Rehovot, Israel
JOHANNES DENSCHLAG(263), Institut f'tir Experimentalphysik, Universitfit Inns-
bruck, 6020 Innsbruck, Austria
R. DORNER (1), Institut f'tir Kernphysik, August Euler Str. 6, 60486 Frankfurt,
Germany
P. FEN6 (357), Department of Physics, University of St. Thomas, St. Paul,
Minnesota 55105
RON FOEMAN (263), Physikalisches Institut, Universitfit Heidelberg, 69120
Heidelberg, Germany
NIR FRIEDMAN(99), Weizmann Institute of Science, Department of Physics of
Complex Systems, Rehovot, Israel
E G~SBON (35), Max-Planck-Institut f'tir Quantenoptik, Hans-Kopfermann-Str. 1,
85748 Garching, Germany
HARTMUT H~FFNER (191), Johannes Gutenberg University, Department of
Physics, 55099 Mainz, Germany
M. HATTASS(1), Institut f'tir Kernphysik, August Euler Str. 6, 60486 Frankfurt,
Germany
CARSTENHENKEL(263), Institut ffir Physik, Universit~it Potsdam, 14469 Potsdam,
Germany
WONHO JIqE (153), School of Physics and Center for Near-field Atom-photon
Technology, Seoul National University, Seoul 151-742, South Korea
x Contributors
M UL TIPL E IONIZATION IN
S TR ONG LASER FIELD S
R. DORNER*, Th. WEBER, M. WECKENBROCK, A. STAUDTE,
M. HATTASS and H. SCHMIDT-BOCKING
Institut fiir Kernphysik, August Euler Str. 6, 60486 Frankfurt, Germany
I. I n t r o d u c t i o n . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
II. C O L T R I M S - A C l o u d C h a m b e r for A t o m i c Physics ................... 3
III. Single I o n i z a t i o n and the Two-step M o d e l . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
IV. M e c h a n i s m s o f D o u b l e Ionization . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
V. Recoil Ion M o m e n t a . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
A. F r o m N o n s e q u e n t i a l to Sequential D o u b l e I o n i z a t i o n ................. 11
B. The Origin o f the Double Peak Structure . . . . . . . . . . . . . . . . . . . . . . . . . . 13
VI. Electron E n e r g i e s . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
VII. C o r r e l a t e d Electron M o m e n t a . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20
A. E x p e r i m e n t a l Findings ...................................... 20
B. C o m p a r i s o n to S i n g l e - P h o t o n and C h a r g e d Particle I m p a c t Double Ionization . 23
C. Interpretation within the R e s c a t t e r i n g M o d e l ....................... 25
D. S-Matrix C a l c u l a t i o n s . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 27
E. T i m e - d e p e n d e n t Calculations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28
VIII. Outlook . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 30
IX. A c k n o w l e d g m e n t s . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 30
X. R e f e r e n c e s ................................................ 31
I. I n t r o d u c t i o n
70 years ago Maria G6ppert-Mayer [ 1] showed that the energy of many photons
can be combined to achieve ionization in cases where the energy of one photon is
not sufficient to overcome the binding. Modern short-pulse Ti:Sa lasers (800 nm,
1.5 eV) routinely provide intensities of more than 1016 W/cm 2 and pulses shorter
than 100 femtoseconds. Under these conditions the ionization probability of most
atoms is close to unity. 1016 W/cm 2 corresponds to about 10 l~ coherent photons
in a box of the size of the wavelength (800nm). This extreme photon density
* E-mail: d o e r n e r @ h s b . u n i - f r a n k f u r t . d e
FIG. 1. Experimental setup. Electrons and ions are created in the supersonic gas-jet target. The thin
copper rings create a homogeneous electric field and the large Helmholtz coils an additional magnetic
field. These fields guide the charged particles onto fast time- and position-sensitive channel plate
detectors (Roentdek, www.roentdek.com). The time-of-flight (TOF) and the position of impact of
each electron-ion pair is recorded in list mode. From this the three-dimensional momentum vector
of each particle can be calculated.
easily reaches unity. Thus, within the reaction volume defined by the laser focus
of typically (10~m) 2 • 100~tm all atoms are ionized. Since for coincidence
experiments it is essential that much less than one atom is ionized per laser
shot, a background pressure of less than 10 -1~ mbar is required. The gas jet
has to be adjusted accordingly to reach single-collision conditions at the desired
laser peak power. With standard supersonic gas jets this can only be achieved
by tightly skimming the atomic beam, since a lower driving pressure for the
expansion would result in an increase of the internal temperature of the jet
along its direction of propagation. Single ionization (see Sect. III) allows for an
efficient monitoring of the resolution as well as on-line control of single-collision
conditions.
The ions created in the laser focus are guided by a weak electric field towards
a position-sensitive channel plate detector. From the position of impact and the
time-of-flight (TOF) of the ion all three components of the momentum vector and
the charge state are obtained. A typical ion TOF spectrum from the experiment
reported in ref. [17] is shown in Fig. 2.
The electric field also guides the electrons towards a second position-sensitive
channel plate detector. To collect electrons with large energies transverse to
the electric field a homogeneous magnetic field is superimposed parallel to
the electric field. This guides the electrons on cyclotron trajectories towards
the detector. Depending on their time-of-flight the electrons perform several
II] MULTIPLE IONIZATION IN STRONG LASER FIELDS 5
FIG. 2. Time-of-flight distribution of ions produced by a 6.6 x 1014 W/cm 2 laser pulse. The gas
target was 3He; the residual gas pressure in the chamber was about 2 x 10-l~ mbar. The double peak
structure in the 3He2+ peak can be seen. The total count rate was about 0.1 ion per laser shot.
FIG. 3. Horizontal axis: Electron time-of-flight. Vertical axis: radial distance from a central
trajectory with zero transverse momentum on electron detector, see text.
For all other TOFs the initial momentum can be uniquely calculated from the
measured positions of impact and the TOE Using a magnetic field of 10 Gauss,
4:r solid angle collection is achieved for electrons up to about 30 eV. The typical
detection probability of an electron is in the range o f 3 0 - 4 0 % . Thus, even for
double ionization in most cases only one electron is detected. The positions o f
impact and the times-of-flight are stored for each event in list mode. Thus the
whole experiment can be replayed in the off-line analysis. A detailed description
of the integrated multi-electron-ion m o m e n t u m spectrometer can be found in
ref. [ 18].
FIG. 5. Single ionization of argon by 3.8 • 1014W/cm2. The horizontal axis shows the momentum
component of the recoil ion parallel to the polarization. The vertical axis represents the momentum
of the coincident electron in the same direction. By momentum conservation all true coincidences
are located on the diagonal. Along the diagonal ATI peaks can be seen. The z-axis is plotted in
linear scale.
of the electron and ion m o m e n t u m measurement for the pz component (in this
case 0.25 au full width at half maximum). All events off the diagonal result from
false coincidences in which the electron and ion were created in the same pulse
but did not emerge from the same atom. This allows a continuous monitoring o f
the fraction o f false coincidences during the experiment. Knowing this number
the false coincidences can also be subtracted for double-ionization events.
For single-photon absorption the electron energy is uniquely determined by
the photon energy Ev and the binding energy plus a possible internal excitation
energy of the ion. The resulting narrow lines in the photoelectron energy
spectrum correspond to spheres in m o m e n t u m space. The left-hand panel of
Fig. 4 shows a slice through this m o m e n t u m sphere. The outer ring corresponds
to He 1+ ions in the ground state, the inner rings to the excited states. The
photons are linearly polarized with the polarization direction horizontal in the
figure. The angular distribution of the outer ring shows an almost pure dipole
distribution according to the absorption of one single photon. On the contrary,
in the laser field any number of photons can be absorbed, leading to an almost
continuous energy distribution o f the electrons (right-hand panel in Fig. 4).
Structure o f individual ATI (above threshold ionization) peaks spaced by the
8 R. D6rner et al. [III
photon energy (1.5 eV) is not seen here. This is in agreement with electron
spectra, where at comparable laser intensities ATI structure is not observed either.
The electrons and ions are emitted in narrow jets along the polarization axis.
Such high-angular-momentum states, needed to produce this kind of distribution,
are accessible due to the large number of photons absorbed.
How do the ions and electrons get their momenta? For the case of single-
photon absorption the light field is so weak that there is no acceleration. Also, the
photon carries no significant momentum into the reaction. The photon cuts the tie
between nucleus and electron by providing the energy. The momenta observed in
the final state thus have to be present already in the initial-state Compton profile
of the atom. Single-photon absorption is therefore linked to a particular fraction
of the initial-state wave function, which in momentum representation coincides
with the final-state momentum. The scaling of the photo ionization cross section
at high energies follows, besides a phase space factor, the initial-state momentum
space Compton profile, i.e. the probability to find an electron-ion pair with the
appropriate momentum in the initial state.
In the strong-field case the situation changes completely. The field is strong
enough to accelerate the ions and electrons substantially after the electron is set
free. The momentum balance, however, is still the same as in the single-photon
limit: The laser field accelerates electron and ion to the opposite directions
resulting again in their back-to-back emission (see Fig. 5). This changes only if
the laser pulse is long enough that the electron can escape from the focus during
the pulse. In that case, which we do not consider here, the momenta are balanced
by a huge amount of elastically scattered photons. In the regime of wavelength
and binding energies under consideration here, a simple two-step picture has
been proven useful. In the first step the electron is set free by tunneling through
the potential barrier created by the superposition of the Coulomb potential of
the atom and the electric field of the laser. This process promotes electrons and
ions with zero momentum to the continuum. Then they are accelerated in the
laser field and perform a quiver motion. In this model the net momentum in the
polarization direction, which is observed after a pulse with an envelope of the
electric field strength E(t) being long compared to the laser frequency, is purely
a function of the phase of the field at the instant of tunneling (tunneling time to):
Tunneling at the field maximum thus leads to electrons and ions with zero
momentum. The maximum momentum corresponding to the zero crossing of
the laser field is x/~Up, where Up = I/4~o 2 is the ponderomotive potential
at intensity I and photon frequency ~o (Up = 39.4eV at 6.6x1014W/cm2).
Within this simple model the ion and electron momentum detection provides
a measurement of the phase of the field at the instant of tunneling. We will
generalize this idea below for the case of double ionization.
IV] MULTIPLE IONIZATION IN STRONG LASER FIELDS 9
Single ionization is shown here mainly for illustration. Much more detailed
experiments have been reported using conventional TOF spectrometers (see ref.
[4] and references therein) and photoelectron imaging [19,20].
What are the "mechanisms" leading to double ionization? This seemingly clear-
cut question does not necessarily have a quantum-mechanical answer. The word
"mechanism" mostly refers to an intuitive mechanistical picture. It is not always
clear how this intuition can be translated into theory, and even if one finds
such a translation the contributions from different mechanisms have to be added
coherently to obtain the measurable final state of the reaction [21,22]. Thus, only
in some cases mechanisms are experimentally accessible. This is only the case
if different mechanisms occur at different strengths of the perturbation (such
as laser power or projectile charge) or if they predominantly populate different
regions of the final-state phase space. In these cases situations can be found
where one mechanism dominates such that interference becomes negligible. With
these words of caution in mind, we list the most discussed mechanisms leading
to double ionization:
(1) TS2 or Sequential Ionization: Here the two electrons are emitted
sequentially by two independent interactions of the laser field with the atom.
From a photon perspective one could say that each of the electrons absorbs
photons independently. From the field perspective one would say that each
electron tunnels independently at different times during the laser pulse.
This is equivalent to the TS2 (two-step-two) mechanism in ion-atom and
electron-atom collisions. In this approximation the probability of the double
ejection can be estimated in an independent-particle model. Most simply one
calculates double ionization as two independent steps of single ionization.
A somewhat more refined approach uses an independent-event model, which
takes into account the different binding energies for the ejection of the
first and the second electron (see, e.g., ref. [23] for ion impact, ref. [24] for
laser impact).
(2) Shake-Off: If one electron is removed rapidly (sudden approximation) from
an atom or a molecule, the wave function of the remaining electron has to
relax to the new eigenstates of the altered potential. Parts of these states
are in the continuum, so that a second electron can be "shaken off" in
this relaxation process. This is known for example from beta decay, where
the nuclear charge is changed. Shake-off is also known to be one of the
mechanisms for double ionization by absorption or Compton scattering of
a single photon (see the discussion in ref. [25] and references therein).
However, only for very high photon energies (in the keV range) it is
the dominating mechanism. For helium it leads to a ratio of double to
10 R. D 6 r n e r et al. [IV
V. Recoil Ion M o m e n t a
Recoil ion m o m e n t u m distributions have been measured for helium (He 1+,
He2+)[40], neon (Ne 1+, Ne 2+, Ne3+)[41] and argon (Ar l+, Ar2+)[45,46].
Figure 6 summarizes some of the results for neon. The m o m e n t u m distribution
of the singly charged ion is strongly peaked at the origin as in the case o f helium
(Fig. 4), reflecting the fact that tunnel ionization is most likely at the m a x i m u m
of the field (see Eq. 1). The structure o f the m o m e n t u m distribution of the doubly
charged ions changes strongly with the peak intensity. In the region where the
rates suggest the dominance of nonsequential ionization the ion momenta show
a distinct double peak structure (Fig. 6(2)). At higher intensities, where rates can
be described by assuming sequential ionization, the momenta o f the Ne 2+ ions
are peaked at the origin as for single ionization. The studies for helium show a
similar double peak structure at 6.6 x 1014 W/cm 2 (see Fig. 9).
The evolution of the ion momentum distributions with laser peak power has
been studied in detail for argon [46], too, confirming the fact that at the transition
to the nonsequential regime an increase in laser power results in colder ions. The
argon data, however, show no distinct double peak structure (see Fig. 7), where
the sequential ionization already sets in at about 6.6x 1014 W/cm 2. The reason
might be that the sequential contribution fills "the valley" in the m o m e n t u m
FIG. 6. Neon double ionization by 800 nm, 25 fs laser pulses. Left-hand panel: Rate of single and
double ionization as a function of the laser power (from ref. [47]). The solid line shows the rate
calculated in an independent event model. Right-hand panel: Recoil-ion momentum distributions
at intensities marked in the left-hand panel. A projection of the double-peaked distribution (2) is
shown in Fig. 10. Horizontal axis: Momentum component parallel to the electric field. Vertical axis:
One momentum component perpendicular to the field (data partially from ref. [41]).
12 R. D 6 r n e r et al. [V
(a)
~3
9;, /1: - \\
9 //" " \\ o,~
FIG. 7. Momentum distribution of Ar 2+ ions created in the focus of a 220 fs, 800 nm laser
pulse at peak intensities of (a) 3.75• l0 TMW/cm 2 and (b) 12• 1014 W/cm 2 in the direction of the
polarization. The distributions are integrated over the directions perpendicular to the polarization.
Solid circles: distribution of Ar 2+ ions; dotted line: distribution of Ar 1§ ions; dashed line: results of
the independent electron model of convoluting the Ar l+ distribution with itself; solid line: results
of the independent-electron ADK model (see text); open circles in (a): distribution of He 2+ ions at
3.8• l014 W/cm 2 (figure from ref. [46], helium data from ref. [40]).
judging from the rates, is in the sequential regime), this very simple approach
describes the ion momentum distributions in double ionization rather well. One
obvious oversimplification of this convolution procedure is that it implicitly
assumes that the momentum distributions do not change with binding energy.
A more refined independent-event approach would use different binding energies
for both steps. As an alternative simple model, the momentum distribution for
removal of the first electron and the second electron have been calculated in
the ADK (Ammosov-Delone-Krainov) model (see, e.g., ref. [48], Eq. 10) using
the correct binding energies for both steps. The result of convoluting these
two calculated distributions is shown by the solid lines in Fig. 7. Clearly such
modeling fails in the regime where sequential ionization dominates (Fig. 7a).
~tlt~
laser pulse as
He2+ ~t, 2
Pz (t~) = E ( t ) sin tot dt + 2 E ( t ) sin tot dt. (2)
2
The first electron is removed at time tl and the ion switches its charge from 1+
to 2+ at time tl 2. It is assumed that there is no momentum transfer to the ion
from the first emitted electron during double ionization. Thus, as in the case of
single ionization the phase of the field at the instant of the emission of the first
and of the second electron is encoded in the ion momentum.
Shake-off and TS2 will both lead to a momentum distribution peaked at zero,
similar to single ionization. In both cases the emission of the second electron
follows the first with a time delay, which is orders of magnitude shorter than
the laser period. Hence tl 2 = t~ in Eq. (2), and since the first electron is emitted
He2+
most likely at the field maximum Pz would also peak at zero for shake-off and
TS1. Consequently, the observed double peak structure for He and Ne directly
rules out these mechanisms.
For the rescattering there is a significant time delay between the emission of
the first electron and the return to its parent ion. Estimating tl 2 for a rescattering
trajectory which has sufficient energy to ionize leads to ion momenta close
to the measured peak positions [40,41,49]. The high momenta of the doubly
and triply charged ions are direct proof of the time delay introduced by the
rescattering trajectory. It is this time delay with respect to the field maximum
14 R. D 6 r n e r et al. [V
time
kb ka
{.
2 1
FIG. 8. Feynman diagram describing the rescattering and TS1 mechanism (from ref. [50]). See
text.
that is responsible for multiple ionization and allows an effective net momentum
transfer to the ion by accelerating the parent ion. Within the classical rescattering
model the final momentum of the doubly charged ion will be the momentum
received from the field (as given by Eq. 2) plus the momentum transfer from the
recolliding electron to the ion.
Soon after the measurement of the first ion momentum distributions Becker
and Faisal succeeded in the first theoretical prediction of this quantity. They
calculated double ionization of helium using (time-independent) S-matrix theory.
They evaluated the Feynman diagram shown in Fig. 8. Time progresses from
bottom to top. Starting with 2 electrons in the helium ground state at time ti, the
laser field couples once at tl to electron 1 (VATI). Electron 1 is then propagated
in a Volkov state (k) in the presence of the laser field, while electron 2 is
in the unperturbed He l+ ground state (j). Physically the Volkov electron does
not have a fixed energy but can pick up energy from the field. This describes
e.g. an acceleration of the electron in the field and its return to the ion. At
time t2 one interaction of the two electrons via the full Coulomb interaction
is included. This allows for an energy transfer from the Volkov electron to the
bound electron. Finally, both electrons are propagated independently in Volkov
states, describing their quiver motion in the field. By evaluating this diagram
Becker and Faisal obtained excellent agreement with the observed ion yields (see
ref. [51,52] for helium and ref. [53] for an approximated rate calculation on other
rare gases). The ion momentum distribution calculated as the sum momentum of
the two electrons predicted by this diagram is shown in Fig. 9b. The calculation
correctly predicts the double peak structure and the position of the maxima.
The minimum at momentum zero is more pronounced in the calculation than
in the data. The major approximations which might be responsible for this are:
Only one step of electron-electron energy transfer is taken into account (see
ref. [57] for a discussion of the importance of multiple steps); no intermediate
excited states are considered; and the laser field is neglected for all bound states
as in turn the Coulomb field is neglected in the continuum states. To unveil
the physical mechanism producing the double hump structure Becker and Faisal
V] MULTIPLE IONIZATION IN STRONG LASER FIELDS 15
I = 6 . 6 . 1 0 '4 W / c m 2
1.0 ' I ' I ' I ' I ' I ' I ' I ' ' I ' I ' I ' I ' I ' I ' i '
0.8 - a] i .. d]
o4 ,, J
o,~ ; ;
_.,.' ........ :. . . . .
9 ! 9 i 9 | - , - , 9 | 9 , - 9 | 9 | 9 | 9 | 9 | 9 | 9 ! 9
~" 0.8- b] _ I
-~ 0.6 , ,
~z 0,4 i
"- 0.2
_ , ~ . , . , . , .~,m .
' I ! I ' I ' i | i , I ' i ' 9 | ' | ' i 9 | 9 ! 9 ! 9 | 9
c] .. f]
0,8-
0,6-
.. ;% ;I
0,4-
L"
0 , 2 -/
0,0 l , a , I , , I ___ , I , I , I , L . I , i
-8 -6 -4 -2 0 2 4 6 -6 -4 -2 0 2 4 6 8
Prz [a.u.]
have evaluated the diagram also by replacing the final Volkov states by plane
waves. Physically this corresponds to switching off the laser field after both
electrons are in the continuum. In the calculation this led to a collapse of the
double peak structure to a single peak similar to single ionization. This confirms
our interpretation given above, that it is the acceleration of the ion in the field
after the rescattering (starting at tl 2 in Eq. 2) that leads to the high momenta.
The S-matrix theory also yielded good agreement with the observed narrow
momentum distribution in the direction perpendicular to the laser field.
Later, different approximations in the evaluation of the diagram (Fig. 8) have
been introduced. First, Kopold and coworkers [58] replaced the electron-electron
interaction by a contact potential and additionally used a zero-range potential
for the initial state. This simplified the computation considerably while still
yielding the observed double peak structure, not only for helium but also for neon
16 R. D 6 r n e r et al. [V
1.0
0.2
O.8
-- 0.6
8 - 1 0 ~4 W / c ~
0,4
o
0,2
c)
0,8
0.6
13" 10~4W/crn:
0,4
0,2
0.0
-8 -6 -4 -2 0 2 4 6 8
Prz (a.u.)
FIc. 10. Momentum distribution ofNe2+: (a) projection of data in Fig. 6 (2) at 13• 1014 W/cm 2
(from Moshammer et al. [41]); (b) S-matrix calculation evaluating the diagram in Fig. 8 with
contact potentials at 8• W/cm 2 (from Kopold et al. [58]); (c) Wannier-type calculation at
13• 1014 W/cm 2 (from Sacha and Eckhardt [56]).
(Fig. 10b) and other rare gases. They found that the inclusion of intermediate
excited states of the singly charged ion yields a filling of the minimum at zero
momentum.
Goreslavskii and Popruzhenko [54,59] used the saddle-point approximation
for the intermediate step. This additional approximation did not change the
calculated ion momenta strongly (see Fig. 9c) but simplified the computation,
allowing to investigate also the correlated electron emission discussed in the next
section.
A conceptionally very different approach was used by Sacha and Eck-
hardt[56]. They argued that the rescattering will produce a highly excited
intermediate complex, which will then decay in the presence of the field.
This decay process will not have any memory of how it was created. They
assumed a certain excitation energy as free parameter in the calculations and then
propagated both electrons in the classical laser field semiclassically in reduced
dimensions. Therefore they analyzed this decay by a Wannier-type analysis.
Wannier theory is known to reproduce the electron angular dependence as well
as the recoil ion momenta for the case of single-photon double ionization [60-
62,25]. In this case the Wannier configuration would be the emission of both
V] MULTIPLE IONIZATION IN STRONG LASER FIELDS 17
electrons back-to-back, leaving the recoil ion at rest on the saddle of the electron-
electron potential. For single-photon absorption from an S state this configuration
is forbidden by selection rules; it would allow, however, the absorption of an even
number of photons.
In the multiphoton case the external field has to be included in addition
to the Coulomb potential among the particles. This leads to a saddle in the
potential, which is not at rest at the center between the electrons but at
momenta which correspond to the observed peaks. Sacha and Eckhardt analyzed
classical trajectories in the saddle potential created by the field and the Coulomb
potentials. At a given laser field the decay of the excited complex in the field is
characterized only by two parameters: The time when the complex is created and
the total energy. Interestingly the recoil ion momentum obtained this way exhibits
a double peak structure, which does not depend strongly on the creation time but
on the energy. They find parallel and perpendicular momentum distributions,
which for helium (Fig. 9f) and for neon (Fig. 10c) are in reasonable agreement
with the experiment. This argument of a time-independent intermediate complex
seems to contradict the claim that the high recoil momenta and the double peak
result from the time delay due to the rescattering. One has to keep in mind,
however, that within the rescattering model the recollision energy and hence
the total energy of the complex analyzed by Sacha and Eckhardt is uniquely
determined by the recollision time. In a recent work they extended this model
to examine the decay of highly excited three-electron atoms [63].
The S-matrix approaches discussed above are based on the time-independent
Schr6dinger equation. One of the advantages of such approaches is that they
allow a precise definition of a mechanism (see, e.g., ref. [ 10]). Each particular
diagram represents one mechanism. The price that has to be paid is the loss
of information on the time evolution of the system. The diagram contains the
time order of interactions, but not the real time between them. Starting from the
time-dependent Schr6dinger equation in contrast gives the full information on
the time evolution of the many-body wave function in momentum or coordinate
space. In these coordinate space density distributions it is, however, often difficult
to clearly define what one means with a mechanism. Lein and coworkers
found a very elegant way to solve this problem [34,35]. Instead of plotting the
density in coordinate space they calculated the Wigner transform of the wave
function, depending on momentum and position. Integrated over the momentum
coordinate it is the density in coordinate space and integrated over the position
it is the distribution in momentum space. The Wigner transform can be read
as a density in phase space. Lein and coworkers plotted for example the phase
space evolution of the recoil ion in the polarization direction. This presentation
of a quantum-mechanical wave function is very close to the presentation of the
classical phase space trajectories. The rescattering mechanism can be seen very
clearly in this presentation.
18 R. D 6 r n e r et al. [V
ion is purely either from the ground state or from the momentum transfer in the
recollision process. All theories which are not confined to one dimension agree
roughly with the experimental width of the distribution. This direction should
be most sensitive to the details of the recollision process since that is where
the parallel momentum acquired from the field is scattered to the transverse
direction. Hence, a closer inspection of the transverse momentum transfer is of
great interest for future experimental and theoretical studies.
Electron energy distributions for double ionization have been reported for
helium [39], argon [80], neon [81] and xenon [38]. All these experiments find in
the sequential regime that the electron energies from double ionization are much
higher than those generated in single ionization. This is in full agreement with the
recoil ion momenta discussed above, since the mechanism being predominantly
responsible for producing high-energy electrons is exactly the same: It is a fact
that due to the rescattering the electrons from double ionization are not promoted
to the continuum at the field maximum but at a later time. Depending on the
actual time delay an energy of up to 2Up (see Eq. 1) can be acquired. The
work for helium (Fig. 11) and neon shows that the electron spectra extend well
above this value. Energies beyond 2Up are only obtainable if the recolliding
electron is backscattered during the (e,2e) collision. In this case the momentum
they have after the recollision adds to the momentum acquired in the field.
A large amount of elastically backward-scattered electrons has been observed for
single ionization where a plateau in the energy distribution is found extending
to energies of up to l OUp.
> 1000
9 ! 9 , 9 , , , 9 . , . .
N
C
100
oO 10
~N
E 0.1
k._
z
O
0.01 (a) (b)
FIG. 11. Electron energy spectra from single ionization (solid line) and double ionization (dots)
of helium at (a) 8• W/cm 2 and (b) 4x 1014 W/cm 2 (from ref. [39]).
20 R. D 6 r n e r et al. [VII
A. EXPERIMENTALFINDINGS
FIG. 12. Momentum correlation between the two electrons emitted when an Ar 2+ ion is
produced in the focus of a 220 fs, 800nm laser pulse at peak intensities of 3.8x 1014 W/cm 2 and
15x 1014 W/cm2. The horizontal axis shows the momentum component of one electron along the
polarization of the laser field; the vertical axis represents the same momentum component of the
corresponding second electron. Same sign of the momenta for both electrons represents an emission
to the same half sphere. The data are integrated over the momentum components in the direction
perpendicular to the polarization direction. The gray shading shows the differential rate in arbitrary
units on a linear scale (adapted from ref. [ 17]). Also compare this figure to Fig. 17.
FiG. 13. Momentum correlation between the two electrons emitted when an Ar 2+ ion is produced
in the focus of a 150 fs, 780nm laser pulse at peak intensities of 4.7• 1014 W/cm 2. Axis as in
Fig. 12. Each panel panel represents a part of the final state for a fixed transverse momentum
(p• of one of the electrons. (a) One of the electrons has a transverse momentum of p • < 0.1 au;
(b) 0.1 < p • < 0.2au; (c) 0.2 < p • < 0.3 au; (d) 0.3 < p • < 0.4au. The gray scale shows the
differential rate in arbitrary units and linear scale (from ref. [43]).
thus indicate that the joint acceleration of the electrons in the laser field clearly
dominates over the influence of electron repulsion.
For argon double ionization Weckenbrock et al. [43] and Moshammer et al.
[84] measured in addition to the momentum parallel to the field also the
transverse momentum of the detected electron. Both find that the correlation
pattern strongly depends on this transverse momentum (see Fig. 13). If one
electron is emitted with any transverse momentum larger than 0.1 au (i.e. at
some angle to the polarization axis) one mostly finds both electrons with a
similar momentum component in the field direction. It is this configuration that
dominates the integrated spectrum in Fig. 12. If, however, one electron is emitted
parallel to the polarization with a very small transverse momentum window of
p• < 0.1 au one finds that the parallel momentum distribution does no longer
peak on the diagonal. In this case most likely one electron is fast and the other
slow. This might be due to the fact that the 1/rl 2 potential forces the electrons
into different regions in the three-dimensional phase space. Consequently, for
electrons to have equal parallel momentum some angle between them is required.
VII] MULTIPLE IONIZATION IN STRONG LASER FIELDS 23
One might expect that the pure effect of electron repulsion could be studied in
double ionization by single-photon absorption with synchrotron radiation. In this
case there is no external field in the final state that could accelerate the electrons.
Many studies have shown however, that the measured momentum distribution is
not only governed by the Coulomb forces in the final state, but also by selection
rules resulting from the absorption of one unit of angular momentum and the
accompanying change in parity. For helium for example the two-electron contin-
uum wave function has to have ~p0 character. Since these symmetry restrictions
on the final state are severe it is misleading to compare distributions of kezl versus
kez2 a s in Fig. 12 directly to those from single-photon absorption (this distribution
can be found in ref. [86]). The effect of electron repulsion can be more clearly
displayed in a slightly different geometry as shown in Fig. 14. Here one electron
is emitted along the positive x-direction and the momentum distribution of the
second electron is shown. The data are integrated over all directions of this
internal plane of the three-body system relative to the laboratory. Clearly electron
repulsion dominates the formation of this final state distribution: there is almost
no intensity for emission to the same half sphere. There is also a node for
emission of both electrons back-to-back. This is a result of the odd symmetry
of the final state. In the multiphoton case this node is expected for those events
where an odd number of photons is absorbed from the field (see e.g. [88]).
Another instructive comparison is the process of double ionization by charged
particle impact. Experiments have been reported for electron impact [89-91]
and fast highly charged ion impact [79,92]. The latter is of particular interest
from the strong field perspective since the potential "shock" induced at a target
atom by a fast highly charged projectile is in many aspects comparable to a
half cycle laser pulse. The time scale however is much shorter than that accessible
with lasers today. For their experiment colliding 1 GeV/u U 92+ projectiles on
helium for example Moshammer and coworkers [93] estimated a power density
of > 1019 W/cm 2 and a time of sub attoseconds. Under such conditions ion-
24 R. D 6 r n e r et al. [VII
Fie. 14. Single-photon double ionization of He at l eV and 20eV above threshold by linearly
polarized light (synchrotron radiation). Shown is the momentum distribution of electron 2 for fixed
direction of electron 1 as indicated. The plane of the figure is the internal momentum plane of the
two particles. The data are integrated over all orientations of the polarization axis with respect to
this plane. The figure thus samples the full cross section and all angular and energy distributions
of the fragments. The outer circle corresponds to the maximum possible electron momentum; the
inner one represents the case of equal energy sharing (from ref. [87]; compare also ref. [83]).
FIG. 15. Double ionization of helium by 100 MeV/u C 6+ impact. The horizontal and vertical axes
(Pill and P211) show the momentum components of electrons 1 and 2 parallel to the direction of the
projectile. The dashed curves demarcate the region of the two-electron momentum space which is
not accessed by the spectrometer. The gray scale is linear (adapted from ref. [92]).
projectile accelerates both electrons into the forward direction (see also ref. [96]
for a theoretical interpretation of the double ionization process; see ref. [99] for
another experiment showing directed multiple electron emission; see ref. [78] for
an analysis of the acceleration of an electron in the field of the projectile).
5" 1
d
-2
-3
-4
-3 -2 -1 0 1 2 3 4
P z, e l ( a . u . ]
FIG. 16. Classically allowed region of phase space within the rescattering model for double
ionization of argon by 4.7 x 1014W/cm2, 800 nm light. Each circle corresponds to a fixed recollision
energy. Axis as in Fig. 12 (adapted from ref. [44]).
I I I I I I
- I I
I
_ I
I 9 ~
I
. , - m I I
II
I
I --O . . . . n l i ~ l l l I l i - . / I
9= , m , emInm, / I
I ii ~ I
I m l i m i I I
o
i
I I I l m , I
nImn I
Q_ I I I I
-I -- I W
I m I
I
I
_
-- I I . . . . . . I
I
I
I
I
I
I. . . . . . . . . . . I
I 1 I I I I
-3 -2 -1 0 1 2 3
pl I [a.u.]
FIG. 17. Correlated electron momentum spectrum of two electrons emitted from argon atoms
ii
at 0.25x 1015 W/cm 2. plI is the electron momentum component along the light polarization axis
of electron 1. Dashed line: kinematical constraints for recollision with excitation, assuming the
excited state is not immediately quenched. Solid line: kinematical constraints for recollision with
(e,2e) ionization (from ref. [45]).
of the field. Therefore one can expect that the excited state survives at least
until the next field maximum. Feuerstein et al. estimated an expected region in
phase space for excitation as shown in Fig. 17. For recollision events where the
second electron is lifted into the continuum the allowed region of phase space is
somewhat smaller than in Fig. 16 and confined to the two circles on the diagonal.
Feuerstein et al. used this argument to separate events in which the recollision
leads to an excited state and those which involve electron impact ionization.
Supporting this notion of an intermediate excited complex Peterson and
Bucksbaum [80] reported an enhanced production of low-energy electrons in the
ATI electron spectrum of argon previously unobserved which can be interpreted
in terms of inelastic excitation of Ar + or of multiple returns of the first electron.
Electrons from excited states field ionized at the field maximum will be detected
with very little momentum as they receive almost no drift velocity in the laser
field.
D. S-MATRIX CALCULATIONS
The full diagram shown in Fig. 8 has not yet been evaluated to obtain the
correlated electron momentum distribution. Goreslavskii and Popruzhenko suc-
ceeded, however, in calculating those distributions by making use of the saddle-
point approximation in the integration (see Fig. 18). The calculations shown
in Fig. 18 are restricted to zero transverse momentum; similar distributions for
28 R. D 6 r n e r et al. [VII
FIG. 18. Two-electron momentum distributions for double ionization of argon (similar to
Fig. 12), calculated by evaluating diagram 8 in the saddle-point approximation at an intensity of
3.8 x 10TMW/cm2. Contrary to the experimentthe calculations are not integrated over all momentum
components transverse to the field but restricted to electrons with no transverse momentum. The
right-hand panel presents the same distribution with the classically forbidden region of phase space
shown in white (compare Fig. 16) (adapted from ref. [54]).
neon and argon integrated over all transverse momenta can be found in ref. [85].
These calculations do not include intermediate excited states but only the direct
(e,2e) process. The calculations do not show a maximum on the diagonal as
seen in the experiments. To the contrary, they favor the situation where one
electron is slow and the other is fast. The authors of ref. [54] point out that
this is a direct consequence of the sharing of the excess energy in the (e,2e)
collision; the long-range Coulomb potential favors small momentum transfer
in the collision. By replacing the Coulomb potential with a contact potential
Goreslavskii and coworkers find a distribution which peaks on the diagonal,
much like the experimental results. The main reason is that a contact potential
does not emphasize small momentum transfers. It has to remain open at present
how well justified such a modification of the interaction potential is.
These calculations have been restricted to electrons with zero transverse
momentum. The trend seen in these calculations is in agreement with the
observation by Weckenbrock et al. [43] shown in Fig. 13a, where one electron
was confined to small transverse momenta. The calculations do not include
intermediate excited states but only direct electron impact ionization during
rescattering. Therefore the theoretical results are not too surprising since
electron impact ionization favors unequal energy sharing at the return energies
dominating here.
E. TIME-DEPENDENT CALCULATIONS
FIG. 19. Two-electron momentum distributions for double ionization of helium (similar to Fig. 12)
calculated by solving the one-dimensional time-dependent Schr6dinger equation at the following
intensities: (a) 1 x 1014 W/cm 2, (b) 3x 1014 W/cm 2, (c) 6.6x 1014 W/cm 2, (d) 10x 1014 W/cm 2,
(e) 13x 1014 W/cm 2, (f) 20x1014 W/cm 2 (adapted from [34]).
repulsion can lead to an opening angle between the electrons having the same
momentum component in the polarization direction, this is impossible in one
dimension. Here the electron repulsion necessarily leads to a node on the
diagonal for electrons emitted at the same instant in the field.
For 400nm radiation these calculations have also shown clear rings corre-
sponding to ATI peaks in the sum energy of both electrons [ 105]. Analogous to
ATI peaks in single ionization they are spaced by the photon energy. Similar rings
have been seen also in three-dimensional calculations at shorter wavelength [65].
VIII. Outlook
The application of COLTRIMS yielded the first differential data for double
ionization in strong laser fields. Compared to the experimental situation in double
ionization by single-photon absorption, however, the experiments are still in
their infancy. So far correlated electron momenta have been measured only for
argon and neon. Clearly experiments on helium are highly desirable since this
is where theory is most tractable. Also, mainly the momentum component in
the polarization direction has been investigated so far, resulting in a big step
forward in the understanding of multiple ionization in strong laser fields. None
of the experiments up to now has provided fully differential data since not all
six momentum components of the two electrons were analyzed. Therefore, no
coincident angular distributions as for single-photon absorption are available at
this point (see ref. [88] for a theoretical prediction of these distributions). Most
important for such future studies is a high resolution of the sum energy of the two
electrons, which would allow to count the number of photons absorbed. From
single-photon absorption it is known that angular distributions are prominently
governed by selection rules resulting from angular momentum and parity, hence,
from the even or oddness of the number of absorbed photons.
Another important future direction is a study of the wavelength dependence of
double ionization. The two cases of single and multiphoton absorption discussed
here are only the two extremes. The region of two- and few-photon double
ionization is experimentally completely unexplored. Experiments for two-photon
double ionization of helium will become feasible in the near future at the
VUV FEL facilities such as the TESLA Test facility in Hamburg.
IX. Acknowledgments
providing the laser facilities for the experiments. Moreover, H. Rottke, C. Trump,
M. Wittmann, G. Korn and W. Sandner made decisive contributions to the
experimental setup, helping in the realization of the experiments during beam-
times and contributed strongly in the evaluation and interpretation of the data.
We thank A. Becker, E Faisal and W. Becker for many helpful discussions
and for educating us on S-matrix theory. We have also profited tremendously
from discussions with K. Taylor, D. Dundas, M. Lein, V. Engel, J. Feagin,
L. DiMauro and P. Corkum. This work is supported by DFG, BMBF, GSI. R.D.
acknowledges supported by the Heisenberg-Programm of the DFG. R.M., B.E
and J.U. acknowledge support by the Leibniz-Programm of the DFG. T.W. is
grateful for financial support of the Graduiertenf'6rderung des Landes Hessen.
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A D V A N C E S IN ATOMIC, M O L E C U L A R , A N D O P T I C A L PHYSICS, VOL. 48
I. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 36
A. Experimental Methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38
B. Theoretical Methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 39
II. Direct Ionization . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 40
A. The Classical Model . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 40
B. Quantum-mechanical Description of Direct Electrons . . . . . . . . . . . . . . . . . 44
C. Interferences of Direct Electrons . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 47
III. Rescattering: The Classical Theory . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5O
IV. Rescattering: Quantum-mechanical Description . . . . . . . . . . . . . . . . . . . . . . . . 53
A. Saddle-point methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 55
B. Connection with Feynman's path integral . . . . . . . . . . . . . . . . . . . . . . . . . . 57
C. Connection with closed-orbit theory . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 58
D. The role of the binding potential . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 59
E. A homogeneous integral equation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 60
E Quantum orbits for linear polarization . . . . . . . . . . . . . . . . . . . . . . . . . . . . 61
G. Enhancements in ATI spectra . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 63
H. Quantum orbits for elliptical polarization . . . . . . . . . . . . . . . . . . . . . . . . . 68
I. Interference between direct and rescattered electrons . . . . . . . . . . . . . . . . . . 71
V. ATI in the Relativistic Regime . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 73
A. Basic Relativistic Kinematics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 73
B. Rescattering in the Relativistic Regime . . . . . . . . . . . . . . . . . . . . . . . . . . . 75
VI. Quantum Orbits in High-order Harmonic Generation . . . . . . . . . . . . . . . . . . . . 76
A. The Lewenstein Model of High-order Harmonic Generation . . . . . . . . . . . . . 77
B. Elliptically Polarized Fields . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 78
C. H H G by a Two-color Bicircular Field . . . . . . . . . . . . . . . . . . . . . . . . . . . . 78
D. H H G in the Relativistic Regime . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 84
VII. Applications of ATI . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 86
A. Characterization of High Harmonics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 87
B. The "Absolute Phase" of Few-cycle Laser Pulses . . . . . . . . . . . . . . . . . . . . 90
VIII. Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 92
IX. References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 92
I. I n t r o d u c t i o n
reviews pertinent to ATI have been given by Eberly et al. (1991), Mainfray and
Manus (1991), DiMauro and Agostini (1995), and Protopapas et al. (1997a). The
entire field of laser-atom physics has been succinctly surveyed by Kulander and
Lewenstein (1996) and, recently, by Joachain et al. (2000). Both of these reviews
concentrate on the theory. Nonsequential double ionization is well covered in a
recent focus issue of Optics Express, Vol. 8.
A. EXPERIMENTAL METHODS
.~. .L
,,,,l,,,,l,,,,iiiiii-,,,,l,,,, i,,,,I,,,,I,,,,
I0 20 KE (eV) :30 40
FIG. 2. (a) Measured and (b) calculated photoelectron spectrum in argon for 800 nm, 120 fs pulses
at the intensities given in TW/cm 2 in the figure (10Up = 39eV). From Nandor et al. (1999).
B. THEORETICAL METHODS
Nurhuda and Faisal (1999). The most detailed calculations have been carried
out by Nandor et al. (1999) and by Muller (1999a,b, 2001a,b). The techniques
are detailed by Muller (1999c). To our knowledge, no results for high-order ATI
for elliptical polarization based on numerical solution of the TDSE have been
published to this day.
Recently, numerical solution of the TDSE for a two-dimensional model
atom by means of the split-operator method has been widely used in order to
investigate various problems such as elliptical polarization (Protopapas et al.,
1997b), stabilization (Patel et al., 1998; Kylstra et al., 2000), magnetic-drift
effects (V~izquez de Aldana and Roso, 1999; V~izquez de Aldana et al., 2001)
and various low-order relativistic effects (Hu and Keitel, 2001).
Efforts to deal with the two-electron TDSE and, in particular, to compute
double-electron ATI spectra are under way (Smyth et al., 1998; Parker et al.,
2001; Muller, 2001c). In one dimension for each electron, such spectra have
been obtained by Lein et al. (2001).
An approach that is almost complementary to the solution of the TDSE starts
from the analytic solution for a free electron in a plane-wave laser field, the so-
called Volkov solution (Volkov, 1935), which is available for the Schr6dinger
equation as well as for relativistic wave equations, and considers the binding
potential as a perturbation. The stronger the laser field, the lower its frequency,
and the longer the pulse becomes, the more demanding is the solution of the
TDSE, and the more the Volkov-based methods play out their strengths.
This review concentrates on methods of the latter variety.
The classical model of strong-field effects divides the ionization process into
several steps (van Linden van den Heuvell and Muller, 1988; Kulander et al.,
1993; Corkum, 1993; Paulus et al., 1994a, 1995). In a first step, an electron
enters the continuum at some time to. If this is caused by tunneling (Chin et al.,
1985; Yergeau et al., 1987; Walsh et al., 1994), the corresponding rate is a highly
nonlinear function of the laser electric field ,~(t0). For example, the quasistatic
Ammosov-Delone-Krainov (ADK) tunneling rate (Perelomov et al., 1966a,b;
Ammosov et al., 1986) is given by (in atomic units)
2n*-Iml-I
r'(t) = A E w [~7(t)l exp ' 3[E(t) I (1)
where ,~(t) is the instantaneous electric field, EIp > 0 is the ionization potential of
the atom, n* = Z~ 2x/2E~p is the effective principal quantum number, Z is the charge
II] ATI: CLASSICAL TO QUANTUM 41
for a laser with intensity I and wavelength/l. If the electron is to have a nonzero
velocity v0 at time to, one has to replace eA(t0) by eA(t0)+ mv0 = p in the
velocity (2).
Most of the time, we will be concerned with the monochromatic elliptically
polarized laser field (-1 ~< ~ <~ 1)
coA
F_,(t) = ~ (~ sin cot - ~S' cos cot) (5)
V/1 +~2
A
A(t) = ~ (~ cos cot + ~S' sin cot) (6)
V/1 +~2
2~ 2 2
1+ ~2 Up ~ Edrift <~ 1 + ~2 Up. (7)
For linear polarization, it can acquire any value between 0 and 2Up, while
for circular polarization it is restricted to the value Up. Quantum mechanics
considerably softens these classical bounds. However, these bounds are useful as
benchmarks in the analysis of experimental spectra (Bucksbaum et al., 1986),
in particular for high intensity (Mohideen et al., 1993; Reiss, 1996) or low
frequency (Gallagher and Scholz, 1989).
In general, it is important to recall that the ionization probability depends
on the electric field, while the drift momentum p = eA(t0) is proportional
to the vector potential, both at the time to of ionization. The probability of
a certain drift momentum is weighted with the ionization rate at time to. The
electron is preferably ionized when the absolute value of the electric field is
near its maximum. Then, for linear polarization, the vector potential and, hence,
the drift momentum are near zero. In order to reach the maximal drift energy
of 2Up, the electron must be ionized when the electric field is zero and, hence,
the ionization rate is very low. This explains the pronounced drop of the ATI
electron spectrum for increasing energy, see Fig. 1. Sometimes, this interplay
between the instantaneous ionization rate and the drift momentum has surprising
consequences, notably for fields where the connection between the two is less
straightforward than for a linearly polarized sinusoidal field, e.g. for a two-color
II] ATI: CLASSICAL TO QUANTUM 43
FIG. 3. Dependence of the photoelectron yield as a function of the ellipticity ~ of the elliptically
polarized laser field (5) for electrons with an energy of 16.1 eV. Only electrons emitted parallel to
the major axis of the polarization ellipse are recorded. The ATI spectrum corresponding to linear
polarization (~ = 0) is shown in the inset. The laser intensity was 0.8x 1014 W/cm 2 at a wavelength
of 630 nm. The figure illustrates the dodging effect mentioned in Sect. II.A.I: ionization primarily
takes place when the electric field is near an extremum. For elliptical polarization, the electric field
then points in the direction of the major axis of the polarization ellipse, and the vector potential in
the direction of the minor axis. Hence, the electron's drift momentum p = eA(t0) is in the direction of
the minor axis. It is the larger, the larger the ellipticity ~ is. Consequently, emission in the direction
of the large component of the field decreases with increasing ellipticity: the electron dodges the
strong component of the field. The effect vanishes when circular polarization is approached and the
distinction between the major and minor axes disappears. From Paulus et al. (1998).
field (Paulus et al., 1995; Chelkowski and Bandrauk, 2000; Ehlotzky, 2001).
Another illustration is the dodging phenomenon for the direct ATI electrons
in an elliptically polarized laser field (Paulus et al., 1998; Goreslavskii and
Popruzhenko, 1996; Mur et al., 2001), see Fig. 3.
We have tacitly assumed that pulses are short enough to pass over the electron
before it has a chance to experience the transverse spatial gradient of the focused
pulse. In this event, the spatial dependence of the vector potential A(t) can
truly be neglected. Hence the drift momentum p is conserved and is indeed
the momentum recorded at the detector outside the field (Kibble, 1966; Becker
et al., 1987). The wiggling energy Up is lost or, in a self-consistent description,
returned to the field when the electron is left behind by the trailing edge of
the pulse. In the opposite case, where the electron escapes from the pulse
perpendicularly to its direction of propagation, the wiggling energy is converted
into drift energy (Kruit et al., 1983, Muller et al., 1983). This limit is also
realized in ATI by microwave ionization of Rydberg states (Gallagher and
44 W. Becker et al. [II
Mp =
t ~ e~,
lim
t t ~ --(X3
(lpp(t) Iu(t, t')l ~p0(t')). (8)
1 ~r2
H ( t ) = -2--mm - er . s + V(r), (9)
which includes the atomic binding potential V(r) and the interaction - e r . g ( t )
with the laser field. Furthermore, we introduce the Hamiltonians for the atom
without the field and for a free electron in the laser field without the atom,
with ]p - eA(t)) a plane-wave state [(rip - eA(t)) = (2:r) -3/2 exp i[(p - eA(t)) 9r]
and
Sp(t) = ~ dr [p - eA(r)] 2. (13)
The lower limit of the integral is immaterial. It introduces a phase that does not
contribute to any observable.
II] ATI: CLASSICAL TO QUANTUM 45
The time-evolution operator U(t, t') satisfies integral equations (Dyson equa-
tions), which are convenient if one wants to generate perturbation expansions
with respect to either the interaction H t ( t ) = - e r . g(t) with the laser field,
t
Equation (14) also holds if U and Ua in the second term on the right-hand side
are interchanged. The equivalent is true of Eq. (15). With the help of the integral
equation (14), using the orthogonality of the eigenstates of Ha, we rewrite Eq. (8)
in the form
The physical content of this substitution is that, after the electron has been
promoted into the continuum at time to due to the interaction Ht(to) = - e r . F-.(to)
with the laser field, it no longer feels the atomic potential. This satisfies the above
definition of a "direct electron." Amplitudes of the type (17) are called Keldysh-
Faisal-Reiss (KFR) amplitudes (Keldysh, 1964; Perelomov et al., 1966a,b;
Faisal, 1973; Reiss, 1980); for a comparison of the various forms that exist,
see Reiss (1992).
In the amplitude (17), one may write
Y Y
- e r . e(t0) = H/(tol-Ha + V(r) = - i ~ 0 - i ~ 0 + V(r). (is)
Via integration by parts, the amplitude (17) can then be rewritten as
d
[Eipt + Sp(t)] = EIp + ~ [ p - eA(t)] 2 = 0. (20)
dt
Let us consider a periodic (not necessarily monochromatic) vector potential with
period T = 23:/co. In terms of the solutions ts of Eq. (20), the amplitude (19)
can then be written as (Gribakin and Kuchiev, 1997; Paulus et al., 1998)
/lip oc Z 6 (p2
-~-mm+ Eip + mp - n oJ
)
n
(21)
2~i
• ~s S~'(ts) ei[Ewts+Sp(ts)](p-eA(ts)lV[lP~
where S~~ denotes the second derivative of the action (13) with respect to time.
The sum over s extends over those solutions of Eq. (20) within one period of
the field (e.g. such that 0 ~< Re t, < T) that have a positive imaginary part.
Obviously, the saddle points are complex unless Eip = 0. For Eip - 0, we retrieve
the classical drift momentum (2) provided p is such that p = eA(t) at some time t.
The imaginary part of to can be related to a tunneling time (Hauge and Stovneng,
1989).
In Eq. (21), the ionization amplitude is represented as the coherent sum over all
saddle points within one period of the field. The fact that the spectrum consists
of the discrete energies
p2
Ep - 2m - n m - U p - Eip (22)
Interferences also exist for an elliptically polarized laser field for fixed electron
momentum as a function of the ellipticity. Since, in experiments, the ellipticity is
better defined than the intensity, these interferences have been observed (Paulus
et al., 1998); see next subsection.
The amplitude (19) admits a vector potential A(t) of arbitrary shape; it is
by no means restricted to a monochromatic field of infinite extent. For a pulse
of finite extent, the saddle points are still determined by Eq. (20). They have,
however, no longer any periodicity. Hence, the discreteness of the spectrum is
lost. Interference from different parts o f the pulse may lead to unexpected effects
(Raczyfiski and Zaremba, 1997).
While for an infinitely long monochromatic pulse the spectrum is symmetric
with respect to p ~ - p , this forward-backward symmetry no longer holds for
a finite pulse. Analysis of the spatial asymmetry of the spectrum may aid in
determination o f the pulse length or the absolute carrier phase (Dietrich et al.,
2000; Hansen et al., 2001; Paulus et al., 2001b); see Sec. VII.B.
For linear polarization and a drift m o m e n t u m p = p~ with [p] <~ eA, there
are two possible ionization times cot01 = Jr/2 + 6 and O)to2 = 3 3 r / 2 - 6. The
corresponding classical orbits are illustrated in Fig. 4. As discussed above, while
A(t01) = A(t02), the field satisfies s = -•(t02). Hence, electrons ionized at
t01 and t02 depart in opposite directions right after the instant of ionization. As
illustrated in Fig. 4, the electric field changes sign soon after t01. Hence, the
electron ionized at this time turns around at a later time and acquires the same
drift momentum as the electron ionized at time t02, which keeps its original
direction. We expect quantum-mechanical interference of the contribution of
these two ionization channels.
to~ = Jr/2 + 6
0 2 4 6 8 0 2 4 6 8
rot~Jr ~ot # r
FIG. 4. Classical trajectories (dashed lines) of electrons having the same drift momentum. The
solid line is the effective potential V(x)- exg(t) at times t01 (left) and t02 (right). The electron
ionized at to] is turned around by the field shortly after ionization. In contrast, the electron ionized
at t02 maintains its original direction. This is a strongly simplified picture of the physics underlying
the interferences of direct electrons.
48 W. B e c k e r et al. [II
3.0 a)
E
l ~=0.78
.,qo
0.0 0.2 0.4 0.6 0.8 1.0
~2.0 ~=o.7~..-.--T---....~=o.7
E
,,....=
1.0
, ,
F1G. 5. (a) Positions of the saddle points Ogts in the upper half of the complex ~ot plane in the
interval 89 ~<Rewt <~ 3Jr, calculated from Eq. (23) forE= 17~o-Ew-Up, where EIp = 15.76 eV,
Up = 3.68 eV, and h w - 1.96eV. The arrows indicate the motion of the saddle points for increasing
ellipticity ~. The two branches meet at ~0 = 0.755. For several values of the ellipticity, insets depict
the ellipse traced out by the electric-field vector, and the positions of the latter at the emission
times Re ts are marked by solid dots. (b) The function Re ~, which determines the magnitude of the
amplitude Mp. The existence of the valley near the ellipticity ~0 is related to the effect of dodging,
illustrated in Fig. 3. (c) The function cosZ(Im 9 + ~p), whose oscillations are caused by constructive
and destructive interference. The essential physics behind this interference is sketched in Fig. 4.
From Paulus et al. (1998).
10 0 , , ,
f - o - 8.23eV ~104
~ 10.03eV
11.38eV
~ ,,d %, ~
,o~2~ 4~a ~%,
o=o103
'-
t 48.88eV
c--
ln-2 , , ,
"-1 .00 -0.50 0.00 0.50 1.00
ellipticity
FIG. 6. ATI spectra in xenon for an intensity of 1.2x 1014 W/cm 2 for various energies in the
direction of the large component of the elliptically polarized field as a function of the ellipticity.
The inset shows the energy spectrum for linear polarization. The three traces for the lower energies
display the interference phenomenon of the direct electrons discussed in Sect. II.C; the one for the
highest energy belongs to a plateau electron. The interference dips are related to Fig. 5c. From
Paulus et al. (1998).
there is no interference. In the first case, the amplitude can be written in the
form Mp ~ exp(Re ~)cos(Im 9 + ~p), in the second case the cosine is absent.
The two arguments are also plotted in Fig. 5.
The corresponding interferences have been observed by Paulus et al. (1998);
see Fig. 6. They are responsible for the undulating pattern in the ellipticity
distribution, which moves to smaller ellipticity for increasing energy. The same
tendency can be observed in the numerical evaluation of the amplitude (21); see
Paulus et al. (1998) for an example.
For elliptical polarization, the KFR amplitude (19) must be applied with
due caution: it predicts fourfold symmetry of the angular distribution, while
the experimental distributions only display inversion symmetry (Bashkansky
et al., 1988). Mending this deficiency requires improved treatment of the binding
potential (Krsti6 and Mittleman, 1991). More discussion of this point has been
provided elsewhere by Becker et al. (1998), who also give further references.
The spatial dependence introduced by Coulomb-Volkov solutions in place of the
usual Volkov solutions (12) already suffices to destroy the fourfold symmetry,
and angular distributions have been calculated with their help by Jarofi et al.
(1999). However, even for a zero-range potential the fourfold symmetry is
50 W. B e c k e r et al. [III
broken provided the effects of the finite binding energy are treated beyond the
KFR approximation (Borca et al., 2001).
Very similar interferences have been seen by Bryant et al. (1987) in the
photodetachment of H- in a constant electric field. Here the electron, once
detached, has the choice of starting its subsequent travel either against or with
the direction of the electric field, by close analogy with the opposite directions
of initial travel for the ionization times t01 and/02 in the present case; see Fig. 4.
A spatial resolution of the same effect is observed by the photodetachment
microscope of Blondel et al. (1999). The theoretical description reproduces the
observed patterns. Additional bottle-neck structures develop when a magnetic
field is applied parallel to the electric field (Kramer et al., 2001).
Thus far, we have dealt with "direct" electrons, which after the first step of
ionization leave the laser focus without any additional interaction with the ion.
In this and the next section, we will consider the consequences of one such
additional encounter.
The classical model becomes much richer if rescattering effects are taken
into account. To this end, we integrate the electron's velocity (2) to obtain its
trajectory
x(t) = -- (t - to) A(t0) - dr A(r) . (24)
m to
The condition that the electron return to the ion at some time tl > to is
x(tl) - 0. For linear polarization in the x-direction, this implies x ( t l ) = 0, and
y ( t ) = z ( t ) - O. This yields tl as a function of to. We defer discussion of elliptical
polarization to Sect. IV.H.
When the electron returns, one of the following can happen (Corkum, 1993):
(1) The electron may recombine with the ion, emitting its energy plus the
ionization energy in the form of one photon. This process is responsible
for the plateau of high-order harmonic generation.
(2) The electron may scatter inelastically off the ion. In particular, it may dis-
lodge a second electron (or more) from the ionic ground state. This process is
now believed to constitute the dominant contribution to nonsequential double
ionization.
(3) The electron may scatter elastically. In this process, it can acquire drift
energies much higher than otherwise.
In the following, we will concentrate on this high-order above-threshold
ionization (HATI). We will, however, also briefly discuss high-order harmonic
generation in Sect. VI.
III] ATI" CLASSICAL TO QUANTUM 51
From Eq. (2), the kinetic energy of the electron at the time of its return is
e2
Eret - ~m [A(tl) - A(t0)] 2 . (25)
Maximizing this energy with respect to to under the condition that X(tl ) = 0 yields
Eret, m a x = 3.17Up for oJt0 = 108 ~ and ootl = 342 ~ (Corkum, 1993; Kulander
et al., 1993). It is easy to see that after rescattering the electron can attain a
much higher energy: Suppose that at t = tm the electron backscatters by 180 ~ so
that m v ( t l -- O) = e[A(to) - A ( t l )] j u s t before and mv(tl + O) = - e [ A ( t o ) - A(tl )]
just after the event of backscattering. Then, for t > t l , the electron's velocity is
again given by Eq. (2), but with Px = e [ 2 A ( t m ) - A(t0)] so that
e2
Ebs - ~m [2A(tl) - A(t0)] 2. (26)
Maximizing Ebs under the same condition as above yields Ebs, max = 10.007Up
(Paulus et al., 1994a) for tot0 = 105 ~ and totl = 352 ~ These values are very
close to those that afford the maximal return energy.
It is important to keep in mind that for maximal return energy or backscat-
tering energy, the electron has to start its orbit shortly after a maximum of the
electric field strength. As a consequence, it returns or rescatters near a zero of
the field, see Fig. 7. This also provides an intuitive explanation of the energy
gain through backscattering: if the electron returns near a zero of the field and
backscatters by 180 ~ then it will be accelerated by another half-cycle of the
field.
In general, the equation X(tl) = 0 for fixed to may have any number of
solutions. This becomes evident from the graphical solution presented in Fig. 7.
If the electron starts at a time to just past an extremum of the field, it returns
to the ion many times. These solutions having long "travel times" t l - to are
very important for the intensity-dependent quantum-mechanical enhancements
of the ATI plateau to be discussed in Sect. IV.G. Here we will be satisfied with
mentioning another property of the classical orbits" obviously, the return energy
will have extrema, e.g. the maximum of Ebs, max -- 10.007Up mentioned above,
which is assumed for a certain time t0,max (t0,max = 108 ~ in the example). If
we are interested in a fixed energy Ebs < Ebs, max, there are two start times that
will lead to this energy: one earlier than t0, max, the other one later. From the
graphical construction of Fig. 7 it is easy to see that the former has a longer
travel time than the latter. In the closely related case of HHG, these correspond
to the "long" and the "short" orbit (Lewenstein et al., 1995b). The cutoffs of the
solutions with longer and longer travel times are depicted in Fig. 8.
If we consider rescattering into an arbitrary angle 0 with respect to the
direction of the linearly polarized laser field, we expect a lower maximal energy
since part of the maximal energy 3.17Up of the returning electron will go into the
52 W. Becker et al. [III
-- ....-.......
9 ~149
9 ~
.
t~ t',
. . . . . .
FIG. 7. Graphical solution of the return time t 1 for given start time to; cf. Paulus et al. (1995):
The return condition X(tl) = 0 can be written in the form F ( t l ) - F(to) + (tl - to)Fl(to), where the
function F(t) = f t dr A ( r ) ~ sin ~ot (solid curve) is an integral of the vector potential A ( r ) ~ cos w r
(dotted curve) 9 The thick solid straight line, which is the tangent to F ( r ) at r = to, intersects F ( r )
for the first time at r = tl. The start (ionization) time to was chosen such that the kinetic energy Ere t
(Eq. 25) at the return time tl is maximal and equal to Eret,ma x = 3.17Up. The two adjacent straight
lines both yield the same kinetic energy Ere t < Eret,ma x. The figure shows that one starts earlier and
returns later while the other one starts later and returns earlier. Obviously, there can be many more
intersections with larger values of ti provided the start times are near the extrema of F ( r ) . They
correspond to the orbits with longer travel times.
transverse motion. This implies that, for fixed energy E b s , there is a cutoff in the
angular distribution; in other words, rescattering events will only be recorded for
angles such that 0 ~< 0 ~< 0max(Ebs). This is a manifestation of rainbow scattering
(Lewenstein et al., 1995a). All of this kinematics is contained in the following
equations (Paulus et al., 1994a):
Here 00 is the scattering angle at the instant of rescattering, which may have
any value between 0 and Jr, as opposed to the observed scattering angle 0 at
the detector (outside the field). In Eq. (27), the upper (lower) sign holds for
A(to) > A(h) (A(to) < A(tl)).
Pronounced lobes in the angular distributions off the polarization direction
were first observed by Yang et al. (1993), while the rescattering plateau in the
energy spectrum with its cutoff at 10Up was identified by Paulus et al. (1994b,c).
IV] ATI: C L A S S I C A L TO Q U A N T U M 53
Fie. 8. Maximum drift energy after rescattering (ATI plateau cutoff) upon the mth return to the ion
core during the ionization process. Electrons with the shortest orbits (m = 1) can acquire the highest
energy, whereas electrons that pass the ion core once before rescattering at the second return (m = 2)
have a rather low energy. Each return corresponds to two quantum orbits: the mth return corresponds
to the quantum orbits 2m + 1 and 2m + 2.
These spectra prominently display the classical cutoffs at 0max and Ebs,max.
The classical features become the better developed the higher the intensity is.
Hence, they are particularly conspicuous in the strong-field tunneling limit.
This has been shown theoretically by comparison with numerical solutions of
the Schr6dinger equation (Paulus et al., 1995) and experimentally for He at
intensities around 1015 W/cm 2. Indeed, the latter spectra show an extended
plateau for energies between 2Up and 10Up (Walker et al., 1996; Sheehy
et al., 1998). For comparatively low intensities, angular distributions have been
recorded in xenon with very high precision by Nandor et al. (1998). They also
show the effects just discussed, but with much additional structure that appears to
be attributable to quantum-mechanical interference and to multiphoton resonance
with ponderomotively upshifted Rydberg states (Freeman resonances; Freeman
et al., 1987).
which now describes both the direct and the rescattered electrons. The physical
content of the amplitude (29) corresponds to the recollision scenario: The
electron is promoted into the continuum at some time to; it propagates in the
continuum subject to the laser field until at the later time tl it returns to within the
range of the binding potential, whereupon it scatters into its final Volkov state.
Exact numerical evaluation of the amplitude (29) for a finite-range binding
potential is very cumbersome. For a zero-range potential, however, the spatial
integrations in the matrix element become trivial, and the computation is rather
straightforward. If the field dependence of the Volkov wave function and the
Volkov time-evolution operator is expanded in terms of Bessel functions, one of
the temporal integrations in the amplitude (29) can be carried out analytically
and yields the same 6 function as in Eq. (21), specifying the peak energies. The
remaining quadrature with respect to the travel time tl - t o has to be carried
out numerically; see Lohr et al. (1997) and Milo~evi6 and Ehlotzky (1998a),
where explicit formulas can be found; for elliptical polarization see Becker et al.
(1995) and Kopold (2001). Alternatively, the integral over the travel time may
be done first, and the integral over the return time tl is then evaluated by Fourier
transformation (Milo~evi6 and Ehlotzky, 1998b).
The relevance of the rescattering mechanism to ATI and multiple ionization
was suggested early by Kuchiev (1987) and by Beigman and Chichkov (1987).
Improvements of the customary KFR theory by including further interactions
with the binding potential were already discussed by Reiss (1980). The first
explicit calculations of angular-resolved energy spectra were carried out by
Becker et al. (1994a, 1995) and by Bao et al. (1996). Closely related rescattering
models were presented by Smirnov and Krainov (1998) and by Goreslavskii and
Popruzhenko (1999a,b, 2000).
The physics of high-order ATI is related to electron scattering at atoms in the
presence of a strong laser field. For high-order ATI, the initial state of the electron
is a wave packet created by tunneling, while for electron-atom scattering it is
a plane-wave state. This latter problem was studied theoretically by Bunkin and
Fedorov (1966) and by Kroll and Watson (1973). Corresponding experiments
IV] ATI: CLASSICAL TO QUANTUM 55
A. SADDLE-POINT METHODS
For sufficiently high intensity, the temporal integrations in the amplitude (29)
can be carried out by the saddle-point method, as in the case of the direct
amplitude (19). This procedure provides much more physical insight than
Bessel-function expansions, and establishes the connection with Feynman's path
integral, to be discussed below.
In this context, rather than taking advantage of the explicit form of the Volkov
time-evolution operator, we expand it in terms of the Volkov states (12),
S,'k I, (30.
so that the amplitude Mp is represented by the five-dimensional integral
Mp ~
Sp(tl,to, k) - 1
2m d r [p - e A ( r ) ] 2
ftl ~
(33)
dr [k - eA(T)] 2 + dr EIp
2m
in the exponent consists of three parts, according to the three stages discussed
above.
As above in Eq. (20), we approximate the amplitude (31) by expanding the
phase (33) of the integrand about its stationary points. In this process, we assume
that the function mp(tl, to, k) depends only weakly on its arguments. Indeed, for
a zero-range potential, it is a constant. We now have to determine the stationary
points with respect to the five variables tl, to and k. They are given by the
solutions of the three conditions (Lewenstein et al., 1995a)
[k - eA(t0)] 2 = -2mEip, (34)
parent ion, and the third one (36) expresses that, on this occasion, it rescatters
elastically into its final state. In general, the saddle-point equations have several
solutions (tls, t0s, ks), (s = 1,2,...), of which only those are relevant for which
Re tls > Re t0s, such that the recollision is later than ionization, cf. the limits of
the integral in Eq. (31). The matrix element can be written as
k15)
1/2
where ql s) (i = 1 , . . . , 5 ) runs over the five variables tls, tos and ks. As we
noted already for the direct electrons in the context of Eq. (21), the sum has
to be extended only over a subset of the solutions of the saddle-point equations
(34)-(36). However, in the present case, determining this subset may be tricky
(Kopold et al., 2000a). For a periodic field, the sum over the periods in Eq. (37)
can be carried out by Poisson's formula. This leaves a sum over the saddle points
within one period and produces a 6 function as in Eq. (21).
The computation of ATI now consists of two separate tasks. First, the solutions
of the saddle-point equations (34)-(36) have to be determined and, second,
the appropriate subset has to be inserted into expression (37). Note that we
apply the saddle-point approximation to the probability amplitude for given final
momentum p, and not to the complete wave function of the final state. This is the
reason why only few solutions contribute, while a semiclassical computation of
the wave function, which contains all possible outcomes, requires consideration
of a very large number of trajectories (van de Sand and Rost, 2000).
Since EIp > 0, the condition (34) of "energy conservation" at the time of
ionization cannot be satisfied for any real time to. As a consequence, all solutions
(tls, tos, ks) become complex. If the ionization potential EIp is zero, then, for
a linearly polarized field, the first saddle-point equation (34) implies that the
electron starts on its orbit with a speed of zero. Provided the final momentum p
is classically accessible, the resulting solutions are entirely real. They correspond
to the so-called "simple-man model" (van Linden van den Heuvell and Muller,
1988; Kulander et al., 1993; Corkum, 1993). For EIp r 0, so long as the Keldysh
parameter 72= Eip/(2Up) is small compared with unity, the imaginary parts of
the solutions of Eqs. (34)-(36) are still not too large, and the real parts are still
close to these simple-man solutions. In this case, approximate analytical solutions
to the saddle-point equations can be written down, which yield an analytical
approximation to the amplitude (31) (Goreslavskii and Popruzhenko, 2000). On
the other hand, for elliptical polarization, the solutions are always complex, even
when EIp = 0. This reflects the fact that, for any polarization other than linear,
an electron set free at any time during the optical cycle with velocity zero will
never return to the point where it was released. Equation (34) then only implies
that k - eA(t0) is a complex null vector.
IV] ATI: CLASSICAL TO QUANTUM 57
With the solutions (tls, to,, ks) (s = 1,2 .... ) of Eqs. (34)-(36), the sth quantum
orbit has the form
We regard the orbit as a function of the real time t. The conditions x(t0) = 0
and X(tl) = 0, however, are satisfied for the complex times to and tl. As a
consequence, the quantum orbit (38) as a function of real time does not depart
from the origin but, rather, from the "exit of the tunnel." This is clearly visible in
Figs. 14, 15, 17 and 20 below. In contrast to the start time to, the return time tl is
real to a good approximation, see Fig. 10 (below). Accordingly, the orbits return
almost exactly to the origin.
where S(t, t') = ft t, dr L[r(r)], r] is the action calculated along a system path, and
the integral measure D[r(r)] mandates summation over all paths that connect
(rt) and (r' t') (see, e.g., Schulman, 1977).
The path integral (39) sums over the functional set of all continuous
paths. In the quasi-classical limit, this can be reduced to a sum over all
classical paths, which are those for which the action S(t,t') is stationary.
For quadratic Hamiltonians, this WKB approximation is exact. In our case,
motivated by the success of the classical three-step model of Sect. III, we
have reduced the exact transition amplitude to the form (31). In implementing
the strong-field approximation, we have approximated the exact action of the
system appropriately at the various stages of the process: before the initial
ionization, in between ionization and rescattering, and after rescattering, as in
the decomposition (33) of the action. This still left us with a five-dimensional
variety of paths. Out of those, finally, the saddle-point approximation (37) selects
the handful of "relevant paths" (Antoine et al., 1997; Kopold et al., 2000a;
Sali~}res et al., 2001). These are essentially the orbits of the classical model, yet
quantum mechanics is fully present: Their coherent superposition as expressed
in the form (37) allows for interference of the contributions of different orbits,
and the fact that they are complex accounts for their origin via tunneling.
58 W. Becker et al. [IV
This differs from the photoabsorption cross section (40) only by the presence
of the Volkov time-evolution operator u(Vv)(tl,t0), which reflects the strong-
field approximation, instead of the exact time-evolution operator U(t, 0) of the
time-independent problem [for which the time-evolution operator U(t, t ~) only
IV] ATI: CLASSICAL TO QUANTUM 59
depends on the time difference t - t~]. In the total ionization probability (41),
via the same partial integration (18) as above, the electron-field interaction
r. s can be replaced by V(r). The result then looks like the differential
HAIl amplitude (29) except that it is sandwiched by the ground state. This
correspondence is a manifestation of the optical theorem.
The improved Keldysh approximation (29) has been written down for an
arbitrary binding potential V(r). The expansion in terms of the binding potential,
introduced via the Dyson equation (15), is a strong-field approximation (SFA),
which is valid when the electron's quiver amplitude is so large that most of its
orbit is outside the range of the binding potential. This is trivially guaranteed
for the three-dimensional binding potential of zero range,
This potential supports a single (s-wave) bound state at the energy -tc2/2m
and a continuum that is undistorted from the free continuum except for the
s wave, as required by completeness (Demkov and Ostrovskii, 1989). Without the
regularization operator (O/Or)r, which acts on the subsequent state, the potential
does not admit any bound state. There are several possibilities to adjust the one
parameter tr to an individual atom or ion. In most cases one will determine it
so as to reproduce the ionization potential; see, however, Sect. IV.G.
The zero-range potential (42) underlies many of the explicit results exhibited
in this chapter. However, we emphasize that the amplitude (29), as well as its
saddle-point approximation (37), hold for a much wider class of potentials.
Regardless of the potential, the saddle-point equations (34)-(36) have the
electron start from and return to the center of the binding potential, which is
the origin, and do not depend on its shape. The potential only enters via the
form factors in Eq. (32). For the SFA to be applicable, they must depend on
time only weakly. The procedure corresponds to the Born approximation. It will
be the better justified, the shorter the range of the potential is, so that the form
factor depends only weakly on the momenta. Excited bound states do not enter
the amplitude (29) regardless of the potential used.
For a comparison of a high-order ATI spectrum calculated for the zero-range
potential (42) with the same spectrum extracted from a solution of the three-
dimensional TDSE for hydrogen, see Cormier and Lambropoulos (1997) for the
latter and Kopold and Becker (1999) for the former. There is good qualitative
agreement within the ATI plateau; in particular, the positions of the dips in the
spectrum that are due to destructive interference agree within a few percent.
The comparison confirms that the detailed shape of the potential has only minor
significance for the HATI spectrum. This holds for hydrogen and the rare gases,
60 W. Becker et al. [IV
but not for the alkali-metal atoms (Gaarde et al., 2000). The height of the
rescattering plateau with respect to the direct electrons does depend on the atomic
species; for the theoretical modeling, see Goreslavskii and Popruzhenko (1999a,
2000). Clearly, however, the real physical systems best described by a zero-
range potential are negative ions with a s-wave ground state. Angular-resolved
photoelectron spectra in H- have been recorded recently by Reichle et al. (2001).
Attempts have been made at including the effects of the binding potential
of the residual ion beyond the first-order Born approximation. Kamifiski et al.
(1996) and Milogevi6 and Ehlotzky (1998c) have employed the so-called
Coulomb-Volkov (CV) states, which are obtained from the ordinary Volkov
states (12) by replacing the plane wave [ p - eA(t)) by a Coulomb outgoing-wave
scattering state with momentum p (ordinary CV state) or p - eA(t) (improved
CV state). These are then substituted in the transition amplitudes (17) or (29)
for the ordinary Volkov states. A systematic assessment of the merits of this
approach appears not to have been made; recently, however, it has been compared
with the solution of the TDSE and was shown to work well for ionization by
ultrashort pulses having a duration shorter than the orbital period of the initial
bound state (Duchateau et al., 2001).
/'
version (29) starts from the homogeneous integral equation
which holds for the state that develops out of the unperturbed ground state
due to its interaction with the laser field. This integral equation can be derived
immediately from the Dyson equation (15) if one applies both sides of the latter
to the atomic ground state [~P0(t~)) in the limit where t ~ ---, -oo. By inspection,
one may convince oneself that the term Uf(t,t')[~Po(t')) makes no contribution
for t - t ~ --, cx~ so that Eq. (43) is left. This equation was first introduced in the
context of the quasi-energy formalism by Berson (1975) and by Manakov and
Rapoport (1975) for circular polarization and Manakov and Fainshtein (1980)
for arbitrary polarization.
Inserting on the right-hand side of the integral equation (43) the expansion (30)
of Uf in terms of Volkov states and replacing [W(r)) by the unperturbed
atomic ground state [~P0(~')), one can read off the matrix element (19) for direct
ionization. Iterating Eq. (43) one gets
which yields the improved KFR amplitude (29) in the same fashion.
The integral equation (43) is particularly useful for the zero-range poten-
tial (42), since in this case it allows one to calculate the wave function in all space
IV] ATI: CLASSICAL TO QUANTUM 61
provided it is known at the origin. For the latter, to a first approximation, one
may employ the unperturbed wave function. Better approximations are obtained
by using more accurate expressions. These incorporate the possibility that the
ionized electron revisits the core, as illustrated by Eq. (44).
For the zero-range potential and a monochromatic plane wave with circular
polarization, it can be shown that the wave function near the origin exactly obeys
qJ(r,t) o( ( 1 / r - t c ) e x p ( - i E t ) for all times. The complex quasi-energy E has
to be determined as the eigenvalue of a nonlinear integral equation (Berson,
1975; Manakov and Rapoport, 1975). For any polarization other than circular,
the time dependence at the origin is given by a Floquet expansion (Manakov and
Fainshtein, 1980; Manakov et al., 2000). The interaction with a laser field for a
finite period of time was considered along similar lines by Faisal et al. (1990)
and Filipowicz et al. (1991); see also Gottlieb et al. (1991) and Robustelli et al.
(1997). The integral equation (43) was also used for two-center potentials in
order to model molecular ions (Krstid et al., 1991; Kopold et al., 1998).
"E - 1 2
-o -16 10
~-~ -22
~ -24
!
-26
-28 0 | !
1
J
"N,
P,
2 3 4 g t5 "7 8 9 10 11 12
electron energy [Up]
FIG. 9. Upper panel: ATI spectrum in the direction of the laser field for linear polarization for
1015 W/cm 2, hto = 0.0584 a.u., and a binding energy of Eip = 0.9 a.u. The electron energy is given
in multiples of Up. The curve at the top (solid circles) is the exact result from Eq. (29). The other
curves were calculated from the saddle-point approximation (37). From bottom to top, more and
more quantum orbits are taken into account; the results are displaced with respect to each other for
visual convenience. The curve at the bottom incorporates just the pair of orbits with the shortest
travel times, the next one up includes in addition the pair with the next-to-shortest travel times, and
so on. The occasional small spikes are artifacts of the saddle-point approximation, cf. Goreslavskii
and Popruzhenko (2000) and Kopold et al. (2000a). Lower panel: The envelopes of the contributions
of the individual pairs are shown all on the same scale so that the quantitative relevance of the various
pairs is put in perspective. The cutoffs of the various orbits agree with those displayed in Fig. 8.
From Kopold et al. (2000a).
IV] ATI: C L A S S I C A L TO Q U A N T U M 63
Re cot Re c o ( t - t ' )
2 3 4 3 4 5
i ' i ' i 0
, 1 , i [!11.51 , -
_ 11.5~ _
0.5
-0.5
2.5
_a o
-1
~,, 9 -o- - o- - -iBt~ 11.5 s
tl E
-1.5
I
--
-0.5 e91 1 5 9
t11.5
i ~ J , I -2
, _
' ' ' I ' ' ' '
i , i , i 1,15 I
0.2 i
m
-0.1
< 0.1 - 11.5 ~ ~ 2 5 -
<
i1) _ ~ 0 1 "" m
0
_.,. ~-.z-.:_ .. ,, 2.54 -0.2 x "
t
_ /,o-~ 11.5 -
E -0.1 - ~ ~ E m
-
i , i , "
~
9
11.5
, I , i i
...2.,s i 1 i i
v
FIG. 10. Saddle points (ts, t~,ks) for the orbits (s = 1,2) having the two shortest travel times. In
this figure, ts is the return time (elsewhere denoted by t]s), and ts~ the start time (elsewhere denoted
by tos). The figure shows a comparison of elliptical polarization (~ --0.5, solid circles) and linear
polarization (open squares). The values of the other parameters are those of Fig. 9 (eA = 2.04 a.u.).
The symbols identify electron energies of 11.5, 10.4, 8.92, 6.01, and 2.49, all in multiples of Up.
The dashed orbits have to be dropped from the sum (37) after the cutoff. With the scaling of k
given on the ordinate, the saddle points depend only on the Keldysh parameter y = v/IEoI/2Up.
(drawn dashed in the figure) has to be dropped from the sum (37). This causes the
artifact of the small spikes visible in Fig. 9. For energies above the cutoff, just one
orbit contributes and, as a consequence, the spectrum smoothly decreases without
any trace o f interferences. The real part o f the parameters stays approximately
constant, while the imaginary part increases strongly with increasing energy. This
is responsible for the steep drop o f the spectrum after the cutoff. Similar behavior,
as a function o f ellipticity, occurs in Fig. 5.
The procedure o f dropping one o f the orbits o f each pair after its cutoff
can be replaced by a more rigorous method. In the vicinity o f the cutoffs,
an approximation in terms of Airy functions was used by Goreslavskii and
Popruzhenko (2000). A uniform approximation was described in a different
context by Schomerus and Sieber (1997). It reproduces the spectra o f Fig. 9
without the spikes (Figueira de Morisson Faria et al., 2002b).
105
103 . . . . . . . . . .
==
8 lo 2
101
I
0 10 20 30 40
electron energy [eV]
FIc. 11. ATI spectra in argon at 800 nm recorded in the direction of the linearly polarized field for
various intensities rising by increments of 0.110 from 0.5 I0 (bottom curve) to 1.010 (top curve). The
horizontal lines mark the maxima of the ATI plateaus for each intensity. For intensities I > 0.8 I0 a
group of ATI peaks between 15 eV and 25 eV rears up quickly. (The spectra shown here represent
only a fraction of those actually measured.) From Paulus et al. (2001a).
the plateau region (by up to an order of magnitude) have been observed upon
a change of the laser intensity by just a few percent (Hertlein et al., 1997;
Hansch et al., 1997; Nandor et al., 1999). This behavior suggests a resonant
process. Near the resonances, the contrast of the spectra is remarkably reduced
(Cormier et al., 2001). For the experiments reported so far, the effect is most
pronounced for argon. This holds not only for a laser wavelength of 800nm
but also for 630nm (Paulus et al., 1994c). The enhancements are so strong
that in experiments implying significant focal averaging the observed spectral
intensity may well be dominated by these enhancements, regardless of the actual
peak intensity. In this sense, ATI in toto has been called a resonant process
(Muller, 1999b). A big step towards understanding the physical origin of the
enhancements was made in theoretical studies that reproduced the enhancements
in the single-active-electron approximation by numerical solution of the one-
particle time-dependent Schr6dinger equation in three dimensions (Muller and
Kooiman, 1998; Muller, 1999a,b; Nandor et al., 1999), thereby ruling out any
mechanism that invokes electron-electron correlation.
In Fig. 11 we show results of a measurement of the same effect, but for
a shorter pulse length of 50 fs (Paulus et al., 2001a). Spectra in an intensity
interval of 0.5 to 1.0 • I0 in steps of 0.1 • I0 are displayed. The maximum
intensity I0 was calibrated by using the cutoff energy of 10Up. This leads to
I0 ~ 8• 1013 W/cm 2. There is a striking difference between the spectra for
I ~< 0.810 and those for higher intensity: within a small intensity interval a group
IV] ATI: CLASSICAL TO QUANTUM 65
0.00
iI
o
d
. _
co
" -0.05
O
o
I1) I
N tI
-0.10 t
\
E - plateau
0 a 7.3 eV
• 6.4eV
-0.15 I = I I ~ J
FIG. 12. Comparison of the intensity dependence of ATI electrons with different energies. For
visual convenience, the overall increase in yield with increasing intensity has been subtracted. The
electrons at 6.4eV and 7.3 eV are due to the strongest Freeman resonances, i.e. resonance with
atomic states. Those labeled "plateau" are electrons in the plateau region of the spectra. As a
consequence of the subtraction of the overall increase, the resonance-like behavior corresponds to
those intensities where the respective curves start rising. It is evident that for the plateau electrons
this does not happen at those intensities where the atomic states shift into resonance. Quite to the
contrary, the intensity at which the yield of the plateau electrons starts its rise is reflected in the yield
of the low-energy electrons by a brief halt in their rise. This is indicated by the dashed circles.
I 12
! 4~
/ 1"1= 2.626
-13 ~ ~ ,'- "-. ........
~, -14
t-
O
i_
tO
-15
o ~", I , ' , i t,rajec] ~
0 10 20 30 40 50
- 12 j oo q = 2.326
-13 e ~
-14 ,....,,
-15"" ,, --- 6 9
',' trajectories 04
10 20 30 40 50
electron energy [eV]
Fic. 13. ATI spectra for Eip = 14.7eV, oJ = 1.55 a.u., and three intensities: at a channel closing
(71 = Up/oJ = 2.526, middle panel), below the channel closing (7/= 2.326, lower panel), and above
(7/= 2.626, upper panel). In each panel, the exact result calculated from Eq. (29) is shown (solid
symbols) and approximations involving the first 2 (dashed line), 6 (dot-dashed line), and 40 (solid
line) quantum orbits in Eq. (37). From Kopold et al. (2002).
Fig. 9 shows that too few orbits contribute for energies above about 8Up. Indeed,
the enhancements observed experimentally are restricted to the lower two-thirds
of the plateau. The interpretation also implies that the enhancements should
disappear for ultrashort pulses, where late returns do not occur. This has been
observed in experiments by Paulus et al. (2002). In numerical simulations o f
H H G based on the three-dimensional TDSE, the same effect has been noticed
by de Bohan et al. (1998).
W h e n the modified K F R matrix element (29) is used to describe data for real
atoms, the ionization potential EIp has to be replaced by an effective (lower)
value that corresponds to the d e f a c t o onset o f the continuum (Paulus et al.,
68 W. B e c k e r et al. [IV
2001 a; Kopold et aL, 2002). It is a fact that, for a Coulomb potential, the actual
onset of the continuum is hard to see and may better be replaced by an effective
value. This is illustrated, for example, by the photoabsorption spectra of Garton
and Tomkins (1967).
Numerical simulations predict very similar enhancements in high-order
harmonic spectra (Becker et al., 1992; Toma et al., 1999; Kuchiev and Ostrovsky,
2001; Kopold et al., 2002) and in nonsequential double ionization (NSDI) of
helium (Muller, 2001c). Experimentally, in argon irradiated by a flat-top pulse
from a Ti:Sa laser, resonant-like enhancement of the 13th harmonic was observed
by Toma et al. (1999). In HHG in one dimension, the dependence of the
enhancements on the shape of the potential and the presence or absence of
excited bound states has been investigated (Figueira de Morisson Faria et al.,
2002a). The results are largely compatible with the quantum-orbit picture.
In a semiclassical framework, the binding potential can be incorporated into
the orbits. This leads to Coulomb refocusing (Ivanov et al., 1996; Yudin and
Ivanov, 2001a): orbits that would miss the ion in the absence of the binding
potential are refocused to the ion in its presence. This emphasizes the importance
of late returns and leads to a substantial increase of rescattering effects without,
however, resonant behavior. If late returns are cut off due to an ultrashort laser
pulse, the rate of NSDI should decrease. Indeed, this has been experimentally
confirmed by comparison of 12-fs and 50-fs pulses (Bhardwaj et al., 2001).
.m
r -20
. . . . . . . . . . . . . 8.5u j
~"o. -22
FIG. 14. ATI spectrum in the direction of the large component of the elliptically polarized driving
laser field (5) for ff = 0.5 (see the field ellipse in the upper right corner of the figure) and electron
energies between 2.5 and 10.5Up. The other parameters are o9 = 1.59eV, EIp = 24.5eV, and
I = 5• 1014 W/cm 2. The open circles give the yields of the individual ATI peaks calculated from
the integral (29) for the zero-range potential. The other curves represent the contributions to the
quantum-path approximation (37) of the shortest trajectories 1 and 2 (dot-dashed line), 3 and 4
(long-dashed line), and 5 and 6 (short-dashed line), as well as the sum of all six (solid line). Note
that some of these curves overlap partly or entirely. The orbits responsible for each part of the
spectrum, viz. 1 and 2, 3 and 4, and 5 and 6, are presented near the margins of the figures. The
position of the ion is marked by a cross; notice that the orbits do not depart from there, but rather
from a point several atomic units away from it. This is the point where the electron tunnels into the
continuum. The electron travels the orbits in the direction of the arrows. Experimental data for a
similar situation are shown in Fig. 15. From Kopold et al. (2000b).
FIG. 15. ATI spectrum in xenon for an elliptically polarized laser field with ellipticity ~ = 0.36
and intensity 0.77• 1014W/cm2 for emission at an angle with respect to the polarization axis as
indicated in the upper right. The spectrum has a staircase-like appearance. The respective steps are
shaded differently. For each step, the real parts of the responsible quantum orbits are displayed. The
dots with the crosses mark the position of the atom, and the length scale is given in the upper left
of the figure. From Sali~res et al. (2001).
illustrated in Figs. 8 and 9. The main difference is that for elliptical polarization
the orbits are two-dimensional and encircle the ion. The pair of orbits with
the shortest travel times generates the part of the spectrum preceding the final
(highest-energy) cutoff. However, this part is very weak in relation to the yields
at lower energies. The latter are generated by orbits with longer travel times,
whose contributions for linear polarization are marginal, see Fig. 9.
Intuitively, this staircase structure can be understood as follows. Return o f the
electron to the ion is possible if the electron has a nonzero initial velocity. This
velocity is largely in the direction o f the small component o f the elliptically
polarized field. The larger this velocity is, the smaller is the contribution that
the associated orbit makes to the spectrum. [This can be compared with the
distribution of transverse momenta in a Gaussian wave packet (Dietrich et al.,
1994; Gottlieb et al., 1996).] For the shortest orbit, while the large component
of the field changes sign so that the electron is driven back to the core in this
direction, the small component has the same sign for the entire duration o f the
orbit. Hence, a particularly large initial velocity in this direction is required in
order to compensate the drift induced by the small field component. For the
longer orbits, the small component changes direction, too, during the travel time
and, consequently, a smaller initial transverse velocity suffices to allow the
electron to return to the ion. Support for these qualitative statements can be
found in the orbits depicted in Fig. 14.
The parameters of the two shortest quantum orbits can be read from Fig. 10
IV] ATI: CLASSICAL TO QUANTUM 71
and compared with the case of linear polarization. For elliptical polarization, the
momentum ks has two nonzero components, kxs and kys. Both have substantial
imaginary parts, in particular ky~. This is a consequence of the lack of a
classical simple-man model for elliptical polarization, as discussed above. For the
orbits ( s - 3, 4) (not shown), the imaginary parts are much smaller, in keeping
with the fact that they make a larger contribution to the spectrum.
Figure 15 presents a corresponding measurement of an ATI spectrum and
displays the staircase structure predicted by the theory. The first step (the one
corresponding to energies below 10 eV) is due to direct electrons and does not
concern us here. The other ones correspond to the steps of Fig. 14. The real
parts of representative orbits, calculated from Eqs. (34)-(36), are shown in the
figure. In order to reach a maximum contrast for the steps, the spectrum was
recorded at 30 ~ to the major axis of the polarization ellipse.
In the lower part of the plateau, the electron can reach a given energy either
directly or after rescattering so that one expects interference of these two paths.
However, Fig. 9 shows that, for linear polarization and high intensity, the
transition region where both paths make a contribution of comparable magnitude
is very narrow. The situation is more favorable for elliptical polarization:
since the plateau turns into a staircase (Fig.14), the yields of the two paths
remain comparable over a larger energy region. This has permitted experimental
observation of this interference effect in the energy-resolved angular distribution
(EAD) (Paulus et al., 2000).
Figure 16 shows a comparison of the EAD's for linear and for elliptical
polarization at the same intensity. For linear polarization, the standard plateau
in the direction of the laser polarization is very noticeable. The side lobes
corresponding to rainbow scattering, mentioned in Sect. III, are also visible.
For elliptical polarization, the plateau has split into two, one to the left of the
direction of the major axis of the field and another weaker one to its right. The
lower panel of Fig. 16 exhibits (on the right) EAD's of a sequence of ATI peaks
where the interference is best developed and (on the left) compares them with
theoretical calculations from the amplitude (29). The parameters underlying the
calculation do not exactly match the experiment. This is mostly attributable
to the insufficient description of the direct electrons for elliptical polarization.
The theoretical results, however, show the same interference pattern. In order
to make sure that this pattern is really due to interference between direct and
rescattered electrons, the two contributions have been displayed separately for
one of the peaks (s = 17): neither one shows a pronounced dip, only their
coherent superposition does. For more details of the theory we refer to Kopold
(2001).
72 W. B e c k e r et al. [IV
FIG. 16. Upper panels: density plots of measurements of the energy-resolved angular distributions
for Xe at an intensity of 7.7 • 1013 W/cm 2 and a wavelength of 800 nm for (a) linear polarization and
(b) elliptical polarization with ellipticity ~ = 0.36. The direction of the major axis of the polarization
ellipse is at 0 ~ Dark means high electron yield. Yields can only be compared horizontally, not
vertically, since the data were normalized separately for each ATI peak. For linear polarization,
the cutoff is at I OUp = 46eV. Lower panels: (a) theoretical calculation from Eq. (29) of the
angular distribution for the ATI peaks s = 11,... ,21 for elliptical polarization (~ = 0.48). The
other parameters are Eip = 0.436 a.u. Oust below the binding energy of xenon in order to stay away
from a channel closing) and I = 5.7 • 1013 W/cm 2. For the ATI peak s = 17, the contributions of the
direct electrons (dashed line) and the rescattered electrons (dotted line) are displayed separately. The
slight variation in the former is unrelated to the interference pattern of the total yield (solid line),
which results from the coherent sum of the two contributions. (b) Experimental angular distribution
extracted from the upper panel (b) of the ATI peaks s - 1 5 , . . . , 25. From Paulus et al. (2000).
V] ATI: C L A S S I C A L TO Q U A N T U M 73
where flu = y(c, v) with v = v(t) the ordinary velocity d x / d t , and the usual
relativistic factor ~, = [1 - ( v / c ) 2 ] - 1 / 2 (not to be confused with the Keldysh
parameter). The four-velocity satisfies ~2 ~ ~ . ~ ~ ~/t~/~ -- C2 SO that
the four-vector mfi is on the mass shell. Equation (46) is the analog o f the
nonrelativistic Eq. (2).
We will consider a plane-wave field o f arbitrary polarization,
2
A" = Z ai(k. x)e; (47)
i=1
u =_ k . x / c o = t - z / c , (48)
From the condition that ~2 = C 2, using the conditions (49), we obtain the energy
as a function of u,
e2
E _ 1+ ( A ( u ) - A(uo))2 (50)
~, - mc 2 2m 2c 2
This is exactly the same decomposition into drift energy and ponderomotive
energy as in the nonrelativistic case, Eq. (3). The ponderomotive energy is
still defined by Eq. (4), and the classical bounds of the spectrum discussed
in Sect. II.A.1 are unchanged. However, velocity and canonical momentum are
connected by the relativistic expresion myv = P r - eA, and the cycle average
was performed with respect to u rather than the time t. Since it can be shown
that u is proportional to the electron's proper time, this was, actually, the proper
thing to do (Kibble, 1966).
The fact that p . k is a conserved quantity implies that the electron's velocity
in the propagation direction of the laser field is given by
The presence of this momentum reflects the fact that a laser photon has a
momentum in the direction of its propagation or, alternatively, that the magnetic
field via the Lorentz force causes a drift in the propagation direction or,
alternatively, that the laser field exerts radiation pressure. All three statements
are essentially equivalent. As a consequence, electrons born with zero velocity in
a relativistic laser field are no longer emitted in the direction of its polarization,
but acquire a component in the propagation direction of the laser so that, for
circular polarization, they are emitted in a cone given by the angle
1
tan 0 - IvT(t)l
2m _ . / 2
(53)
Iv~(t)l Ipr/ Vyo~-1
with respect to the propagation direction. The subscript oc characterizes
quantities outside of the laser field. In the derivation, Eqs. (49)-(52) were used.
The angle 0 has been observed by Moore e t al. (1995, 1999) for intensities
V] ATI: CLASSICAL TO QUANTUM 75
of several 1018 W/cm 2 and ~ = 1.053~tm and was used to draw conclusions
regarding the actual (nonzero) value of the initial velocity (McNaught et al.,
1997), which can be introduced as discussed in the nonrelativistic case in
Sect. II.A. 1. There are, however, still some unresolved issues in the interpretation
of these experiments (Taieb et al., 2001).
The cycle average of Eq. (50) can be written in the covariant form
where p2 and (cA) 2 < 0 are invariant four-dimensional scalar products. This
relation is often used to introduce the so-called "relativistic effective mass" m,.
It occurs very naturally in the context of the Klein-Gordon equation
which explicitly displays the effective mass. However, one has to keep in
mind that this apparently increased mass is just due to the transverse wiggling
motion of the electron, viz. the ponderomotive energy, and that there is nothing
especially relativistic about it. All the same, envisioning the ponderomotive
energy as a mass increase makes sense since, like the rest mass, it is an energy
reservoir that is not easily tapped.
The classical kinematics just discussed are embedded in quantum-mechanical
calculations, which can be carried out along the lines of the strong-field
approximation (17), taking the relativistic instead of the nonrelativistic Volkov
wave function (Reiss, 1990; Faisal and Rado2ycki, 1993; Crawford and Reiss,
1997). In particular, the stationary-phase approximation is well justified, leading
to a form similar to Eq. (21) (Krainov and Shokri, 1995; Popov et al., 1997; Mur
et al., 1998; Krainov, 1999; Ortner and Rylyuk, 2000).
With increasing laser intensity, the first relativistic effect to become significant-
before the ponderomotive potential becomes comparable with the electronic rest
mass - is the drift momentum (52) in the direction of propagation of the laser
field, which can be traced to the Lorentz force. This has virtually no effect on
the initial process of ionization where the electron's velocity is low, but since it
is always positive it prevents the electron from returning to the ion. Therefore,
with increasing intensity it gradually eliminates the significance of rescattering
processes. This effect can be estimated by calculating the distance by which
the electron misses the ion in the z-direction when it returns to the ion in the
76 W. B e c k e r et al. [VI
x - y plane (approximately at the time/ret ~ T/2). From Eqs. (52) and (51) (where,
for simplicity, we only kept Up), we obtain
Up
(Vz) T/2 ~ )~ (56)
2mc 2
with/l the wavelength of the laser field. Obviously, this distance can exceed the
width of the wave packet of the returning electron to the point where it does not
overlap anymore with the ion, even when Up/mc 2 << 1.
In HHG the consequences have been investigated in a number of recent
theoretical works (see Sect. VI.D) and were found to cause a dramatic drop of the
plateau. The same should be expected for high-order ATI, but to our knowledge,
this has not been explored in detail. However, in the analysis of multiple-
nonsequential-ionization experiments of neon at 2 • 10 ~s W/cm 2 a conspicuous
suppression of the highest charge state has been attributed to the magnetic-field-
induced drift (Dammasch et aL, 2001).
According to the rescattering model, the physics of high-order ATI and high-
order harmonic generation differ only in the third step: elastic scattering versus
recombination. Correspondingly, the description in terms of quantum orbits can
be applied to HHG as well; in fact, quantum orbits were introduced for the first
time in the analysis of HHG by Lewenstein et al. (1994). It is from the practical
point of view that the two processes differ greatly: HHG by one single atom has
never been observed, only HHG by an ensemble of atoms. This introduces phase
matching as an additional consideration, equal in significance to the single-atom
behavior (Sali~res et al., 1999; Brabec and Krausz, 2000).
Below we will consider examples of a quantum-orbit analysis of HHG for
several nonstandard situations. The first example is an elliptically polarized laser
field. A bichromatic elliptically polarized laser field was considered by Milogevi6
et al. (2000), and in Sect. VI.C we concentrate on a special case of such a field: a
two-color bicircular field. Finally, in Sect. VI.D the quantum-orbits formalism is
extended into the relativistic regime. A bichromatic linearly polarized laser field
was investigated by Figueira de Morisson Faria et al. (2000), and a simplified
version of the quantum-orbits formalism was used to deal with problems in the
presence of a laser field and an additional static electric field (Milogevi6 and
Starace, 1998, 1999c) or a laser field and an additional magnetic field (Milo~evi6
and Starace, 1999a,b, 2000).
VI] ATI: CLASSICAL TO QUANTUM 77
The matrix element for emission of a photon with frequency fl and polarization e
in the HHG process in the context of the strong-field approximation (Lewenstein
et al., 1994),
Me(f2) " dtl dto d3k exp [iSn(tl, to, k)] me(tl, to, k), (57)
OO
has the same structure as the corresponding expression (31) for ATI. The
function
is the product of two matrix elements: one that describes the ionization at time to
due to interaction with the laser field, and another one at time tl that corresponds
to recombination into the ground state followed by emission of the high-order
harmonic photon having the polarization e. The difference to ATI is mostly in
the first term of the action:
The last equation corresponds to the condition of energy conservation at the time
of recombination and replaces the condition (36) of elastic rescattering in HATI.
For a linearly polarized monochromatic field, quantum orbits were employed
from the very beginning for the evaluation of HHG in the Lewenstein model
(Lewenstein et al., 1994, 1995b) and routinely applied in the theoretical analysis
and interpretation (Sali6res et aL, 1999). Conversely, numerical solutions of the
TDSE were analyzed in terms of the short (rl) and the long (r2) quantum orbit,
and the dominance of these two orbits was corroborated (Gaarde et al., 1999;
Kim et al., 2001). The contributions of the long and the short orbit could be
spatially resolved in an experiment by Bellini et al. (1998). Spectral resolution
was achieved by exploiting the dependence of phase matching on the position of
the atomic jet with respect to the laser focus by Lee et al. (2001) and by Salibres
et al. (2001).
78 W. Becker et al. [VI
24 I (4) I
~ ..- / /// _
~ -2 // -
co
.0
.'.~.7.~.'.~.....~.."~
~..~ ~....... // (2) '
~- -28 -1
o -'-. '.1/- - ,/ .
4
Eo -30 "''"''" "" 9- " ...... ""121
0
_9o
~-32 - - " 'sumlZ 13l2'. ,612""... 1112~__t
, , ~ . . . . a . . . . t.,
" , , , ~ ,""., , , ~ , , ,~tl
" '
30 4O 50 60 70
harmonic order
FiG. 17. High-order harmonic spectrum for an elliptically polarized laser field with the same
parameters as in Fig. 14 and harmonic orders between 25 and 77. The open circles are calculated
from the integral (57), and the curves labeled 1 through 6 represent the individual contributions to
the quantum-orbit approximation of the six shortest quantum orbits, numbered as in Fig. 14. The
contributions from quantum orbits 2, 4 and 6 have to be dropped above their intersections with
curves 1, 3 and 6, respectively. The coherent sum of all six orbits is represented by the solid line.
Typical orbits responsible for each part of the spectrum are depicted as in Fig. 14. From Kopold
et aL (2000b).
see Eichmann et al. (1995) for experimental results and Long et al. ( 1 9 9 5 ) for
a theoretical description. We will call this field "bicircular." This high efficiency
was surprising because, for a monochromatic field, the harmonic emission
rate decreases with increasing ellipticity (cf. the preceding subsection) and a
circularly polarized laser field does not produce any harmonics at all. A more
detailed analysis, based on the quantum-orbits formalism, gives an explanation
of this effect (Milo~evi6 et al., 2000, 2001 a,b). The harmonics produced this way
can be of a practical importance because of their high intensity (Milo~evi6 and
Sandner, 2000) and temporal characteristics (attosecond pulse trains; Milo~evi6
and Becker, 2000). The more general case of an roo-s~o (with r and s integers)
bicircular field was considered by Milo~evi6 et al. (2001 a).
For the laser field (61), selection rules only permit emission of circularly
polarized harmonics with frequencies s = (3n + l)6o and helicities +1.
Similar selection rules govern harmonic generation by a ring-shaped molecule
(Ceccherini and Bauer, 2001) or a carbon nanotube (Alon et al., 2000).
80 W. Becker et al. [VI
.m
t--
~ , i . . . . . . . . . r . . . . . . . . . , . . . . . . . . . r . . . . . . . . . i . . . .
-13
ID
I,._
r
o
~ -15
E
~O
r
o
E
~- -17'
4
O
-19 ...........................................................
10 20 30 40 50 60
harmonic order
Flo. 18. Harmonic-emission rate as a function of the harmonic order for the bicircular laser
field (61) with 09 = 1.6eV and intensities I l = 12 = 4x1014 W / c m 2. The ionization potential is
Eip = 15.76 eV (argon). The inset shows the laser electric-field vector in the x - y plane for times
- 89T ~< t ~< 89T, with T = 23r/o9 being the period of the field (61). The arrows indicate the time
evolution of the field. The ionization time to and the recombination time t I of the three harmonics
Q = 19~o, 31o9 and 43~o are marked by asterisks and solid circles, respectively. These times and
harmonics correspond to the dominant saddle-point solution 2 in Fig. 19. In between the ionization
time (asterisks) and the recombination time (solid circles) the x-component of the electric field
changes from its negative maximum to its positive maximum, whereas its y-component remains
small and does not change sign. From Milo~evi6 et al. (2000).
0.05 . . . . . . . .
2 4 5 7 8 10 11 (a)
1
6 4 52 13 42 15 413
~,- 0 J(7 7 25 ~
24 ~ 7
21
,,.~'~"'~ 25
E
-- 8 17 50,1 1 4
-0.05
0 05 1 15 2
Re (tl-t0)/T
"~ -11
g9 -15 11 ~ ~ ~ ~ . ~ . / "
/
"~___ 4 "" _ _ " , - ~ . \- - " .. .... I
.0
m 9 , \ I
;," "",
t- '...' ,. ~ _ ~ ~ ". " \
',, ,,,s
/ I " ~ ~ ~ ~ ~ ~
O a
,-E -17
9
t-
v
o
o
-19
10 20 30 40 50 60
harmonic order
Fie. 19. Saddle-point analysis of the results of Fig. 18. (a) The imaginary part of the recombination
time tl as a function of the real part of the travel time tl - t o , obtained from the solutions of the
saddle-point equations (34), (35) and (60). Each point on the curves corresponds to a specific value
of the harmonic frequency f2, which is treated as a continuous variable. For the interval of Re(t1 - to)
covered in the figure, eleven solutions were found, which are labeled with the corresponding numbers
at the top and bottom of the graph. Values of the harmonic order that approximately determine the
cutoffs for each particular solution are marked by stars with the corresponding harmonic numbers
next to them. Those values of the harmonic order for which I Im tl] is minimal are identified as
well. (b) The partial contributions to the harmonic-emission rate of each of the first eight solutions
of the saddle-point equations. From Milo~evi6 et al. (2000).
82 W. Becker et al. [VI
/ ,,
,/ "X / \
/ , / \
I \ i X
20 i" "\jl \\
'1 ii '\ x
/ /..---,~.. x
/ XX5
"7'.
-', 0 i
>,,
-20 /
,/ 1
/ ,/
/ t"
-40 .....................................
-20 0 20 40
x [a.u.]
FIG. 20. Real parts of the quantum orbits for the same parameters as in Fig. 18 and for the
harmonic fl = 43r Five orbits are shown that correspond to the saddle-point solutions 2, 3, 4, 5
and 8 in Fig. 19. The direction of the electron's travel is given by the arrows. In each case, the
electron is "born" a few atomic units away from the position of the ion (at the origin), where its
orbit almost exactly terminates. The dominant contribution to the 43rd harmonic intensity comes
from the shortest orbit number 2, whose shape closely resembles the orbit in the case of a linearly
polarized monochromatic field. From Milo~evi~ et al. (2000).
emission decreases with increasing absolute value of the imaginary part of the
recombination time tl. The possible cutoff of the harmonic spectrum can be
defined as the value of the harmonic order after which I Im tll becomes larger
than (say) 0.01T. The probability of HHG is maximal when I Im tll is minimal.
For each solution in Fig. 19a, these points are marked by asterisks and by the
corresponding harmonic order. As a consequence of wave-function spreading,
the emission rate decreases with increasing travel time ti - t o . This gives an
additional reason why the contribution of solution 2 is dominant in the plateau
region.
Let us now consider the quantum orbits. In Fig. 20 for the fixed harmonic
= 43~o, we present the five orbits that correspond to saddle-point solutions
2, 3, 4, 5 and 8 in Fig. 19. The dominant contribution comes from the shortest
orbit 2 (thick line). It starts at the point (4.06, 0.66) by setting off in the negative
y-direction, but soon turns until it travels at an angle of 68 ~ to the negative y-axis.
Thereafter, it is essentially linear, as would be the case for a linearly polarized
field. This behavior can be understood by inspection of the driving bicircular field
depicted in the inset of Fig. 18, where the start time and the recombination time
of the orbit are marked. During the entire length of the orbit, the field exerts
a force in the positive y-direction. The effect of this force is canceled by the
electron's initial velocity in the negative y-direction. The force in the x-direction
VI] ATI: C L A S S I C A L TO Q U A N T U M 83
0
I
, , i , , i ,
Quantum orbits can also be employed in the relativistic regime starting from
the Klein-Gordon equation (55). Milo~evi6 et al. (2001c, 2002) found that
the relativistic harmonic-emission matrix element has a form similar to that in
Eq. (57), but with the relativistic action (h = c = 1)
Sfa(tl, to, k) = L Cx~du (EIp - m - f2) - L tl du ek(u) + ftOcxDdu (EIp - m), (62)
where
k + ~A(u)
ek(u) = Ek + eA(u) 9 (63)
Ek-~.k
equation for Hamilton's principal function it can be shown that ek(u) is the
classical relativistic electron energy in the laser field. In the relativistic case,
the function m E ( t l , t o , k ) in Eq. (57) consists of two parts: the dominant part
is responsible for the emission of odd harmonics ~ = (2n + 1)~, while
the other one originates from the intensity-dependent drift momentum of the
electron in the field and allows for emission of even harmonics ~ = 2n~.
Similarly to the nonrelativistic case, the integral over the intermediate electron
momentum k can be calculated by the saddle-point method. The stationarity
condition ftto' du Oek(u)/Ok = 0, with Oek/Ok = d r / d t , implies r(t0) = r(tl), so
that the stationary relativistic electron orbit is such that the electron starts from
and returns to the nucleus. As above, the start time and, to a lesser degree, the
recombination time are complex.
In the relativistic case, the stationary momentum k = ks is introduced in
the following way. For fixed to and tl, its component ks• perpendicular to the
photon's direction of propagation f~ is given by
tl
(tl - to) k s • =
L du cA(u). (64)
(.A/j2 _ ks2_L)2
k 2 = ks2 + 4 ( m 2 + .A/j2) , (65)
VI] ATI: C L A S S I C A L TO Q U A N T U M 85
-20
~0
~
r
nonrelativistic
= -40
_ _Z [a'u']
-100 -50 0 ~ relativistic
~- -60
t-
O 750 _
ffl
ffl
l
-80
o
.m
t-
O
E
I._
c.- -100
o
T-
O}
0
-120
0 50000 100000 150000
harmonic order
Fie. 22. Harmonic-emission rate as a function of the harmonic order for ultrahigh-order harmonic
generation by an Ar8+ ion (Eip = 422eV) in the presence of an 800-nm Ti:Sa laser having the
intensity 1.5• 1018 W/cm 2. Both the nonrelativistic and the relativistic results are shown. The
corresponding relativistic electron orbit with the shortest travel time that is responsible for the
emission of the harmonic ~ -- 100000o9 is shown in the inset. The arrows indicate which way the
electron travels the orbit. The laser field is linearly polarized in the x-direction and the v • B electron
drift is in the z-direction. From Milo~evi6 et al. (2002).
which yields ek~ as a function of to and tl. The two stationarity equations
connected with the integrals over to and tl are
Another advantage over conventional nonlinear optics is that the nonlinear effect
of photoelectron emission can be observed from more or less any direction,
whereby different properties of the effect can be exploited.
A. CHARACTERIZATION OF H I G H HARMONICS
02F
oc Ipl- m =-~']2 ~f V/2(Eio)2+ moo) O(E - moo - Ei). (68)
OEOff2
Here, ,5'f is the amplitude of the electric field of the fundamental, m is the order
of the sideband, p is the momentum of the photoelectron (]p[ = V/2(Ei + moo)),
and tim is the Bessel function of the first kind. The intensities of the side bands
are not, in general, symmetric. However, for sufficiently weak fields, both fields
can be treated by lowest-order perturbation theory. It follows that a sideband of
,r r m ]
order m is proportional to "~h'~y , where ,5'h is the field strength of the harmonic
radiation. In this case, the cross correlation for a sideband of order m can be
calculated as (X3
w w w w
Fie. 23. Cross-correlation of near-infrared and soft-X-ray pulses. A harmonic of order q creates
photoelectrons at the kinetic energy qho9- Eip. Sidebands are created by simultaneous irradiation
with the fundamental of frequency o9. Plotted are the heights of the sidebands for various side-band
orders m versus the delay r between the fundamental and the harmonic. The solid line represents
the analytical approximation (69), whereas the points were calculated by numerically solving the
appropriate (one-dimensional) Schr6dinger equation. In each case, the analytical approximation was
normalized to the maximum of the numerical result.
1.35 fs,
i
10
2~.50 as
5
0 , ! 9
0 ~1 ,,,~ 3 ', 4 " 5
\ I
\ I
, \ /
,, t i m e [fs] ' \ /
'
FIG. 24. Reconstruction of a train of attosecond pulses synthesized from the five harmonics
q = 11 . . . . . 19. The attosecond pulses are separated by 1.35 fs, which is half the cycle time of the
driving laser. The latter is represented by the dashed cosine function. Reprinted with permission from
Paul et al. (2001), Science 292, 1689, fig. 4. 9 2001 American Association for the Advancement
of Science.
can be generated by absorption of the lower harmonic plus one NIR photon
(Eq -- ( q - 1)ho) + boo) or by absorption of the upper harmonic and emission
of one NIR photon (Eq = (q + 1)hco- ha)). Each of these two channels receives
contributions from two different quantum paths, which are related to the temporal
order of the interaction with the harmonic and the NIR field. (In contrast to
the quantum orbits we considered elsewhere in this chapter, the quantum paths
here are defined in state space rather than position space.) The photoelectron
yield at energy Eq is proportional to the square of the (coherent) sum of the
amplitudes of all four quantum paths. Due to the fact that two paths represent
absorption from the NIR field whereas the other two represent emission into it,
the interference term between these two contributions is essentially proportional
to cos(~q_l --~q+l 4- 2htor). By varying the delay r between the harmonic and
the NIR radiation, the difference ~q-1 --~q+l of the phases of the two harmonics
can be recorded. The result of the corresponding experiment (Paul et al., 2001)
is that the phase of the harmonics depends almost linearly on their frequency.
Hence, the harmonics considered in the experiment (q = 11 to 19) are mode-
locked and make up a train of attosecond pulses of 250 as FWHM duration, see
Fig. 24.
regime). Then, however, the spectral width of the harmonics will be so broad
that it is no longer possible to identify individual sidebands as necessary for the
method of Paul et al. (2001).
Nevertheless, Drescher et al. (2001) and Hentschel et al. (2001) succeeded
in performing measurements of the harmonic-pulse length with a resolution of
1.8 fs and 150 as, respectively. The experimental setup, in principle, resembles
that of Paul et al. with the difference that higher intensities of the NIR ra-
diation are used for the photoionization cross correlation. In addition, only
photoelectrons ejected perpendicularly to the laser polarization are detected.
The motivation for choosing these conditions can be deduced from a classical
analysis of trajectories of electrons that were injected into the electric field of
the few-cycle NIR pulse by absorption of a harmonic photon. If the duration of
the X-ray pulse is shorter than the optical period T in the NIR, then the final
kinetic energy of the photoelectrons depends on the phase tot0 when the injection
took place, i. e. it exhibits a modulation with a period of T/2. By delaying
the fundamental with respect to the harmonic, the modulation can be recorded.
This was done in the experiment of Drescher et al. (2001). Hentschel et al.
(2001) realized that the width of the photoelectrons' kinetic energy distribution
also exhibits such a modulation, and is measureable with much higher precision
than the center of mass of the distribution. For the two approaches, it is not the
envelope of the fundamental that enters the correlation function, but rather the
optical period. The restriction to photoelectrons emitted perpendicularly to the
laser polarization suppresses the influence of effects related to the emission and
absorption of photons from the laser field, i.e. the sidebands which were crucial
for the experiment of Paul et al. (2001).
The need for highest intensities and extremely broad bandwidths in several areas
of the natural sciences is driving the development to shorter and shorter laser
pulses. At a FWHM duration shorter than a few optical cycles the time variation
of the pulse's electric field depends on the phase q~ of the carrier frequency with
respect to the center of the envelope, the so-called "absolute phase." The electric
field should be written as
where the function g0(t) is maximal at t = 0. Clearly, for a long pulse the phase q~
can be practically eliminated by resetting the clock. For a short pulse, however,
the shape of the field (70) strongly depends on this phase, which, therefore, will
influence various effects of the laser-atom interaction. This is one reason for the
significance of this new parameter of laser pulses. The precise knowledge and
control of the absolute phase will pave the way to new regimes in coherent X-ray
VII] ATI: CLASSICAL TO QUANTUM 91
FIG. 25. Evidence of absolute-phase effects from few-cycle laser pulses. In this contingency map,
every laser shot is recorded according to the number of photoelectrons measured in the left and
the right arm of the "stereo" ATI spectrometer. The number of laser shots with electron numbers
according to the coordinates of the pixel is coded in grey shades. For visual convenience the darkest
shades were chosen for medium numbers of laser shots. (The most frequent result of the laser pulses
was about 5 electrons in each of both arms.) The signature of the absolute phase is an anticorrelation
in the number of electrons recorded with the left and the right detector. In the contingency map they
form a structure perpendicular to the diagonal. Shown here is a measurement with krypton atoms
for circular laser polarization, a pulse duration of 6 fs, and an intensity of 5 x 1013 W/cm 2. From
Paulus et al. (2001b).
In a recent experiment, Paulus et al. (2001b) were able to detect effects due
to the absolute phase by performing a shot-to-shot analysis of the number of
photoelectrons emitted in opposite directions. To this end, a field-free drift tube is
placed symmetrically around the target gas. Each end of the tube is equipped with
an electron detector. Because of its characteristic appearance, this was dubbed a
stereo-ATI spectrometer.
A characteristic feature of few-cycle pulses such as (70) is that, depending
on the absolute phase, the peak electric-field strength (and thus also the vector
potential) is different in the positive and negative x-directions. Recall from
Eq. (2) that the electron's drift momentum depends on the vector potential at
its time of birth. Therefore, depending on the value of the absolute phase,
such a laser pulse creates more electrons in one direction than in the other.
A theoretical analysis of the photoelectrons' angular distribution was given by
Dietrich et al. (2000) and Hansen et al. (2001) for the nonperturbative intensity
regime. Interestingly, the effect is predicted to be much less pronounced in the
perturbative regime (Cormier and Lambropoulos, 1998). Equivalent to a left-
right asymmetry of the photoelectron angular distribution is that the number
of electrons emitted to the left vs. those emitted to the right is anticorrelated:
A laser shot for which many electrons are seen at the right detector is likely to
produce only a few that go left, and vice versa. This can be proved by correlation
analysis. Each laser shot is sorted into a contingency map according to the
number of electrons recorded at both detectors. Anticorrelations can then be seen
in structures perpendicular to the diagonal, see Fig. 25.
VIII. Acknowledgments
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98 W. B e c k e r et al. [IX
I. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 99
II. Background . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 101
A. Trapping Cold Atoms using Repulsive Dipole Forces . . . . . . . . . . . . . . . . . 101
B. Loading Atoms into Dark Optical Traps . . . . . . . . . . . . . . . . . . . . . . . . . . 103
C. Hollow Laser Beams . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 104
III. Multiple-Laser-Beams Dark Optical Traps . . . . . . . . . . . . . . . . . . . . . . . . . . . 106
A. Adding Beams Incoherently: Light-sheets and Hollow-beam Traps . . . . . . . . 107
B. Evanescent-wave Traps . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 109
C. Using Interference: Dark Optical Lattices . . . . . . . . . . . . . . . . . . . . . . . . . 111
IV. Single-Beam Dark Optical Traps . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 113
A. Generating Dark Volumes using Refractive Optical Elements: Axicon Traps . . 113
B. Creating Single-beam Dark Traps with Diffractive Optical Elements . . . . . . . 115
C. Scanning-beam Dark Optical Traps . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 122
D. Comparing Different Traps . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 124
V. Applications . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 127
A. Manipulations in Phase Space: Cooling and Compression . . . . . . . . . . . . . . 127
B. Precision Measurements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 136
C. Dynamics of the Trapped Atoms . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 141
VI. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 147
VII. References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 148
I. I n t r o d u c t i o n
Trapping of neutral atoms has become possible in the last 15 years, thanks to the
advances in laser cooling techniques (Adams and Riis, 1997). Several kinds of
traps were developed and investigated (Balykin et al., 2000), the most useful ones
being magnetic, magneto-optical and dipole force traps. Optical dipole traps use
the interaction between the electric field of the light and an electric dipole, which
is induced in the atom by this field. This force is weaker than the magneto-optical
and magnetic forces, and typical dipole trap depths are below 1 mK. These traps
offer the possibility to trap atoms in all internal states, as well as a possibility
to lower the dissipative component of the interaction between the atoms and the
trapping light by increasing the detuning of the laser from the atomic resonance
(which also unavoidably reduces the depth of the trapping potential). These traps
and their properties have been described in a recent review by Grimm et al.
(2000).
Fla. 1. Fluorescence images of atoms in optical dipole traps. (a) Atoms trapped inside a
red-detuned trap; imaging is performed when the trapping beam is on. Atoms close to the focus of
the trapping beam are not observed, since they experience a large ac Stark shift, which shifts them
out of resonance with the probe beam. (b) Same as (a), but imaging is performed a short time after
the trapping beam is shut off. All atoms are detected. (c,d) Atoms trapped inside a blue-detuned trap,
with the same detuning and laser power as those of the red-detuned trap. All atoms are observed,
irrespective of whether the trapping beam is on (c) or off (d), indicating reduced perturbation in this
dark trap.
To further reduce the interaction between the atoms and the trapping laser,
dark optical traps were developed, in which the atoms are trapped by a repulsive
dipole interaction with the laser. The repulsive force is achieved by detuning the
trapping laser above the atomic resonance, such that there is a phase difference
between the field and the induced dipole. In these dark optical dipole traps,
cold atoms are trapped inside a dark region which is surrounded by a repulsive
dipole potential wall. To visualize the lower perturbations that are observed by
atoms inside a dark optical trap, consider Fig. 1, in which fluorescence images
of trapped atomic clouds are presented, for both attractive and repulsive optical
dipole traps. In the attractive (red-detuned) trap, atoms around the b e a m focus
are not observed, since they are shifted out of resonance with the fluorescence
beams, due to the large ac Stark shift induced by the trapping laser. W h e n the
measurement is repeated just after the trapping b e a m is shut off, these atoms
are easily observed. For the repulsive (blue-detuned) dark trap, which had the
same laser power, the same detuning and the same dimensions, there is no
II] DARK OPTICAL TRAPS FOR COLD ATOMS 101
difference between the measurements with and without the trapping beam. This
result indicates that perturbations due to the trapping beam are largely suppressed
for dark traps. Throughout this review we will present quantitative evidences for
this suppression.
Experimentally, dark traps (also called "blue-detuned" traps) are harder to
realize than attractive (or "red-detuned") dipole traps, where already a single
focused beam constitutes a trap. Several configurations have been demonstrated,
the first of which used multiple laser beams to form a confinement by light in
three dimensions, or used repulsive light structures to support the cold atoms
against gravity, which provided the trapping potential in the vertical direction.
Later, simpler trap designs were realized, which use only a single laser beam,
and traps with optimized properties were designed for various applications.
In this review, we describe dark optical traps, the techniques in which they
are experimentally realized, and their main applications in atomic physics. We
start with a short background section discussing the optical dipole force and
the process of loading cold atoms into the trap. We also describe hollow laser
beams, methods by which they can be formed, and their application as atom
guides, which confine atoms in two dimensions. In Sect. III we discuss dark
traps created using multiple laser beams, including gravito-optical traps, traps
that use evanescent light fields as the confining walls, and far-detuned dark
optical lattices. In Sect. IV, single-beam dark optical traps are considered, with
special emphasis on the optical techniques used in their construction. In both
sections, the focus is on trap designs that have been experimentally realized,
and the measured properties of the trapped atomic ensembles are described. In
Sect. V, the main applications of dark traps are discussed, including advanced
laser-cooling methods for dense atomic samples, the use of dark traps as a
favorable environment for precision spectroscopy, and the study of the dynamics
of trapped atoms.
II. Background
A. TRAPPING COLD ATOMS USING REPULSIVE DIPOLE FORCES
Light can exert a force upon atoms by momentum exchange due to photon
absorption and emission. The force that a laser field applies on an atom is usually
separated into two terms which correspond to a scattering force and a dipole
force. The scattering force results from absorption followed by spontaneous
emission of a photon in a random direction. The average momentum exchanged
is therefore one photon momentum, hkL, in the direction of the absorbed photon
(kf = 2:r//~, where/~ is the wavelength of the laser). In the case of the dipole
force, the photon is emitted in a stimulated way into a mode of the laser field. The
momentum transfer in this case is the vector difference between the momenta
of the absorbed and emitted photons.
102 N. Friedman et al. [II
For a two-level atom, the forces can be calculated by using the solutions of
the optical Bloch equations, while translational degrees of freedom are taken into
account (Cohen-Tannoudji et al., 1992). The resulting expression for the average
scattering force is then
The last term is equal to Eq. (12) of Grimm et al. (2000), which was derived for
the classical oscillator model of the atom, using the rotating wave approximation.
The same result can also be derived in the dressed-state model, where the
combined Hamiltonian for the atom and the laser field is solved. (See, for
example, Cohen-Tannoudji et al., 1992). Equation 4 indicates that the dipole
potential is proportional to the laser intensity and inversely proportional to its
detuning. Comparing the expressions for the dipole force and scattering rate,
under the above approximations, yields the relationship
Udipole _ ~, (5)
h),s ),
which means that a trap with a reduced scattering rate can be made by increasing
the detuning while maintaining the ratio I/6.
II] DARK OPTICAL TRAPS FOR COLD ATOMS 103
The usual loading scheme of atoms into optical dipole traps starts with a
magneto-optical trap (MOT) (Raab et al., 1987), which traps atoms from a
vapor or an atomic beam and cools them to a typical temperature of 100 ~tK.
Since most dipole traps are relatively shallow and small as compared with the
MOT, it is advantageous to further cool the atoms and increase their density
in order to enhance the loading efficiency. The loading of red-detuned dipole
traps was thoroughly investigated both for trapping laser detunings of few nm
(or -3 • 105 V) (Kuppens et al., 2000), for larger detunings (~ 1 • 107 V) (Han et al.,
2001), and also for CO2 laser traps (O'Hara et al., 2001), where the detuning
is comparable to the atomic resonance frequency. In the CO2 trap, spatial and
phase-space densities much higher than that of a MOT are achieved, a fact that
led recently to the first demonstration of a Bose-Einstein condensate (BEC)
created in an all-optical way (Barrett et al., 2001).
There are some differences in the loading process between red- and blue-
detuned dipole traps. For red-detuned traps, the atoms are loaded into a region
of high trapping light intensity, which may interfere with the loading process.
The trap may reduce the optical cooling efficiency, since it results in a spatially
inhomogeneous Stark shift of the cooling line. The level shifts may influence also
104 N. Friedman et al. [II
the photon reabsorption since both the spontaneous emission and the absorption
spectra are altered. Combined with the trap's potential, which is usually steeper
than that of the MOT, it can result in a higher atomic density in the trap.
For blue-detuned traps, the loading seems to be simpler since the atoms
are loaded into a dark region, hence their interaction with the trapping light
is much smaller than their interaction with the MOT. This is supported by
several experimental observations. First, in many experiments the density and
temperature of the atoms loaded into the dark trap are very close to those in the
MOT. Second, the number of trapped atoms almost does not change if the trap is
present during the whole loading stage, or is turned on just at the end of the MOT
operation. These findings suggest that the loading is purely geometrical - those
atoms that are inside the dark "box" will stay there, those outside the box will not
be trapped, while the trap does not interfere with the operation of the MOT. The
different loading mechanism of bright and dark dipole traps is emphasized by an
experiment where atoms are first loaded from a MOT into a red-detuned dipole
trap, and are then transferred into an overlapping dark trap. In this manner, an
increase of about x2.5 in the number of atoms in the dark trap was observed,
as compared to direct loading of the dark trap from the MOT (Friedman et al.,
200 l a). This indicates that the red-detuned trap can enhance the atomic density,
while the dark trap leaves it almost unchanged. In this way, a dark trap may be
used as a probe for investigating loading into other traps, since it can sample
the atomic density and temperature at a given time. The advantage is that the
measurement can be performed at a later time, when the MOT atoms that were
not trapped have expanded and have fallen out of the detection region.
C. HOLLOWLASER BEAMS
where P is the total laser power, the waist size is w ( z ) = w0v/1 + (2/ZR) 2, and
zR = :rw2/)~ is the Rayleigh range. The phase of the beam changes linearly with
the azimuthal angle, 0, and there is a phase singularity on the beam axis. These
modes were extensively studied in the last decade, mainly due to their special
property of having orbital angular momentum lh per photon. For a review of this
subject see (Allen et al., 1999).
LG modes were generated experimentally from high-order Hermite-Gaussian
modes (which are easy to produce directly from laser resonators), by a
mode converter composed of two cylindrical lenses (Beijersbergen et al., 1993).
Such a cylindrical-lens mode converter was used to produce a LG g mode that
was part of a 3D dark optical trap (Kuga et al., 1997), as will be discussed in
Sect. III.A.
LG modes were generated also by using a computer generated hologram,
with a "fork" in the grating pattern. When illuminated with a plane-wave (or
a TEM00 laser beam), a "charge-one" phase singularity will be created in the
beam, centered around the fork defect. The resulting 1st diffraction order is a
good approximation of the required LG~ field distribution, although it is not a
pure mode (Heckenberg et al., 1992).
Such computer-generated holograms were used to create hollow beams which
served as guides for cold atoms (Kuppens et al., 1998; Schiffer et al., 1998).
In these experiments, metastable neon atoms were guided inside a focused LG~
hollow beam, a first demonstration of guiding cold atoms in free space 2. Atoms
were guided along a distance of 30cm and focused to a spot size o f - 6 . 5 ~tm.
Polarization-gradient cooling (PGC) in the transverse direction was applied in
order to further increase the phase-space density (see Sect. V.A.1). In later
experiments, a BEC was adiabatically transferred into a hollow LG 1 beam and
its propagation inside this optical guide was studied (Bongs et al., 2001).
A TEM00 Gaussian beam will be projected with a high efficiency onto a
LGt0 beam when it passes through a spiral phase element having a transmission
1 Another example for structurally stable hollow beams is constituted by high-order Bessel beams,
which are non-diffractive and were considered as atom guides (Arlt et al., 200 l b).
2 Cold atoms have been guided previously with light propagating inside hollow fibers (Balykin,
1999).
106 N. F r i e d m a n et al. [III
During the last decade, several types of dark optical traps were proposed and
demonstrated. The first dark traps were formed by incoherently adding several
laser beams that served as the trap's walls. These first traps were shallow and
had a relatively small volume, hence captured only a modest number of atoms.
However, these first experiments demonstrated the main advantages of dark traps,
namely low photon scattering rates and long coherence times of the trapped
atoms. Later improvements in trap design led to traps with larger volumes, in
which large number of atoms could be captured and manipulated. In this chapter,
traps based on multiple laser beams are described in a comparative way. The main
dark-trap designs are considered, and the performance of experimentally realized
traps is discussed. In order to compare traps made for different atomic species
on a common basis, trap properties are given in a normalized way: the detuning
is normalized by y (the linewidth of the relevant excited state) and the trap depth
is normalized by the recoil energy of the atom, Erec = hZk~/2m, where m is the
mass of the atom.
In the first dark optical dipole trap for cold atoms, realized in 1995 in Stanford
(Davidson et al., 1995), sodium atoms where trapped using light from an Ar-ion
laser. This trap consisted of two elliptical light sheets (generated by focusing
a Gaussian beam with a cylindrical lens) intersecting at 90 ~ and forming a
"V"-shaped cross section. Confinement was provided by gravity in the vertical
direction and by the beams' divergence in the longitudinal direction. The two
beams had powers of 4 and 6 W, were linearly polarized, and had different wave-
lengths (488 and 514.5 nm) so that they did not interfere in the overlap region and
formed a smooth potential. The large detuning of the trap beams, ~ 107 y, resulted
in a relatively low potential of ~10E~ec, and hence a low number of trapped
atoms (~3000), but also an extremely low photon scattering rate, calculated as
~ 10-3 s-1 , and a long lifetime of 5 s, limited by the background vacuum. A spec-
troscopic measurement of the hyperfine splitting of Na, which was performed on
the trapped atoms (see Sect. V.B), yielded a coherence time of 7 s. This coher-
ence time was 300 times longer than that achieved in a red-detuned trap having
the same potential height and a larger detuning, emphasizing the advantage of
a dark trap for precision measurements. The coherence time was limited by
inhomogeneous broadening, since different atoms acquire different Stark shifts,
depending on the velocity distribution and the dynamics of the trapped atoms.
In a later work (Lee et al., 1996), this trap was improved by intersecting two
such "V" traps at a right angle, resulting in an inverted-pyramid trap (see Fig. 2).
The polarization of the beams in the second pair was rotated by 90 ~ with respect
to the first in order to prevent interference in the trapping region, which would
lead to trap loss. A much larger number of atoms (4.5 • 105) were confined in this
trap, and its shape produced coupling between the motion in all three dimensions.
This allowed cooling in three dimensions by applying one-dimensional Raman
cooling (see further discussion in Sect. V.A.2). The issue of atom dynamics
108 N. F r i e d m a n et al. [III
FIG. 2. Schematic illustration of the inverted pyramid dark optical trap, which is composed of
four blue-detuned light sheets. (From Lee et al., 1996, Phys. Rev. Lett. 76, 2658, Fig. 1).
FIG. 3. Schematic illustration of the dark hollow beam trap, which is based on a hollow
Laguerre-Gaussian beam and two plugging beams. (From Kuga et al., 1997, Phys. Rev. Lett.
78, 4713, Fig. 2).
and its possible implication for cooling and spectroscopy will be discussed later,
Sect. V.C.
A different trap configuration was demonstrated by Kuga et al. (1997): it
consisted of a hollow laser beam (LG 3) and two additional "plug" beams that
confined the atoms in the propagation direction of the hollow beam (see Fig. 3).
The hollow beam had a power of 600 mW and a radius of 600 ~m. A detuning
of ~1047 resulted in a potential of ~100Erec, higher than the typical energy of
PGC-cooled Rb atoms. The deep potential, combined with a very large volume
of 2 • 10-3 cm 3, enabled the loading of a much larger number of atoms (1 • 108),
with a very good loading efficiency of about one-third from the MOT. However,
the relatively small detuning resulted in a high photon scattering rate of~100 s-1 ,
which limited the lifetime of the trap to 150 ms due to heating of the atoms above
the potential barrier. To reduce this heating effect, pulsed PGC was applied,
resulting in a longer lifetime of 1.5 s (Torii et al., 1998).
There have been several proposals for traps using a vertical hollow beam
combined with a horizontal plug beam that supports the atoms against gravity,
so forming a gravito-optical trap (Morsch and Meacher, 1998; Yin et al., 1998).
The hollow beam can be produced in either of the ways discussed in the previous
section, and can be focused to create a conical shape, forming a funnel that
III] DARK OPTICAL TRAPS FOR COLD ATOMS 109
potentially increases the loading efficiency from a MOT into the dipole trap.
These proposed schemes suggest the use of inelastic reflection of atoms from
the trapping light (reflection Sisyphus cooling, see Sect. V.A.3) to reduce the
relatively high kinetic energy of atoms that fall from the MOT into the trap,
and also to balance the heating due to spontaneous photon scattering. A similar
configuration was used by Webster et al. (2000): 103 Cs atoms were trapped
above the focus of a vertical LG 1 beam from an Ar-ion laser. No plug beam was
used here, but the loss of atoms through the very small hole at the bottom of the
trap is negligible due to the relatively high temperature of the atoms. The trap
was loaded from a magnetic trap, in which evaporative cooling was performed
to lower the kinetic energy of the atoms below the dipole trap potential. Since
no reflection cooling occurs at this large detuning, gravity was balanced by a
magnetic field gradient, such that atoms were falling very slowly into the dark
trap.
B. EVANESCENT-WAVE TRAPS
A = (7)
2~ V/n 2 sin 2 0 - 1
repumping l l
beam ,~::z~,,..~]
atoms in MOT V ~ ; [
1 1 evan.
atoms in GOST " ~ T wave
P D
v F=4
9.2 GHz
,~ F=3
dielectric vacuum
EW laser W ~
beam hollow beam
(a) (b)
FIG. 4. (a) Schematic illustration of the experimental setup of the gravito-optical surface trap.
The trap is formed by an evanescent light wave that supports atoms against gravity, and a hollow
beam that provides confinement in the horizontal direction. (From Ovchinnikov et al., 1997, Phys.
Reu. Lett. 79, 2225, Fig. 1). (b) The reflection cooling cycle, with the relevant energy levels for the
Cs D 2 line. An atom moves towards the mirror in the lower hyperfine level (F -- 3). Close to the
classical turning point, it may undergo a spontaneous Raman transition to the upper level ( F - 4), by
scattering a photon from the evanescent wave. It is then reflected from the mirror along the lower
potential observed by the upper level. The cycle is closed by spontaneous scattering of a photon
from a repumping beam, which takes the atom back to the lower level. (From Engler et al., 1998,
Appl. Phys. B 67, 709, Fig. 2).
(induced by the surface curvature). The trap's lifetime was ~lOOms, limited
mainly by scattering o f stray light from the surface, which either heats the atoms
or optically pumps them into a state for which the potential is weaker, hence the
effective area o f the mirror is smaller.
In order to form a trap with a longer lifetime and a better confinement, a
vertical hollow beam was added to confine the atoms in the horizontal direction,
as shown in Fig. 4a (Ovchinnikov et al., 1997). In this trap, the evanescent wave
was produced using a 6 0 - m W laser b e a m which was detuned by only ~ 2 0 0 7 from
the lower hyperfine level of the atomic ground state, creating a potential barrier
of 104Erec for that level (taking into account the van der Waals interaction
with the surface). For the upper hyperfine level, the detuning is larger by the
hyperfine splitting ( - 1 7 5 0 y in Cs), hence the potential is lower. The different
potential for these two levels is used in the reflection Sisyphus cooling to be
discussed in Sect. V.A.3. The 1 2 0 - m W hollow b e a m had a radius o f 360[am
and a characteristic ring width o f w0 - 18 [am. It was detuned by 0.3 n m from
resonance (6 = 2 x 104) ,) and produced a potential barrier o f ~500Erec. The high
potential barrier and large volume m a d e it possible to trap a large n u m b e r o f
Cs atoms: 2 x 105 in the first experiment, which was later increased up to 2 x 107
by improving the loading scheme o f the M O T ( H a m m e s et al., 2000). From a
III] DARK OPTICAL TRAPS FOR COLD ATOMS 111
measurement of the heating rate of the trapped atoms, the upper bound for the
total photon scattering rate in this trap was calculated to be 50 s -1.
The large number of atoms at relatively low temperature and high density
make this trap a good candidate for evaporative cooling towards quantum
degeneracy in an all-optical way in a dark trap. Evaporative cooling of Cs atoms
was indeed demonstrated by lowering the potential height, as will be discussed in
Sect. V.A.4. Due to the very different confinement in the vertical and horizontal
directions, this trap has some promising applications in the investigation of
quantum degeneracy of a 2D gas (Petrov et al., 2000). For this purpose, the
atoms can be confined more tightly in the vertical direction by adding a red-
detuned evanescent wave that will create a narrower potential well (Engler et al.,
1998), or by adding a vertical standing wave above the surface. In this scheme,
an atom falls on the evanescent wave and at the turning point is transferred by
a spontaneous Raman transition to a different internal state, which is uncoupled
from the evanescent wave but is coupled to the standing-wave potential that has
a minimum at this point. Such a scheme was demonstrated experimentally with
metastable Ar atoms, which were preferentially loaded into a single potential well
of a red- or blue-detuned standing wave with an increase of 100 in spatial
density (Gauck et al., 1998). This scheme can be extended to alkali atoms by
a proper choice of laser polarizations, as discussed by Spreeuw et al. (2000).
Finally, the evanescent-wave surface trap can also be used to explore atom-
surface interaction, which is of theoretical as well as practical importance for
various atom-optics devices such as waveguides and traps close to surfaces.
Cold atoms can be trapped in the dark nodes of interference patterns of blue-
detuned light. Only three-dimensional (3D) blue-detuned optical lattices will
provide 3D trapping, while even a 1D red-detuned optical lattice is capable
of confining atoms in three dimensions. In a first demonstration of a 3D dark
optical lattice, lithium atoms were trapped in a non-dissipative way (Anderson
et al., 1996). The lattice was formed by the interference of four intersecting laser
beams, detuned either to the red (10 nm) or to the blue (1 nm, or - 1 x 105 y) of
the atomic resonance. Typical lifetime of the trapped atoms was on the order
of 50ms, limited by heating due to photon scattering with a scattering rate of
~100s -1. This scattering rate is relatively high as compared to far-detuned dark
optical traps since the lattice potential height was comparable to the kinetic
energy of the atoms, so no effective "darkness factor" was obtained 4.
4 Note that a higher potential is needed for trapping the lighter Li atoms, since the typical momenta
of laser-cooled alkalis are comparable, resulting in a higher kinetic energy for the lighter atoms.
112 N. Friedman et al. [Ill
ysO, 9 (t + m + n + 3 ) .
With the experimental parameters, gs was as low as 6 S-1 for the (0, 0, 0) ground
band. Another band-dependent loss mechanism is tunneling of a trapped atom
to a neighboring lattice site, and eventually out of the lattice by diffusion. The
detuning of the lattice beams was 6 = 2.5x 105,/, and the trap depth was
54Erec, not much higher than the initial kinetic energy of the atoms. Due to
the low potential, only the lowest bands with l, m, n ~< 3 are bound and initially
populated, with a total number of 104 atoms. The RMS momentum of the atoms
remaining in the trap decreased as a function of trapping time, indicating the
band-dependent loss described above. The population in each band was resolved
by ramping down the potential slowly such that higher lying bands were released
first, and atoms in the lower state were released in a later, resolvable time.
The decay time for the lowest band was found to be 0.31 s, as compared to
0.13 s for the next-higher band, leading to a preparation of an atomic sample in
the ground band after about 0.45 s of storage in the lattice. Since the preparation
was done by selection and not by cooling to the ground state, only a very small
number of about 50 atoms were trapped in the ground state.
Muller-Seydlitz et al. (1997) constructed the lattice by three orthogonal
standing waves with mutually orthogonal linear polarizations. Since the atoms
are trapped in a J = 0 state, the dipole potential is independent of the local
polarization of the light and is proportional to the sum of intensities. For atoms
in a J ;~ 0 state, the relative phases of the three orthogonal standing waves have to
be stabilized. Alternatively, standing waves with a frequency difference between
them can be used such that on average the polarization is linear (DePue et al.,
1999; Chin et al., 2001), or an inherently stable configuration with only four
beams can be used, as did Anderson et al. (1996).
A related proposal describes a way of producing a 1D blue-detuned optical
lattice using two counter-propagating Gaussian beams with different waists such
that confinement is achieved also in the radial direction (Zemanek and Foot,
1998). Here, as opposed to the 3D lattice, the intensity in the nodes is zero
only at z = 0, where the waists of the two waves are located, and the intensities
are equal. Out of this plane the two waves have different divergence angles due
to the different waist sizes, resulting in a gradual increase in the intensity at
the well bottom and a decrease in the darkness factor. Since the confinement in
IV] DARK OPTICAL TRAPS FOR COLD ATOMS 113
the radial direction results from non-perfect destructive interference, the radial
potential depth is much smaller than that in the longitudinal direction.
Dark optical lattices are promising candidates for performing precision
measurements, such as of the electron's permanent electric dipole moment, as
discussed recently by Chin et al. (2001), and to be described in Sect. V.B. Finally,
far blue-detuned optical lattices have attracted much attention as a possible
system for the realization of quantum information processing (Brennen et aL,
1999). Here, the main advantages are the low interaction of an atom with its
environment leading to long coherence time, and the possibility to control the
interactions between individual atoms to induce entanglement.
In this section we describe dark optical traps created with a single laser beam.
These traps are simpler to align than traps using several beams, hence it is
easier to optimize the trap properties. The simplicity of these traps also permits
easy manipulation and dynamical control of the trapping potential, its size and
its shape. As opposed to the 2D case, where any desired light distribution can
be generated using diffractive or refractive optical elements, there is no simple
procedure to design an arbitrary 3D light distribution. Actually, there are not
enough degrees of freedom in the design of an optical element to achieve a
full 3D arbitrary light distribution 5. Nevertheless, with the combined use of
refractive and holographic optical elements, it is possible to extend the methods
described in Sect. II.C in order to produce light distributions which are suitable
for trapping atoms in the dark using a single laser beam. Such light distributions,
which comprise of a dark volume completely surrounded by light, were realized
using either combinations of axicons and spherical lenses, diffractive optical
elements, or rapidly scanning laser beams. The following subsections describe
the various trap designs, and analyze the properties of the resulting traps. In the
last subsection, traps of different classes are compared quantitatively.
5 This issue has been discussed, for example, by Piestun and Shamir (1994), Spektor et al. (1996)
and Shabtayet al. (2000), who designed hologramsthat produce some specific 3D light distributions,
and discussed the limits of these design procedures.
114 N. F r i e d m a n et al. [IV
Fic. 5. Schematic illustration of the conical beam optical trap. The conical hollow beam, directed
upwards, is generated with two equal axicons (an "axicon telescope") and a spherical lens. (From
Ovchinnikov et al., 1998, Europhys. Lett. 43, 510, Fig. l a).
light facing upward was realized (Ovchinnikov et al., 1998). The optical setup,
illustrated in Fig. 5, consisted of two axicons with identical angles (an "axicon
telescope") followed by a spherical lens. As opposed to the funnel trap described
previously (Sect. III.A), the apex of the cone in this case is not hollow and
no plug beam is needed. In the experiment, a 250-mW laser beam was used
to form the conical trap with an opening angle of 150mrad. The detuning of
the laser was 3 GHz (6 = 560),) with respect to the lower hyperfine level of
Cs (F = 3), producing a potential barrier o f ~ 3 x 10SErec in the focal plane (apex
of the cone), decreasing linearly with height. The trap was loaded from a MOT
located 5 mm above the apex. A Cs atom that falls 5 mm acquires a kinetic energy
o f - 8x 103Erec and hence is easily confined by the trap potential. Six molasses
beams were left on during the experiment, to realize a combined polarization gra-
dient cooling and reflection Sisyphus cooling. The measured loading efficiency
from the MOT into the trap was very high, ~ 80%, resulting in -8 x 105 atoms in
the trap, at a temperature of-10Trec. The trapped atomic cloud had an elongated
shape with a length of about 1 mm in the vertical direction, and a radial size of
100 ~tm. Two drawbacks of this trap are the high photon scattering rate from the
conical beam, ~3 x 103 s-1 , and the poorly defined potential shape near the apex
[probably caused by interference (Webster et al., 2000)]. This can be inferred
from the elongated shape of the resulting atomic cloud, which does not compress
towards the apex as would be expected from the equipartition of energy.
Recently, a related scheme producing a 3D single-beam dark trap has been
demonstrated by two groups (Cacciapuoti et al., 2001; Kulin et al., 2001). This
scheme uses a single axicon placed between two spherical lenses (see Fig. 6).
IV] D A R K OPTICAL TRAPS F O R C O L D ATOMS 115
FIG. 6. Schematic illustration of the experimental setup for a single-beam dark optical trap, based
on an axicon and two spherical lenses. The axicon and the first lens provide a virtual image of the
trap (with radius r) indicated by the dashed lines, which is imaged by the second lens to form the
dark trap (with radius R). (From Cacciapuoti et al., 2001, Eur. Phys. J. D 14, 373, Fig. 1).
After passing through the first lens, a divergent Gaussian beam hits the axicon.
The second lens focuses the resulting divergent conical beam into a ring o f
light with a dark center. Since the divergence angle o f the beam is larger than
the opening angle o f the cone of light, the trap is closed also along the beam
propagation direction. Traps in a large range o f dimensions (40 ~tm < r < 740 ~tm)
were experimentally realized, demonstrating the flexibility of this design 6. In
the second experiment (Kulin et al., 2001), this optical scheme was used to
produce a large trap, with r = 740 ~tm, L = 150 mm, and V = 8 x 10 -2 cm 3. The
optical darkness factor (defined as the ratio between the light intensity inside the
trap and the intensity in the focal plane ring) was about 1 : 1000, while along
the axis there was a residual peak, probably caused by light going through the
apex of the axicon. Since the opening angle of the conical beam is not zero, the
two cusps on the optical axis are not of the same height, the one closer to the
lens being about 10 times higher. The lowest points in the potential barrier are
located off-axis, close to the far end o f the trap. This trap was used to capture
Xe atoms in a metastable state. The high trap volume resulted in a good loading
efficiency o f 50% from the MOT which contained a few million atoms. The
lifetime o f the trap was only about 2 0 m s , limited by the gravitational energy
of the heavy Xe atoms in the large trap, which is larger than the height of the
potential barrier at the far end o f the trap.
6 Actually, the trap dimensions can be changed by moving only the axicon, which does not change
the location of the focal plane.
1 16 N. Friedman et al. [IV
FIG. 7. (a) Schematic illustration of the experimental setup for the single-beam dark optical trap
based on a Jr-phase plate element. A destructive interference between the inner part of the beam
(shifted by Jr radians) and the outer ring is formed around the focus of the third lens. (b) Contour
map of the calculated light intensity distribution around the focus, for the parameters described in
the text. The dark minimum is labeled m, and three bright maxima are labeled M. The trap height
is given by the two saddle-points at r _~ 0.017 mm, Z _~ 2504-1 mm. (From Ozeri et al., 1999, Phys.
Rev. A 59, R1750, Fig. 1).
The :r-phase plate trap: The simplest trap o f this kind is realized by placing
a circular phase-plate element into a Gaussian laser beam (Chaloupka et al.,
1997; Ozeri et al., 1999), as shown in Fig. 7a. The phase plate imposes a phase
difference o f exactly Jr radians between the central and outer parts o f the beam,
which have equal intensities. W h e n the b e a m is focused by a lens, destructive
interference between the two parts ensures a dark region around the focus, which
is surrounded by light from all directions, as required. Let b denote the radius
of the inner (phase-shifted) circle, a the outer (clipped) radius o f the Gaussian
beam, and w0 its waist. Equal intensities in the two regions are achieved when
7 Note that this is the maximal volume of the trap. The trapped atoms usually fill a smaller volume,
depending on the ratio between their kinetic energy and the height of the trapping potential.
IV] DARK OPTICAL TRAPS FOR COLD ATOMS 117
Here, K is a constant on the order of 1-3, which depends on the clipping radius a.
The volume of many single-beam dark traps can be expressed in the form
where the constant C depends on the exact realization of the trap. Note that the
volume of a focused Gaussian red-detuned trap is given by V -- 2zR. Jrw2, focus,
which can be written in the form of Eq. (11), with C = 2/jr 2. With the
experimental parameters w0 = 6mm, a = 5 m m (resulting in K ~ 2.3),
f = 250 mm, and/l = 799 nm, the volume of the dark trap is V ~ 9• 10-6 cm 3.
The potential height of the trap is determined by the minimal light intensity
on the trap surface, which is ~ 10% of the peak intensity of the unaltered
Gaussian beam.
In the experiment described by Ozeri et al. (1999), 105 85Rb atoms were
confined in a trap that was realized using this optical setup. The Jr phase plate
was produced by evaporating a thin dielectric layer of an exact thickness on
a glass plate (Davidson et al., 1999). An optical darkness ratio of 750 was
measured, which depends on the amount of light scattered into the dark region,
the degree to which condition 9 is fulfilled, the deviations of the incoming beam
from a Gaussian, and the deviations of the phase shift from Jr. These effects
were studied in detail by Chaloupka and Meyerhofer (2000). In the experiment
of Ozeri et al. (1999), a 1-W laser beam was used, which could be detuned
in the range 4 • 104)' < 6 < 1x 106) ' above resonance. In this range the
lifetime of the trap was 300 ms, limited by collisions with background atoms. For
smaller detunings, the lifetime decreased linearly with 6, which is consistent with
heating-induced lifetime, since the heating rate is proportional to 6 -2 whereas
the trap depth is proportional to 6 -! .
A similar optical configuration was used to optically trap high-energy electrons
with an intense single laser beam, using the ponderomotive force (Chaloupka
and Meyerhofer, 1999). A laser intensity distribution with a local minimum
is essential for trapping electrons with light, since the electrons are always
repelled by the laser field towards the intensity minimum. In this experiment,
the Jr phase shift was realized with a segmented wave plate which can endure a
very high laser intensity.
Spontaneous Raman scattering rate: The amount of interaction between
the atoms and the trapping light was accurately determined by measuring the
spontaneous Raman scattering rate that results from the trapping light (Cline
et al., 1994). This is a very useful experimental technique which permits the
measurement of even very low scattering rates, hence we will present it in some
detail. For this measurement, the trapped atoms were first prepared in the lower
hyperfine level of the ground state, F - 2. The number of atoms in F = 3 after a
variable time t, N3(t), was measured by detecting the fluorescence after a short
pulse of a resonant laser beam. For normalization, the total number of atoms in
118 N. Friedman et al. [IV
0.51 . . . . . . . . ,~ . 9
the two sublevels of the ground state, N3(t)+ Nz(t), can be measured by turning
on also the repumping beam (which is resonant with F = 2) during the detection
pulse. Actually, N3(t) and N2(t) are measured in the same experimental run. Since
the detection beam excites a closed transition, it accelerates the atoms in F = 3,
and these are rapidly shifted out of resonance. Then the repumping laser is turned
on and the number of atoms in F = 2 (which were not accelerated) is measured.
This normalized detection scheme is insensitive to shot-to-shot fluctuations in
atom number as well as fluctuations in frequency and intensity of the detection
laser (Khaykovich et al., 2000). Typical experimental data for the F = 3 fraction
as a function of time in the trap, for a detuning of 0.5 nm (4• 104),), are shown
in Fig. 8. The data are well fitted by the function
FIG. 9. Contour map of the calculated light intensity distribution for the CR-BPE dark trap.
O indicates the trap center, A the transverse maximum, B the axial maximum, and C the lowest
barrier height. (From Ozeri et al., 2000, J. Opt. Soc. Am. B 17, 1113, Fig. 2).
point in the potential barrier (point C in Fig. 9) is - 1 0 times lower than the
transverse potential height (point A) and 60 times lower than the maximal
on-axis intensity (point B). Hence, this trap is relatively shallow, and a very
large detuning cannot be used. The radius of this trap can be estimated as
r = (Jr/2)Mwo, focus, and its length as L - JrMzR, where M = wold, and d is the
width of a phase ring in the radial grating. Since M and w0, focus can be controlled
nearly independently, it is possible to design a trap with a smaller aspect ratio
and a larger volume than the previous ones. Specifically, the volume of this trap
is given by
V ~ ~1jrr2L = ]-~
1 ~ 4 M 3 w 2 0, focusZR = 1-~jrm3
()4
f ~3. (13)
W0
This trap was realized with the following parameters" w0 = 400 [xm, d = 50 ~tm
a n d f = 16mm, giving a volume o f - l . 6 • -4 cm 3. The CR-BPE was formed
as a binary surface-relief phase element, as described by Ozeri et al. (2000).
With a laser power of 120 mW and a detuning of 6 = 1 • 1057 above resonance,
-3 • 106 Rb atoms were loaded into the trap, with a loading efficiency of 5% from
the MOT. The total photon scattering rate was determined from a measurement
of the spontaneous Raman scattering rate to be 10 s-~ . For larger detunings, part
of the atoms were trapped only in two dimensions, and escaped from the trap
through the lowest point in the potential barrier.
An improved trap configuration was recently demonstrated by adding an
axicon telescope before the CR-BPE of the above setup (Kaplan et al., 2002a).
This configuration maximizes the trap depth for a given laser power and
trap dimensions, and greatly reduces the light-induced perturbations to the
trapped atoms. These properties are achieved by surrounding a large dark volume
with a light envelope with (a) an almost minimal surface area for a given
volume, (b) the minimal wall thickness that is allowed by diffraction, and
(c) an almost constant wall height over the entire envelope. The stiffness of the
trap walls, combined with the large detuning allowed by the efficient intensity
distribution, yield a very low calculated spontaneous photon scattering rate for
the trapped atoms. The optical configuration for the creation of this trap is
illustrated in Fig. 10a. The thin ring of light created by the axicon telescope is
diffracted into two cones by the CR-BPE. When these two diffraction orders are
imaged, a light distribution is generated that consists of two equal hollow cones
attached at their bases and completely surrounding a dark region. The height of
the confining potential of this double-conical trap can be approximated by
U(z) L 1
= 9 (14)
U ( z - O) 4 [ ~L _ z] V/1 + (Z/ZR) 2 '
where L is the total trap length. The first term accounts for the linear decrease in
the trap radius away from the focal plane (in both directions) and the second term
IV] DARK OPTICAL TRAPS FOR COLD ATOMS 121
FIG. 10. The double-conical single-beam dark optical trap. (a) Schematic illustration of the optical
setup. A CR-BPE is placed after an "axicon telescope." The +1 and -1 diffraction orders are imaged
to generate the trap (in black). (b) Contour map of the calculated light intensity distribution for the
trap. Note the very thin walls, which provide a very good darkness factor. (c) Measured intensity
cross sections at different planes along the trap's axis [parameters of the optical setup are different
than in (b)]. The two diffraction orders are observed, and the inner one provides the trap walls.
At z = 0 the two orders overlap exactly.
1)3/2 p (15)
I = ~ rw0, focus'
8 Two exceptions are z = 0, where the two diffraction orders overlap, yielding a double potential
height, and z "~ L / 2 , where the singularity in Eq. (14) yields an extremely high potential.
122 N. F r i e d m a n et al. [IV
FIG. 11. (a) Measured cross sections of the time-averaged light intensity in three positions along
the scanning-beam optica! trap, together with a schematic drawing of the trap formation. (b) Lifetime
of atoms trapped in a scanning-beam trap, as a function of the scanning frequency of the trapping
beam, for two trap radii. (From Friedman et al., 2000a, Phys. Reo. A 61, 031403(R), Figs. 1,2).
dimensions of the trap can be changed while maintaining this optimal ratio
between L and zR. The trap volume is given by
w2
1 ~ r 2 L ~ 7yg2r2 o,focus
Z ~ 5 5 /l " (16)
plane. The time-averaged intensity in the focal plane ring (which corresponds to
the radial potential barrier) is given by
2)1/2 i0 2P (17)
/r = ~ 4---R ~ 5~rwo, focus'
where P is the laser power, I0 is the peak intensity of the static focused beam,
and R = r/wo, rocus is the resolution of the scan. The two lowest points in the
potential barrier of the trap are located on the optical axis, and the intensity at
these points (which corresponds to the trap depth) is
Io P
Iz -- 2eR2 Jrer 2 . (18)
Hence, the trap depth depends only on the rotation radius and not on the
resolution. The length of the trap is L = 2zRv/2R 2 - 1, which gives a trapping
volume of 4
V ~ 89 = 2zR2v/ZR2 - 1 -- ~3 (19)
3Jr
of the laser beam (see Fig. 11 b). A large trap (r = 67 ~tm) was found to be stable
for scan frequencies larger than -20 kHz, while for a smaller trap (r = 32 ~tm)
stable trapping was achieved only for higher frequencies (above -60 kHz). As the
scan frequency is decreased, stability is reduced in a gradual way. One reason for
this gradual behavior is the velocity distribution of the trapped atoms, since slow
atoms are easier to trap even with a slowly scanning beam. However, numerical
simulations for a monoenergetic ensemble reveal that the stability of the trap
depends not only on the velocity of the atoms, but also on the exact position in
phase space, and on the shape of the trap. The stability of the scanning-beam trap
is an interesting subject, which will probably be further studied. A spin-relaxation
time of rSR = 380 ms was measured for the trapped atoms by investigating the
spontaneous Raman scattering. Using the branching ratio for the experimental
parameters, this corresponds to a total photon scattering rate of 7 s-1 .
In another realization of a scanning-beam optical trap (Rudy et al., 2001), a
500-mW laser beam was scanned with mechanical scanners at lower frequencies
(2-11kHz). This trap had larger dimensions (w0 = 200~tm, r = 1.5mm),
which made it more stable at low scanning frequencies, but demanded lower
detuning ( o n l y - 1 x 103),) to achieve a sufficient height of the trapping
potential. To increase the height of the potential barrier, the scanning beam
was re-imaged after passing through the vacuum chamber and crossed the
original in an orthogonal direction, such that a nearly spherical trapping volume
was achieved, with a potential height of 100Erec. Up to 8x 105 Na atoms
were loaded into the trap with a lifetime o f - 5 0 m s , limited by heating
due to spontaneous photon scattering from the trapping beam, calculated
to be 500 s -1.
In the realization of scanning-beam traps, two contradicting requirements
exist: a fast scan and a high resolution. Mechanical scanners are usually limited
to scan frequencies below 10 kHz. Acousto-optic scanners are capable of much
faster scans, up to a few 100 kHz, but with nonlinear scans the resolution is
decreased at high frequencies due to the chirp of the acoustic grating over the
laser beam. As demonstrated recently by Friedman et al. (2000b), this limitation
can be corrected through the use of two counter-propagating acoustic waves,
such that the chirp is canceled.
on the common design considerations and trade-offs usually met when choosing
a certain scheme and optimizing its performance.
As a specific example, we assume that the requirement is to trap most o f the
atoms from a magneto-optical trap (MOT) into the dipole trap, and minimize
the spontaneous photon scattering rate o f the trapped atoms. We assume a laser
with a fixed power P -- 1 W and a sample o f alkali atoms, laser-cooled in a
MOT to a temperature o f ks T ,.~ 25Erec, and forming a nearly spherical cloud
with radius -0.5 mm. We will compare the performance o f three dark traps o f the
different classes described previously: a trap based on a Laguerre-Gaussian (LG)
beam (Kuga et al., 1997), a trap based on a scanning beam (Friedman et aL,
2000a), and one based on a diffractive axicon element (the double-conical trap,
Kaplan et al., 2002a).
Adopting a criterion o f > 90% geometrical loading efficiency from the MOT,
we choose a radius r - 0.5 mm for all traps. The beam waist is chosen as
w0 = 50 ~tm (and therefore R = 10) for the scanning-beam trap, and w0 = 10 ~tm
(and therefore R = 50) for the double-conical trap. The length o f the latter is an
independent parameter, chosen as L = 3 m m to optimize the power distribution
as explained in Sect. IV.B. For the LG trap, a LG 3 mode is assumed, with
w0 - 0.5 mm. For comparison, we look also at a red-detuned trap, formed by
two focused Gaussian beams, intersecting at a right angle 9 (Adams et al., 1995).
We neglect the enhanced loading efficiency of red-detuned traps (Kuppens et al.,
2000) (see Sect. II.B), and assume for the crossed red-detuned trap w0 = 0.6 mm,
which corresponds to > 90% overlap with the MOT.
Following Grimm et al. (2000), we introduce the parameter to, defined as
the ratio of the ensemble-averaged potential and kinetic energies of the trapped
atoms, tr = <Epot>/ (Ek >, and refer to it as the "darkness factor" o f the dark trap.
Assuming a trapped atomic gas in thermal equilibrium, and neglecting gravity,
the ensemble-averaged potential energy is given by
fdr(U(r)-Uo) e x p [ - U ( r ) - U0]
<Epot)= kbT ,
fdrexp[-U(r)-kSTUo] (20)
with U(r) the three-dimensional dipole potential function, U0 the potential at
the bottom o f the trap, and the integration taken over the entire trap volume.
3
The ensemble-averaged kinetic energy is (Ek> = ~ksT. To generalize the
darkness factor also for red-detuned traps, we use a modified definition o f
9 We choose a crossed trap, and not a simpler focused Gaussian beam trap, since with a single
focused beam a trap radius of 0.6 mm will result in an extremely large axial size of > 1 m.
126 N. F r i e d m a n et al. [IV
Table I
Required detuning, calculated atomic darkness factor and mean spontaneous photon scattering rate
for Rb atoms confined in the traps analyzed in the text
( Ys ) = - ~Y -~
3 kb T . K.t. (21)
The detuning in the c o m p a r i s o n is c h o s e n such that the trap depth is 3 times larger
than the m e a n kinetic energy o f the atoms. Since a fixed laser p o w e r is
assumed, less efficient traps w o u l d require s m a l l e r detunings to provide the s a m e
trap depth. In Table I, the required d e t u n i n g is p r e s e n t e d for Rb a t o m s in each
o f the different traps, with the p a r a m e t e r s discussed above. Also s h o w n are the
numerically calculated to', and the m e a n s p o n t a n e o u s p h o t o n scattering rate, (Ys),
which d e t e r m i n e s the heating and d e c o h e r e n c e rates o f the trapped atoms.
As expected, all b l u e - d e t u n e d traps have a better d a r k n e s s factor than the red-
detuned trap. Their scattering rates are smaller as well, even for traps requiring
a smaller detuning. The d o u b l e - c o n i c a l trap has a significantly better d a r k n e s s
factor (to' = 0.02) than all other schemes. The a d v a n t a g e o f the d o u b l e - c o n i c a l
trap is even larger w h e n the scattering rate is considered, since the i m p r o v e d
darkness factor is c o m b i n e d with the efficient distribution o f optical p o w e r that
enables an increased detuning ll. We p e r f o r m e d a similar calculation also for a
V. Applications
Dark optical traps offer a relatively interaction-free environment for the confined
cold atoms. This property has opened up a way for several applications, including
precision spectroscopic measurements and the preparation and investigation of
atomic samples at high spatial and phase-space densities. Recently, the dynamics
of atoms inside a dark optical trap has been studied as a versatile experimental
realization of the well-known billiard system. All these applications are discussed
in this section, with a focus on their experimental demonstrations.
In this subsection we describe the main cooling mechanisms that have been
realized inside dark optical traps. These include polarization-gradient cooling,
128 N. Friedman et al. [V
Raman cooling and evaporative cooling, and also the reflection cooling mecha-
nism, which is unique for blue-detuned traps. Cooling inside a trap is favorable
since density increases as the atoms get colder, hence the gain in phase-space
density is larger. Moreover, coupling between the different directions which
results from trap anisotropy or collisions between the atoms makes it possible to
achieve 3D cooling while performing laser cooling along only one dimension.
As opposed to magnetic traps, in an optical dipole trap it is possible to trap and
cool atoms independently of their magnetic sublevel, so that a BEC composed
of different m-states can be achieved (Barrett et al., 2001), it is possible to
investigate a BEC in an arbitrary magnetic field (Inouye et al., 1998) and to
study spinor condensates composed of atoms at different m-states (Stenger et al.,
1998). Moreover, in some atomic species such as Cs, the lowest ground state
cannot be trapped in a magnetic trap, and those states that can be trapped suffer
from a very high inelastic loss rate which limits the achievable phase-space
density below the BEC transition (S6ding et al., 1998). As a result, experimental
effort is directed towards cooling Cs atoms in optical traps.
Experimental and theoretical effort has been devoted to find the limitations of
the various cooling schemes, and many heating and loss mechanisms have been
identified and investigated. [Relevant examples for the present discussion include
Bali et al. (1994), Castin et al. (1998), Winoto et al. (1999), Wolf et al. (2000),
Kerman et al. (2000), Kuppens et al. (2000)]. A detailed description of these
mechanisms is beyond the scope of this review. Here, we will briefly describe
the limiting mechanisms which are relevant for cooling inside dark optical traps.
At the end of this subsection we will discuss compression of the trapped atomic
cloud, as it can lead to better starting conditions for evaporative cooling, and is
also interesting for measurements of cold collisions.
A.2. R a m a n cooling
Raman cooling was first used to cool untrapped alkali atoms below the photon-
recoil limit in one dimension (Kasevich and Chu, 1992) and then in two
and three dimensions (Davidson et al., 1994). This cooling method is based
on accumulating cold atoms in a velocity dark state. In alkalis, the scheme
is realized by transferring atoms between the two hyperfine levels of the
ground state, using pulses of counter-propagating Raman laser beams. The
parameters of these pulses are chosen such that atoms in different velocity
classes (except a velocity class around zero) are transferred to the upper level.
A repumping beam transfers the atoms back to the lower level, via spontaneous
emission. This process is continued until most of the atoms accumulate in the
lower level, in the dark velocity class near v = 0.
This scheme was successfully applied to sodium atoms trapped in the inverted-
pyramid dark trap described in Sect. III.A (Lee et al., 1996). Since the trap
mixes the motion in the three spatial dimensions, cooling in 3D was achieved
by applying the Raman beams in only one dimension. In the trap, 4.5 • 105 atoms
were cooled to a temperature of 0.4Trec at a final density of 4• 1011 cm -3. The
phase-space density was increased by a factor of 320 as compared to the MOT, to
a final value of n/laB ,~ 6• l 0 -3 [with AdB the thermal de-Broglie wavelength],
which is the highest yet achieved inside a dark optical trap. Since the atoms
are trapped, their velocity might change during their interaction with the Raman
pulse, resulting in motional sidebands which reduce the velocity selectivity of the
Raman pulses, and limit the achievable temperature as compared with untrapped
atoms. In a later experiment, a modified scheme was used to simultaneously
Raman-cool the atoms and optically pump them into one magnetic sublevel of
the lower hyperfine state (Lee and Chu, 1998). The modified cooling scheme
resulted in a slightly higher temperature and also some loss of trapped atoms,
130 N. Friedman et al. [V
such that the final phase-space density was comparable to that of the previous
experiment.
For very tight traps, the motional sidebands are resolved, enabling the
realization of Raman sideband cooling schemes. Raman sideband cooling was
applied so far only to atoms trapped inside red-detuned optical lattices (Hamann
et al., 1998; Perrin et al., 1998; Vuleti6 et al., 1998; Kerman et al., 2000), but it
can be applied also for dark optical lattices to cool atoms to the lowest vibrational
level. Cooling inside optical lattices [using either Raman sideband cooling or
PGC (Winoto et aL, 1999)] can also be used to produce a cold and dense source
of atoms, to improve loading into optical dipole traps (Han et al., 2001).
For Cs, one has q = 0.25, dihf = 2Jr • 9.2 GHz, and )' = 2Jr • 5.3 MHz. With
the experimental values of 6 = 1 GHz and A = 300nm, the cooling rate is
V] DARK OPTICAL TRAPS FOR COLD ATOMS 131
/3 ~ 5 • 10-77 ~ 2st x 2.5 Hz. This cooling rate is limited by the relatively long
time between inelastic collisions, and is much lower than the cooling rates of
Doppler cooling and polarization-gradient cooling. The equilibrium temperature
can be estimated by equating the average cooling and heating per bounce. With
the above experimental parameters, a temperature of T ~ 10Trec ,~ 2~tK
is expected, which is similar to that achieved in PGC. This temperature was
experimentally obtained for a sample with a small number of atoms. Higher
temperatures were obtained in dense samples, due to multiple photon scattering,
caused mainly by stray light from the hollow beam. Although the Sisyphus
cooling acts only along the vertical direction, the horizontal direction is also
cooled to the same temperature. This coupling is probably due to evanescent-
wave diffusive reflection from the non-perfect surface of the prism.
Reflection cooling was also demonstrated with traveling waves, in the Axicon
conical trap (Ovchinnikov et al., 1998). Here, cooling was observed only for
larger detunings of the conical beam, 6 = 30GHz. The larger detuning is
required in order that the condition np < 1 be fulfilled [np is the number
of photons scattered per bounce, see Sect. III.B], but it lowers the cooling
rate (22). In traveling-wave dark optical traps with a larger spring constant, such
as the scanning-beam trap, the lower cooling rate might be partially compensated
by the high rate of reflection from the walls, which is of the order of the
oscillation frequency in the trap potential.
A.5. Compression
When the volume of a trap is reduced, the atomic density and temperature
are increased. The increase in density leads to better starting conditions for
evaporative cooling since the cooling rate is limited by the elastic collision
rate or, in the hydrodynamic limit, also by the trap oscillation frequency (Han
et al., 2001; Ketterle and VanDruten, 1996), which are both increased with
compression. Compression of magnetic traps is a common procedure in many
BEC production schemes. In optical traps, compression might have a larger
effect since even higher densities and oscillation frequencies can be achieved.
For example, in the first realization of an all-optical BEC formation (Barrett
et al., 2001), the evaporative cooling time was only 2 s, as compared to > 10 s
usually needed in magnetic traps.
Compression was demonstrated in the scanning-beam dark optical trap
described in Sect. IV.C. Since the shape of the trap is controlled electronically,
it can be changed easily at a desired rate. As an example, when the trap
radius was decreased from 100 ~tm to 27 ~m in 150ms, a 350 times adiabatic
increase in spatial density was observed. These results were improved by adding
a PGC pulse during the compression, which resulted in a cloud of 106 atoms
at a density of 2x1013 cm -3, an axial temperature of 75Trec and a radial
temperature of 110Tr~. This represented a x 130 increase in spatial density and
a x 16 increase in phase-space density over the initial conditions, to a value of
1.2x 10-4.
An interesting effect in this context is that even an adiabatic change in the
potential shape can lead to a change in the maximal phase-space density if the
potential functional dependence is modified, and the elastic collision rate is high
V] DARK OPTICAL TRAPS FOR COLD ATOMS 133
A.6. H e a t i n g a n d loss
In this section we briefly discuss the main heating and loss mechanisms for dark
optical traps. Heating can result either from interaction with the trapping light
itself, or due to photon re-absorption when laser cooling is applied to dense
atomic samples. Loss may result from interaction of atoms with the environment
and with the trapping light, or from inelastic collisions between atoms. Finally,
light-assisted collisions, where two colliding atoms interact with the trap light,
also contribute to trap loss.
Photon scattering: A major source for heating in optical traps is photon
scattering from the trapping light. To minimize the scattering rate, traps with
large detunings are favorable, and dark traps have an advantage over bright traps
(see Sect. IV.D). From a practical viewpoint, it is important to reduce the amount
of stray light scattered into the dark region. Very small amounts of residual
on-resonance light in the trap laser beam might also lead to heating, and should
be filtered in cases where the latter should be kept minimal.
Other heating sources: Intensity or pointing instabilities of the trapping laser
(Savard et al., 1997), and quantum diffractive collisions with background gas in
the vacuum chamber (Bali et al., 1999) cause heating in both bright and dark
optical traps. However, in some experiments the measured heating rate exceeds
the estimated rate based on these processes (Han et al., 2001), indicating that
some other heating mechanisms may exist.
Density-dependent heating: In optically dense samples, reabsorption of
spontaneously scattered photons during a laser-cooling process causes heating,
and limits the attainable equilibrium temperature. A quantitative estimation of
this effect was obtained experimentally for PGC performed on Cs atoms in
134 N. Friedman et al. [V
where n is the atomic density, and integration is over the trap volume (Grimm
et al., 2000). The first term corresponds to loss processes which do not depend on
the atomic density, mainly collisions of the trapped atoms with hot background
atoms in the vacuum chamber. In ultra-high vacuum chambers, the background-
limited lifetime can be of the order of tens of seconds. In shallow traps, heating
of the atoms is also translated into trap loss.
In tightly confining traps, the high density results in two-body loss mech-
anisms, which are described by the second term in Eq. (23). The third term
corresponds to three-body loss which plays a role only at very high densities.
The density-dependent loss can be observed and quantified by measuring the
decay of the number of trapped atoms as a function of time. As an example, the
decay curves for atoms from the compressed scanning-beam dark trap (Friedman
et al., 2000a) are presented in Fig. 12a, for atoms in either the lower or the upper
V] DARK OPTICAL TRAPS FOR COLD ATOMS 135
06 Ur
! F,=2
F,=3
I
10~ I s+p
~ 104 I
I (!)
I
U=(R) I
' S+S
I~ oro o'.5 I'.o ~15 i.o
Time [sl R
(a) (b)
FIG. 12. (a) Measured decay of the number of trapped atoms from a scanning-beamtrap, for atoms
in either of the two hyperfine levels of the ground state. A high density was obtained by compression
of the trap, and resulted in two-body collision loss. (From Friedman et al., 2000a, Phys. Rev. A 61,
031403(R), Fig. 4). (b) Diagram illustrating the light-assisted collision loss mechanism, for two
atoms colliding in the presence of a blue-detuned optical field. A pair of atoms in the ground
state (1) approach each other. At the Condon point (Rc) the laser is in resonance with a repulsive
molecular excited state. The pair might be excited by the laser (2), and reach the turning point (Rtp).
Then, the atoms are repelled (3) and, if not brought back to the ground state by the laser, they share
a gain in kinetic energy which is asymptotically equal to h6. (From Suominen, 1996, J. Phys. B 29,
5981, Fig. 4b).
ground-state hyperfine level. The data are well fitted by the solution to Eq. (23)
neglecting the third term (e = 0). The two-body loss coefficients found from the
fit are flF=3 = 2.0• 10-ll cm3/s and flF=2 = 1.2• 10 -ll cm3/s. The larger two-
body collision loss from the upper hyperfine level is due to hyperfine exchange
collisions, since the energy difference between the two ground-state hyperfine
levels in this case (85Rb) is "-4 • 105Erec, which is much higher than the trap depth
of ~ 103Erec. For this reason, it is important to keep atoms in the lower hyperfine
level in high-density traps.
The two-body loss from the lower hyperfine level is attributed to light-assisted
collisions. When two atoms collide in the presence of a light field, absorption
of a photon will transfer them into an excited molecular state. In the case of
red-detuned light, excitation is possible into an attractive molecular state, which
gives rise to loss processes (Weiner et al., 1999; Suominen, 1996) like radiative
escape and photoassociation. Blue-detuned light can excite the colliding atoms
into a repulsive molecular state (Bali et al., 1994) (see Fig. 12b). The atoms are
then accelerated along the repulsive potential curve and obtain a kinetic energy
which is asymptotically equal to the detuning of the exciting laser from the
atomic resonance. This energy is usually much larger than the potential barrier
of the trap, hence both atoms will be lost. Light-assisted binary collisions in the
presence of blue-detuned light were further investigated in the gravito-optical
surface trap (Hammes et al., 2000). Another blue-detuned beam was applied
136 N. Friedman et al. [V
to the trap, and the induced two-body loss coefficients,/3, were measured for
different detunings and intensities of this "catalysis" laser. The loss was found
to be proportional to//62, in the range 5-80 GHz.
B. PRECISIONMEASUREMENTS
The strong suppression of Doppler and time-of-flight broadening due to the ultra-
low temperatures, and the possibility to obtain very long interaction times, are
obvious advantages of using cold atoms for precision optical and rf spectroscopic
measurements. To obtain long atomic coherence times, spontaneous scattering
of photons and energy-level perturbations caused by the trapping laser should
be reduced. This is achieved by increasing the laser detuning from resonance
and trapping the atoms in dark traps. These advantages were demonstrated
already in the first experimental realization of a dark optical trap for cold
atoms (Davidson et aL, 1995), where the ground-state hyperfine splitting
of sodium, dihf, was measured with a very long coherence time of 4s,
yielding a linewidth of 0.125Hz. The magnetic-field insensitive transition
between the IF = 1,mF = 0) and IF = 2, mF = 0) states was excited with a
~l.77-GHz linearly polarized rf wave. A magnetic field parallel to the rf
polarization direction separated the required transition from the magnetic-field
sensitive transitions. During the experiment, the trap was loaded with atoms
which were optically pumped to F = 1. Then, the rf sequence was applied
and the number of atoms making the transition was measured by a state-
selective fluorescence detection of atoms in the F = 2 state. The rf transition
was excited using Ramsey's method of separated oscillatory fields (Ramsey,
1956) by applying two Jr/2 pulses separated by the measurement time T.
The resulting central Ramsey fringes are shown in Fig. 13a, together with a
sinusoidal fit. The fit yields a fringe contrast of 43%, which was found to decay
exponentially with T, with a decay constant of 4.4 s. The uncertainty in the line
central frequency was + 1.3 mHz, for 200 data points collected during 900 s. This
is higher than the shot-noise-limited frequency sensitivity of the Ramsey method,
which is given by A v = (4:r2NtT) -1/2, where N is the number of atoms and
t is the integration time.
The accuracy resolution of the spectroscopic measurement are limited by the
interaction of atoms with the trapping laser field. First, this interaction causes
an average shift in the line center, since it shifts the energy levels of the atom
(in proportion to I/6). This ac Stark shift is different for the two levels used in
the experiment, due to the (very small) difference in the detuning. (For linearly
polarized light, the dipole matrix elements are identical for all sub-levels of the
ground state.) As a result, the ac Stark shift of the hyperfine transition is lower
than the optical Stark shift by a factor of 6/6hf, which is ~ 4.5 • 10 4 in this case.
In the above experiment, a linear dependence of the Stark shift on the trapping
V] DARK OPTICAL TRAPS FOR COLD ATOMS 137
~.~ 200
8 0.5
" 150
8
100
O
u_ 50
0.0 "- ~
.... "'"'" ~ 1 7 6 "'" , o . . ~, ~ ,,.
0 I . I,, I
-0.3 -0.2 -0.1 0.0 0.1 0.2 0.3 0 5000 10000 15000 20000
f- 1,771,626,130 Hz Light shift (Hz)
(a) (b)
FIG. 13. (a) Central Ramsey fringes of the IF = 1,mf = 0 ) ~ IF = 2, mf = 0 ) rf transition,
measured in the "V"-shaped trap with a 4s measurement time. (b) Calculated ac Stark shift
distributions for atoms stored in blue-detuned dipole traps. The dotted line corresponds to the
"V"-shaped trap, and the solid line is for a more ergodic inverted pyramid trap (composed of three
laser beams). (From Davidson et al., 1995, Phys. Reo. Lett. 74, 1311, Fig. 4).
laser intensity was observed, resulting in a 270-mHz shift of the line center in
the displayed data. Second, it is important to note that this shift is not equal for
atoms which have different trajectories in the trap, yielding an inhomogeneous
distribution of Stark shifts that limits the coherence time of the trap. Hence,
coherence time is related to the dynamics of the trapped atoms. A more chaotic
trap will increase temporal averaging between the atoms and lead to a narrower
distribution and longer coherence times. This averaging effect was calculated
using numerical Monte Carlo simulations; the results are presented in Fig. 13b. In
our discussion, we neglected the contribution of spontaneous photon scattering to
the decoherence rate. This is justified because )'s is smaller than the ac Stark shift
by the factor t~hf/Y ~ 170-2000 for most alkalis. This means that by the time it
takes for a spontaneous scattering event to occur, the inhomogeneous phase shift
of the rf transition due to the ac Stark shift is already hundreds of 2Jr radians.
The Stark shift in the dark optical trap is a great limitation for its performance
as an atomic clock 12. On the other hand, it seems that a dark optical trap is a
very good candidate for precision experiments in atomic physics, such as parity-
nonconservation and permanent electric dipole moment (EDM) measurements
(Bijlsma et al., 1994). Such tabletop experiments are very appealing for tests
12 This limitation can be partially solved by using an additional, very weak, optical field, which
is spatially mode-matched to the trap laser and whose detuning is in the middle of the hyperfine
splitting. The relative Stark shift introduced by this laser compensates that introduced by the trap
(Kaplan et al., 2002b).
138 N. Friedman et al. [V
of the standard model and extensions of it. In some of these theories, for
example, a non-zero EDM value is predicted which is within experimental reach.
Measurement of EDM with optically trapped cold atoms was proposed and
discussed in two recent papers (Romalis and Fortson, 1999; Chin et al., 2001),
and dark optical traps were found to be a promising tool for performing such
measurements with much higher sensitivity than is currently available. The use
of cold atoms can overcome the two limiting factors of current experiments,
namely systematic errors due to the atomic velocity in beam experiments, and
leakage currents in cell experiments.
The EDM measurement is based on measuring a possible energy shift between
two Zeeman sublevels when a static electric field is applied. Therefore, any
perturbation of the Zeeman sublevels should be kept minimal. In dark optical
dipole traps, the limits on the accuracy of the measurement are due to interactions
between the trapping light and the atoms, which cause frequency shifts between
the Zeeman sublevels. The three leading terms of these interactions are (Romalis
and Fortson, 1999): a vector shift caused by a residual circular polarization of
the trapping laser; tensor shifts which result from the interaction of the atoms
with the trapping light in the presence of the static electric field; and a third-
order effect which represents interaction of an induced electric dipole with
the laser field through magnetic-dipole or electric-quadrupole interaction. The
enhanced cross section for cold atomic collisions may result in frequency shifts
(Gibble and Chu, 1993; Bijlsma et al., 1994) and should also be avoided. These
limiting factors have been analyzed by Romalis and Fortson (1999) for the case
of cesium atoms confined in either a red- or a blue-detuned dipole trap. The
vector light shift can be lowered by reducing the residual circular polarization
of the trapping beam, and aligning the beam propagation direction perpendicular
to the static magnetic field (which defines the quantization axis). When the
trapping laser is detuned above resonance, destructive interference between the
amplitudes of the vector light shift from two resonance lines lowers the total
shift 13. The tensor shift is eliminated at a "magic angle" (54.7 ~ which satisfies
3 cos 2 r 1 = 0) between the direction of the electric field of the light and the
quantization axis, or by measuring a IF, mF) ~ I F , - m F ) transition (as suggested
by Chin et al., 2001), for which the tensor shift, which depends on m~, vanishes.
In another work, Chin et al. (2001) have made a detailed error analysis
for a specific experimental realization of an EDM measurement, for Cs atoms
in a dark optical lattice. The calculation was made for a lattice which is
realized with a 532-nm laser (detuning of 4 x 107}I above the Cs 6S1/2 ---+ 6P3/2
transition). The optimal trap depth is "~130Erec, and the photon scattering rate
for atoms in the lattice ground state is -~7x 10-3 s-1. The proposed lattice
13 For Cs, it actually vanishes for two wavelengths: 464 and 474nm, but no sufficiently strong
laser lines are available at these wavelengths.
V] DARK OPTICAL TRAPS FOR COLD ATOMS 139
FIG. 14. (a) Proposed experimental configuration for a measurement of the electron's electric
dipole moment using Cs atoms trapped in a dark optical lattice. The lattice is composed of three
linearly polarized standing waves, with different frequencies. The polarizations of the beams are
perpendicular to the quantization axis defined by the external electric and magnetic fields along
the z-axis. (b) Ground-state tunneling rate (solid line) and scattering rate for blue- (dotted) and
red-detuned (dashed) 3D lattices. Lattice detuning is assumed constant, and the lattice depth is
changed by increasing the laser intensity. The arrow marks the operation point of the proposed
scheme, where tunneling and scattering rates are equal for a blue-detuned lattice. (From Chin et al.,
2001, Phys. Rev. A 63, 033401, Figs. 1, 2).
a different atomic species (Rb, for example) can be trapped in the same lattice,
and serve as a "co-magnetometer," to investigate and correct potential systematic
effects induced by the external fields. It is estimated that using this system with
108 trapped atoms, a 1 s coherence time, and a measurement time of 8 hours,
the sensitivity of the EDM measurement will be 100 times better than current
experiments. The main limitations are stringent requirements on the intensity and
polarization stability of the trapping laser, and the 3rd-order polarizability effect.
Another application for which dark optical traps are considered (Kulin et al.,
2001) is parity-nonconservation measurements (PNC). For these experiments,
the radioactive alkali atom francium appears as a good candidate, since it is
predicted to have a large PNC effect (18 times larger than Cs). In the last few
years, Fr was efficiently trapped in a MOT (Simsarian et al., 1996; Lu et al.,
1997), and its energy structure was investigated spectroscopically (Sprouse et al.,
1998). Precision spectroscopy experiments on Fr atoms in a dark optical trap
seem feasible, and might improve experimental tests of the standard model.
Dark traps are useful also for spectroscopic measurements of extremely
weak optical transitions. While preserving long atomic coherence times, those
traps can provide large spring constants and tight confinement of trapped
atoms, which ensure good spatial overlap even with a tightly focused excitation
laser beam. Therefore, the atoms can be exposed to a much higher intensity
of the excitation laser, yet being relatively unperturbed by the trapping light.
This yields an increased sensitivity for very weak transitions, and especially for
multi-photon transitions. This property was demonstrated by measuring a two-
photon transition in cold Rb atoms trapped in a scanning-beam optical trap, with
a very weak probe laser (Khaykovich et al., 2000). A spectroscopy scheme which
exploits the long spin-relaxation time of the dark trap was used.
In this scheme (see Fig. 15a), atoms with two ground-state hyperfine levels
(Ig,), Ig2)) are stored in the trap in a level Ig,) that is coupled to the upper
(excited) state, [e), by an extremely weak transition which is excited with a
laser. An atom that undergoes the weak transition may be shelved, through
a spontaneous Raman transition, in ]g2), which is uncoupled to the excited
level. After waiting long enough, a significant fraction of the atoms will be
shelved in Ig2)- The detection benefits from multiply excited fluorescence of
a strong cycling transition from the shelved level ]g2). Thanks to the use of
a stable ground state ([g2)) as a "spin shelf," the quantum amplification is
limited only by spin-relaxation processes which are strongly suppressed in a
dark trap. This scheme was realized on the 5S1/2 ----+ 5D5/2 two-photon transition
in cold and trapped 85Rb atoms (see Fig. 15a for the relevant energy levels). The
trapped atoms were optically pumped to the lower (F = 2) hyperfine level. The
spectroscopy was made with an extremely weak (25 ~tW), frequency-stabilized
laser beam, which excited the two-photon transition. The scanning-beam trap was
loaded and then compressed to a lower radius (Friedman et aL, 2000a), to best
V] DARK OPTICAL TRAPS FOR COLD ATOMS 141
• • 5D,a le)
780.24mn
F=3 ig~...,~ 0.30
F--2 I ~ 5Sla 5 10 15 20 25
Frequency [MHz]
(a) (b)
FIG. 15. (a) Energy levels of 85Rb and the relevant transitions for a two-photon spectroscopy
experiment inside a scanning-beam dark trap. Spectroscopy of the Igl) ~ ]e) transition
( 5 S 1 / 2 , F = 2 --~ 5 D 5 / 2 , F t in the case of 85Rb) is performed. Atoms which undergo the transition
are shelved in the level ]g2) (5S1/2, F = 3), from which they are detected using a cycling transition
(to 5 P 3 / 2 , F = 4). (b) Measured spectrum of the 5 S I / 2 , F = 2 ~ 5 D 5 / 2 , F t = 4,3,2, 1 two-photon
transition. Each point corresponds to an experimental cycle, in which atoms are exposed during
500ms to a 25~tW excitation laser. (From Khaykovich et al., 2000, Europhys. Lett. 50, 454,
Figs. 1, 4b).
overlap with the excitation laser. After 500 ms, the fraction of atoms transferred
to F = 3 was measured. In Fig. 15b, the measured F = 3 fraction is presented as
a function of the frequency of the two-photon laser. The hyperfine splitting of the
excited state was resolved, and the measured frequency differences and relative
line strengths are in a good agreement with theory and previous measurements
(performed with much higher laser intensities). A transition rate as small as
0.09 s -I was measured, with a "quantum rate amplification," due to spin shelving,
o f ~ 1 0 7 . This optical spectroscopy technique can be applied for other weak
(forbidden) transitions such as optical clock transitions (Ruschewitz et al., 1998;
Kurosu et aL, 1998) and parity-violating transitions where a much lower mixing
with an allowed transition could be used.
In a dark optical trap, atoms move freely in the dark region, and reflect elastically
from the trapping potential. The similarity of this system to the well-studied
billiard problem has recently led to the realization of "atom-optics billiards"
(Milner et al., 2001; Friedman et aL, 2001b) in which cold atoms move inside
dark traps of various shapes. The motion of the atoms is governed by the shape of
the trap, and can exhibit different types of dynamics, from regular to chaotic. The
billiards were formed as scanning-beam traps, using two perpendicular acousto-
142 N. F r i e d m a n et al. [V
14 Exactly periodic trajectories that are completely stable have only a zero measure, and hence can
be neglected.
V] DARK OPTICAL TRAPS FOR COLD ATOMS 143
FIG. 17. Survival probability of atoms in the gravitational wedge billiard, 300 ms after opening the
hole, as a function of the wedge half-angle. Lower curve: experimental data. Upper curve: results of
a classical numerical simulation (divided by 2 and shifted up by 0.1). The inset shows the measured
intensity cross section at the focal plane of the billiard (with a hole) (From Milner et al., 2001,
Phys. Rev. Lett. 86, 1514, Figs. 3, 4).
15 A "tilted" stadium (and not the more common Bunimovich stadium) is used in the experiment
in order to reduce the number of nearly stable trajectories (Vivaldi et al., 1983).
144 N. Friedman et al. [V
FIG. 18. Survival probability of atoms in billiards of various shapes, as a function of time after
opening a hole in the boundary. (a) Elliptical billiard. The solid symbols denote the unperturbed
case, in which the surviving fraction for the ellipse with the hole on the long side (solid squares)
decays much faster than for the hole on the short side (solid circles). The open symbols show the
case in which 10~ts velocity randomizing molasses pulses are applied every 3 ms. (b) Decay of
atoms from circular and stadium billiards: The decay from the stadium billiard (solid circles) shows
a nearly pure exponential decay. For the circle (solid diamonds) the decay curve flattens, indicating
the existence of nearly stable trajectories. The solid lines represent numerical simulations, including
all the experimental parameters, and no fitting parameters. The dashed line represents exp(-t/rc),
where r c is the escape time calculated for the experimental parameters. The insets show CCD-camera
images of the billiards' cross sections at the beam focus. The size of the images is 300x 300 ~tm.
(From Friedman et al., 2001b, Phys. Rev. Lett. 86, 1518, Figs. 2, 4).
which are not included in the simulation and may decrease the stability, or to
imperfections in the trapping beam.
In another set of experiments, billiards of various shapes were investigated
(Friedman et al., 2001b). First, "macroscopic" separation in phase space was
measured, for the elliptical billiard. Here, phase space is divided into two separate
regions (Koiller et al., 1996): "external" trajectories that are confined outside
elliptical caustics (smaller than the billiard itself but with the same focal points),
and "internal" trajectories confined by hyperbolic caustics, again with the same
focal points, as shown in Fig. 16c. Hence, if a hole exists at the short side of
the ellipse (upper inset of Fig. 18a), atoms in those trajectories remain confined
and never reach the hole. Alternatively, all trajectories, excluding a zero-measure
amount, reach the vicinity of a hole on the long side of the ellipse (lower
inset of Fig. 18a) and hence the number of confined atoms decays indefinitely.
Figure 18a shows the measured survival probability for cold Rb atoms in the
elliptical optical billiard with a hole on either the long or the short side. At
long times, the survival probability for the hole on the short side is much higher
than for the hole on the long side, as expected from the discussion above. Next,
a controlled amount of randomization was introduced to the atomic motion, by
exposing the confined atoms to a series of short PGC pulses (using the six MOT
beams). During each pulse, an atom scatters "--30 photons, and hence its direction
of motion is completely randomized, whereas the total velocity distribution
remains statistically unchanged. The measured decay curves for this case, with a
V] DARK OPTICAL TRAPS FOR COLD ATOMS 145
PGC pulse every 3 ms, are also shown in Fig. 18a, for the two hole positions of
the ellipse. As seen, for the hole on the long side, the randomizing pulses cause
little change. However, for the hole on the short side, a complete destruction
of the stability occurs, and the decay curves for the two hole positions coincide
approximately. The stability decrease was found to be gradual, and the pulse rate
required to significantly reduce the stability is approximately one pulse per rc,
the average 1/e decay time.
Next, decay curves were measured for the circular and the tilted-stadium
billiards. Since the atoms were loaded into the billiard from a cloud in
thermal equilibrium, their velocity was distributed around zero, with a measured
RMS velocity distribution of 1 It)recoil. To better approximate a mono-energetic
ensemble of atoms, and to reduce the relative contribution of gravitational
energy (~< 50Erecoil), the loading scheme was modified. After loading from the
MOT into the trap, the atoms were illuminated with a short pulse of a strong,
on-resonance pushing beam perpendicular to the billiard beam. Following this
pushing beam, the center of the velocity distribution was shifted to 20t)recoil,
while the RMS width was barely changed. The hole was opened 50ms after
the push, to allow for a randomization of the direction of the transverse velocity
through collisions with the billiard's boundaries. The measured decay curves for
the circular and the tilted-stadium billiards, with equal area and hole size, are
shown in Fig. 18b. The decay from the circular billiard is slower, indicating the
existence of nearly stable trajectories, whereas that of the stadium is a nearly
pure exponential. Also shown in the figure are the results of full numerical
simulations that contain no fitting parameters. The simulations include the
measured three-dimensional atomic and laser-beam distributions, atomic velocity
spread, laser-beam scanning, and gravity. It is seen that there is fairly good
agreement between the simulations and the data.
As opposed to ideal billiards which have an infinite potential wall, optical
billiards inherently have a soft-wall potential, which may affect the dynamics
(Rom-Kedar and Turaev, 1999; Gerland, 1999; Sachrajda et al., 1998). For
example, a soft wall may introduce stable regions into an otherwise chaotic
phase space, and create "islands of stability" immersed in a chaotic sea. This
structure greatly affects the transport properties of the system, since trajectories
from the chaotic part of phase space are trapped for long times near the boundary
between regular and chaotic motion (Zaslavski, 1999). This was demonstrated
in a recent experiment by Kaplan et aL (2001), who compared the decay
from billiards with hard and soft walls. The softness of the billiards' wall
was experimentally changed by varying w0 of the scanning beam. In Fig. 19,
experimental results for the decay from a tilted stadium billiard with a harder
(w0 = 14.5~m) and a softer (w0 = 24~tm) wall are presented. When the
hole is located entirely inside the big semi-circle (Fig. 19a), the soft wall
causes an increased stability, and a slowing down in the decay curve. When the
146 N. F r i e d m a n et al. [V
FIG. 19. The effect of wall softness: measured survival probability of atoms in a tilted-stadium
shaped billiard, with two different values of wall softness: w0 = 14.5 ~tm (o), and w0 = 24.5 ~tm (+).
(a) The hole is located inside the big semicircle. The smoothening of the potential wall causes a
growth in stability, and a slowing down in the decay curve. (b) The hole includes the singular point,
no effect for the change in w0 is seen. Also shown are results of numerical simulations, with the
experimental parameters and no fitting parameters. The dashed line represents exp(-t/rc), the decay
curve for an ideal (hard-wall) billiard. The insets show measured intensity cross sections for the
soft-wall billiards, in the beam's focal plane. The size of the images is 300• ~tm. (From Kaplan
et al., 2001, Phys. Rev. Lett. 87, 274101, Fig. 1).
hole includes the singular point, where the straight line and semi-circle meet,
(Fig. 19b), no effect for the change in w0 is seen. These results can be explained
by the formation of a stable island around the trajectory that connects both
singular points, and a "sticky" region around it. This explanation is supported
by numerical simulations, which predict the formation of a stable island around
the singular trajectory when the wall becomes soft. Around this stable island
there is a "sticky" area in which chaotic trajectories spend a long time before
escaping back to the chaotic part of phase space. Similar decay measurements
and simulations for a circular atom-optics billiard showed no dependence on w0
in the range 14.5-24 ~m, and no dependence on the hole position. In another
work, it was shown that adding a force field across the billiard can also stabilize
specific orbits in otherwise chaotic billiards (Andersen et al., 2002a).
Two theoretical works (Liu and Milburn, 1999, 2000) are related to the optical
billiard system. In these works, the classical and quantum dynamics of a gas of
cold atoms trapped inside a circular hollow laser beam or a hollow fiber was
investigated, when the intensity of the trapping light is periodically modulated. In
this system, chaotic dynamics exists for certain values of the modulation index,
and causes atoms to accumulate in rings corresponding to fixed points of the
system.
The ability to form billiards of arbitrary shape which can also be varied
dynamically, together with the precise control of parameters offered by laser-
cooling techniques, provide a powerful tool for the study of dynamical quantum
effects. These effects are expected to become important at lower temperatures
and smaller billiards. Very interesting in this context is the investigation of
the properties of a BEC trapped in an integrable or a chaotic billiard. Other
VI] DARK OPTICAL TRAPS FOR COLD ATOMS 147
VI. Conclusions
In this chapter, we have reviewed the main configurations that are used to form
dark optical dipole traps, and their principal applications. The formation of a
dark, blue-detuned trap is less obvious than that of a red-detuned one, and, as
discussed in Sects. III and IV, some of the effort in the last few years was
directed towards the generation of improved schemes, which are also easier
to implement experimentally. This effort has led to the development of traps
with larger volumes, better loading efficiencies, more efficient use of the laser
power and a larger darkness factor. We believe that dark optical traps have
matured and will now enter into more applications, in which their advantages
will be important. These will include precision spectroscopic measurements,
where the reduced interaction with the trapping field is crucial, and investigation
of atomic dynamics inside atom-optics billiards, both as a model system
for quantum and mesoscopic dynamics and as a tool to further improve the
accuracy of spectroscopic measurements. Other applications may benefit from
the ability to confine atoms with reduced interactions, including quantum
information processing in dark optical lattices, and possibly also quantum-optics
experiments which require long relaxation times of the atomic spins, such as
slow light (Hau et al., 1999; Kash et al., 1999), stopped light (Liu et al., 2001;
Phillips et al., 2001), and entangled atomic samples (Julsgaard et al., 2001).
Finally, the special light distributions employed to trap cold atoms can also be
used to trap electrons (Chaloupka and Meyerhofer, 1999), Rydberg atoms (Dutta
et al., 2000) and molecules (Seideman, 1999) using the ponderomotive force, and
to manipulate larger objects when used as dark optical tweezers (Sasaki et al.,
1992). In all these cases, the advantages of dark traps are twofold: The ability to
trap dark-field seeking objects (e.g. electrons, or metallic beads) and the reduced
light intensity to which the trapped object is exposed.
148 N. Friedman et al. [VII
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A D V A N C E S IN ATOMIC, M O L E C U L A R , A N D O P T I C A L PHYSICS, VOL. 48
I. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 153
II. Theoretical Models for Cold Atoms in Hollow Laser B e a m s . . . . . . . . . . . . . . . . 154
A. Strict Kinetic Theory . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 154
B. Dressed-atom Model . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 157
III. Generation Methods for Hollow Laser Beams . . . . . . . . . . . . . . . . . . . . . . . . . . 160
A. Mode-Conversion Method with Cylindrical Lens . . . . . . . . . . . . . . . . . . . . . 160
B. Computer-Generated Hologram Method . . . . . . . . . . . . . . . . . . . . . . . . . . . . 161
C. Spiral Phase-plate Method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 163
D. Geometric Optics Method with Axicons . . . . . . . . . . . . . . . . . . . . . . . . . . . 163
E. Micro-imaging Method for Hollow Fiber Modes . . . . . . . . . . . . . . . . . . . . . . 166
E Near-field Diffraction Method for Hollow Fiber Modes . . . . . . . . . . . . . . . . . 166
IV. Cold Atom Manipulation in Hollow Laser Beams . . . . . . . . . . . . . . . . . . . . . . . 170
A. Atomic Guidance in Hollow Laser Beams . . . . . . . . . . . . . . . . . . . . . . . . . . 170
B. Atomic Fountain with Hollow Laser Beams . . . . . . . . . . . . . . . . . . . . . . . . . 176
C. Atomic Traps with Hollow Laser Beams . . . . . . . . . . . . . . . . . . . . . . . . . . . 178
V. Acknowledgment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 188
VI. References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 188
I. Introduction
Atom optics has become an active and attractive research field, and numerous
novel atom-optical components that use optical or magnetic methods have been
developed [1-3]. Although magnetic atom optics is a promising approach to
realize coherent atom optics or miniaturized atom-optical elements, atom optics
utilizing optical schemes also provides unique and versatile tools for such stud-
ies. In particular, optical atom optics becomes more powerful when combined
with microscopic atom-optical elements on the surface or even with magnetic
atom-optical techniques.
Cold atoms have been manipulated by optical dipole potentials produced by a
hollow-core optical fiber (HOF)[4-7] and a hollow laser beam (HLB)[8-12].
]/2 V 2
H = Ho - ~ - D . E, (2)
where Ho describes the atomic energy levels E 1 , E 2 , E 3 , and the last term
describes the dipole interaction between the atom and the laser field. The
complete description of the time evolution of an atom can be then given by
the equations for the atomic density matrix in the Wigner representation. The
II] MANIPULATION OF COLD ATOMS IN HLBs 155
d /933 = i/r
( ei(k'r-6't) P(-)13 -- e-i(k'r-'5~t) P(-)'~31)
+iK'2 (e i(k'r-6zt) p~;) --e -i(k'r-62t) p(-))
32
- 2( Yl + Y2)P33
dld [ l l --iK'l
(e_i(k.r_(~,t)
p~l )-
ei(k.r_61t )
pi3 )) + 2y,
/ *(n)
p(n)
33
dan, (3)
d = iKl ei(k.r_6~ t ) ( p l l ) - p(+))
-dt/331
- 33 + itr e i(k'r-6zt) P~l)--( Y1 + 72)P31,
d
dt P32 = iir ei(k .r-,~t)( P~2) _ p(+))
33 + iK'l
ei(k.r-O,t) p(-)
12 - - ( Yl + Y2)P32,
Here the density matrix elements are defined with respect to the time-
dependent, stationary atomic eigenfunctions such that
where (a,b) - (1,2,3) and n is a unit vector that defines the direction of the
spontaneous photon emission. The halves of the Rabi frequencies, ~ , and the
partial spontaneous decay rates, )9, are defined by (j = 1,2)
In Eqs. (3), the function ~(n) describes the angular anisotropy of the spon-
taneously emitted photons. In our simplified model that neglects the atomic-
level degeneracy, the function ~(n) can be chosen to be isotropic such that
9 ( n ) - 1/4sz and f ~(n)dZn - 1. Note that the microscopic equations for the
considered model scheme do not include the integral term for the ground-state
coherence Pl2.
Assuming the interaction time exceeds the spontaneous decay time (tint >>
l"sp = 1/Wsp), one can expand the density-matrix elements in powers of photon
momentum hk. Moreover, when Tint >> Tsp , the Wigner density-matrix elements
become the functionals of the Wigner distribution function, w = w(r, p , t ) =
}-~3a .
= l Paa As a result, one can derive the Fokker-Planck kinetic equation for
156 H.-R. Noh et al. [II
the Wigner distribution function w(r, p,t), to the second order in the photon
momentum hk,
_ 02
0W (914' 0 (Fw)+ E ~(Diiw). (5)
Ot + v Or Op Opi
For a three-level atom, the Rabi frequencies are f2j = r v/[/(2[s)s 1/2 (j = 1,2),
where F = 27' = 2(7'1 + 7'2), I is the intensity of the laser beam, Is = ,rrhcF/(3A 3)
is the saturation intensity, fj. = @/(3areohc3F)l(eldj .eLlgj)l 2 is the relative
transition strength, ~. is the resonant transition frequency from le) to ]gj), and
eL is the polarization unit vector of the electric field EL. Note that the saturation
parameters can be written as G1 = j i G and G2 = J)G, where the reduced
saturation parameter are given by G = I/Is. Consequently, for large positive
detunings and slowly moving atoms (]k. v I << 61,62), the dipole force, the
spontaneous force, and their respective diffusion tensors can be obtained as the
following simple expressions [ 13]:
h VG
Fd = - ~ (ql ~1 + q262) --~-a ' (6)
Fr = hi{l-"Co' (7)
1 G
Dii = -i-~h2k2Fc0 , (8)
where Co = ql/fl + qz/f2 + 3G/2 + 4Cl/l -'2, Cl = qlOZ/fl + q262/f2, the optical
potential is obtained by Ua = - f Fa. dr, and qj = ))/(Yl + 7'2) defines the relative
spontaneous-emission rates for two photon-emission channels with j = 1,2.
The above general relations can now be applied directly to our problem of cold
atoms guided in a hollow laser beam. For an HLB, the dipole gradient force in
Eq. (6) pushes atoms to the central dark hollow region at blue laser detunings. We
assume that HLB is linearly polarized and described by the intensity distribution
Table I
The mean relative transition strengths, J), j = 1,2, o f several alkali atoms.
2 2 2
D2-1ine 3q j j j
or a + or a - j~
2j 2j 2
j
1 1 1
D 1-line fl j J J
1 1
Jr or a + or o- 3~ j J 31
Table II
Mean branch ratio qi, i = 1,2 from the excited state 13) decay to the ground state li) for the excitation
o f the ground state lJ) by the H L B , j = 1,2.
13 20 3
D2-1ine ~ = FI qI T8 ~
5 7 l
q2 l--g ~ 2[
1 5 7
Fj=F2 ql $ ~ 3-6
5 22 29
q2 ~ 2--7 3-6
Dl-line Fj = F l ql ~4 ~13 I
5 14 1
q2 ~ ~-7
1 10 7
/~ = F2 ql ~ ~ 1--8
2 17 11
q2 j 2--7 1-8
For numerical calculation of atomic dynamics, the values o f f for several alkali
atoms are listed in table I. We find that in the case of the traveling-wave laser
field, the values o f f are independent of the polarization o f the laser field. In the
case of D2-1ine transitions, for example, J] =j~ = 2 for all alkali atoms as listed
in table I. In addition, table II presents the relative spontaneous emission rates,
qj (j = 1,2), from le) to [ g j ) [ 1 4 , 1 6 ] .
B. DRESSED-ATOM MODEL
where F is the spontaneously decay rate of the excited state [e) [1 4]. Furthermore,
under the electric-dipole and rotating-wave approximations, the dressed-atom
Hamiltonian at point r within the manifold En can be written as [ 17,1 8]
2
H,(r) = Z {-h(coL - 6j) bjbf - [dj- EL(r)bfaL + dj . t~(r)bja~]} + hcoLa+taL,
j=l
(12)
where the first term describes the atomic energies, the second term is the atomic
dipole interaction Hamiltonian, and the last term represents the laser field. Here
bj = Igj) (el is the lowering operator, bf = ]e) (gj] is the raising operator, dj is the
electric-dipole-moment operator, eL(r) is the laser field, and a~ (aL) is the cre-
ation (annihilation) operator of a photon. In this model, the laser field is also cho-
sen as a spatially inhomogeneous monochromatic laser wave as given in Eq. (1).
In a manifold E~, each eigenstate is given by a linear superposition of three
basis states,
]i(n)) = aTl ]gl,n + 1) +a72 ]g2,n + 1) + a73 ]e,n), (i = 1,2,3), (13)
where ~-~=, lai~ 12 = 1 according to the time-independent Schr6dinger equation,
H~ [i(n))- E,i li(n)). Therefore, the matrix form of H~ becomes
where
ff2j/2
bij = n~oc + 6j - E n i / h ' (16)
with i = l, 2, 3 and j = 1,2. Consequently, the eigen-energies of Hn,
E~i = nhO)L + Ei, (i = 1,2, 3), are given by
2(n))
En / ~ [gl'n+l)/ ~ l(n))
V-
03 L
P Pm o Pm P
FIG. 1. Dressed states for a three-level A-atom interacting with a HLB for positive detunings
(aj, 62 > 0).
the center of HLB, ff2j tends to vanish and thus the atomic levels approach the
uncoupled-state levels.
Taking into account the coupling of the dressed atom with the vacuum-field
reservoir, responsible for spontaneous emission between adjacent manifolds,
one can write a master equation for the density matrix o of the dressed
atom, which describes both the internal free evolution of the dressed atom
and the relaxation due to the atom-vacuum coupling. If we denote three
reduced populations by ;ri(r), corresponding to three dressed states ]i(n)) defined
by ~i(r) = ~-~n (i(n) l~ the evolution of 3-gi is described by
~ = ~-]~i~j(-FijJrj. + Fji:ri) with (i, j) = (1,2,3). Here the rate of transfer Fik
from ]k(n)) to ]i(n - 1)) is given by Fik = ~ - ] 2 Fjaoak3"
2 2 The resulting steady-
state solutions are then calculated as
MS~t = q , f 262
qlf262 + qzf162, (19)
qzflb2 (20)
:r~t = qlf262 + qefl 62,
;r~t = JiJ~GZF4 qlflb2 + qzfzb2 (21)
6462 62 q l j~ 62 + q zj] 62.
160 H.-R. Noh et al. [III
Consequently, the radiation force, the momentum diffusion tensor, and the dipole
force can be obtained as [ 15,17]
Dii : gh
1 2 k 2 rp~', (23)
2
Fa = - Z ygstvui, (24)
i=1
A hollow laser beam (HLB) is a laser beam whose intensity along the central
axis vanishes, having a doughnut-shaped intensity distribution. HLBs include
a ring-shaped TEM~)l mode, high-order Laguerre-Gaussian (LG) beams, high-
order Bessel beams, and vortex solitons. Here we review several methods that
have been developed to generate an HLB, such as the vortex grating method [ 19],
transverse-mode selection [20], direct production from a laser [21 ], the optical
holographic method [22], computer-generated holography [23], mode conversion
from Hermite-Gaussian to LG by use of two cylindrical lenses [24,25], spiral
phase-plate methods [26,27], geometrical methods with axicons [11,28] or a
double-cone prism [29], and use of a hollow-core optical fiber (HOF)[30].
Both the Hermite-Gaussian (HG) and the Laguerre-Gaussian (LG) modes form
complete sets of solutions to the paraxial wave equation [31]. The rectangularly
symmetric HG modes are described by the product of two independent Hermite
polynomials, describing the field distribution in the x and y directions. They
are characterized by integer subscripts m and n representing the order of the two
polynomials, that is, the number of nodes in the electromagnetic field. In contrast,
the circularly symmetric LG modes are similarly denoted by LGlp, where l is the
number of 2Jr cycles in phase around the the circumference and (p + 1) is the
number of nodes across the radial field distribution.
III] MANIPULATION OF COLD ATOMS IN HLBs 161
l(Z)
~p(z) = (m + ~) arctan
ZRx
+(n+ 89
(z)
~
ZRy
. (25)
Note that it is the Gouy phase shift occurring in the presence of a cylindrical
lens that forms the basis of the mode converter.
The generation of an LG beam was first demonstrated by Beijersbergen
et al. [24,25] by transforming an HG mode of arbitrarily high order to an
LG mode. They used a mode converter that consisted of two cylindrical lenses.
Unlike other methods discussed in the remaining part of this section, this method
can produce pure LG modes. Figure 2 shows how the HG~,0 mode rotated at 45 ~
with respect to the x- or y-axis is equivalent to the sum of the HG~,0 and HG0,~
modes, and how these two modes are related to the LG~ mode. Specifically, the
LG~ mode can be formed by a superposition of HG1,0 and HG0,1 modes with a
phase difference of Jr/2.
B. COMPUTER-GENERATEDHOLOGRAM METHOD
FIG. 2. Generation of LG1 mode HLB by mode-conversionmethod (from Padgett et al., 1996,
Am. J. Phys. 64(1), 77, Fig. 2, reprinted with permission).
Bessel beam. By using the CGH method, Heckenberg et al. generated a TEM~)1
doughnut mode [40], a TEM~0 doughnut mode [41], and later an LG~ mode [42].
In particular, by using the LG beam, they demonstrated trapping of reflective and
absorptive microscopic particles, which cannot be trapped by using a Gaussian
spot due to the strong repulsive forces.
Paterson and Smith [23] produced high-order Bessel beams by using an
axicon-type CGH, where an azimuthal phase factor, exp(inq)), is added to the
phase of the hologram. The Bessel beam [43] is one of the propagation-invariant
waves and has an amplitude proportional to Jn(por)exp(in(~), where J,, is the
nth-order Bessel function of the first kind, r is the radial coordinate, q~ is the
azimuthal coordinate, and P0 is the radial spatial frequency. The zero-order
Bessel beam has a sharp intensity peak at its center, while higher-order Bessel
waves have zero-intensity minima at their centers. Paterson and Smith calculated
the amplitudes of the waves produced by an axicon-type hologram by using the
Kirchhoff integral, and experimentally demonstrated the production of Bessel
beams of orders 1 and 10.
Clifford et al. [44] generated LG laser modes with an azimuthal mode index l
ranging from 1 to 6 (p = 0) by using an external cavity diode laser. The
transmittance function is given by T(r, 4))= exp[i6H(r, r in polar coordinates,
where 6 is the amplitude of the phase modulation, and the holographic pattern
is given by
H(r, r = ~ mod lq~ - --~r cos 0, 2~ , (26)
with mod (a, b) = a - b int(a/b). As the azimuthal index l increases, the inner
III] MANIPULATION OF COLD ATOMS IN HLBs 163
dark region of the light becomes larger and the outer ring becomes narrower.
The conversion efficiency was as high as 40% and the efficiency was claimed
to increase by using a phase hologram and blazing it to maximize the power
in a chosen diffracted order. In general, when a hologram is irradiated by a
fundamental Gaussian mode, the output becomes a superposition of an infinite
number of LG modes with the same l and different p. The fraction of p = 0 mode
was 78.5% in the first diffracted order. In an analogous method, they also
generated multi-ringed (p > 0) LG modes with azimuthal index l = 1 [45].
Beijersbergen et al. [26] demonstrated that a spiral phase plate can convert a
Gaussian laser beam into an LG mode with a phase singularity on its axis.
A spiral phase plate is a transparent plate whose thickness increases in proportion
to the azimuthal angle q~ around a point in the middle of the plate. If u(p, q~,z)
is the complex amplitude of the incident beam, the amplitude u I directly after
the plate is given by u' = u exp(-iA/r where Al is the height of the step in
wavelengths given by Al = A n h / X , h is the step height at r = 0, An is the
difference of refractive index between the plate and its surrounding, and X is the
vacuum wavelength.
Beijersbergen et al. chose an acrylic (PMMA, n = 1.49) as a phase plate,
where h = 0.72mm or Al = 577 at 633 nm wavelength. To make Al = 1, the
plate was immersed in a liquid with nearly the same index of refraction. The
effective step size was tuned by controlling the temperature, and they obtained
Al = 1 with An = 8.7x 10-4. They used an LG ~ or LG~ beam as an incident
laser that passed through a phase plate, and the output beam was imaged by a
lens in the focal plane. For each incident beam, the output beam was obtained
with various values of Al ranging from -1 to 2.5 with a step of 0.5. For the
LG ~ mode, a nearly LG~ beam was obtained ( A / = 1). For the LG 1 mode, which
itself is already a helical mode, a mode similar to the input beam was obtained
when Al = 2.
Turnbull et al. [27] generated free-space LG modes at millimeter-wave
frequencies (-100 GHz) by using a spiral phase plate. Due to the large frequency
difference of-104 with respect to the optical field, the orbital angular momentum
is also -104 times smaller. The phase plate was made of polyethylene, which has
a refractive index of 1.52 at millimeter-wave frequencies. They could generate
LG 1 and LG 2 modes with phase plates of step height 6.7 mm and 13.4 mm,
respectively.
Since the time Herman and Wiggins [46] used an axicon [47] to produce a
164 H.-R. Noh et al. [III
FIG. 3. Generation of HLB by axicons (from Manek et al., 1998, Opt. Commun. 14"/, 67, Fig. l,
reprinted with permission).
the dark spot inserted, the intensity at the center was ~0.1% of the maximum
intensity of the ring.
Song et al. [11] used a series of axicons (each with a 3 ~ base angle) and
a simple lens. A hollow beam generated thereby has different focal points for
the inner and outer walls. Therefore, two additional axicons were required to
control the core diameter and wall thickness. An important byproduct of this
arrangement was that most of the diffraction originating from the tip of the first
axicon was located outside the core. Since the LG beams are not generated by
axicons, this HLB generally does not propagate indefinitely, nor is the dark core
preserved when the beam is focused by a simple lens. Nevertheless, a HLB that
is usable for tens of centimeters can be produced routinely, which is useful for
guiding atoms.
A double-cone prism was also used for the generation of HLB by Ito
et al. [29]. Figure 4 explains the conversion mechanism by a double-cone prism.
A Gaussian beam is divided into two parts by the first refraction at the apex of the
prism, and then a nondivergent doughnut-shaped hollow beam appears from the
other side after the second refraction. When a prism with a length of 4.3 mm
and a full apex angle of 90 ~ is used, the inner and outer diameters of the
doughnut-shaped light beam are 0.6 and 1.4 mm at e -1 intensity, respectively.
Although the characteristic feature is not better than can be produced with
multiple axicons, this method is very simple and convenient and is useful, for
example, for generating evanescent waves at the conical hollow prism.
An axicon was also employed for the transformation of an LG beam to
a high-order Bessel beam by Arlt and Dholakia [49]. If an LG mode with
azimuthal mode index l is used to illuminate an axicon placed at its beam
waist, an approximation to a Bessel beam of order I is generated (Fig. 5). First,
they obtained LG modes by the computer-generated hologram method [42]. The
LG beam had a waist of w0 = 2.5 mm and the axicon was positioned at its
beam waist. They generated Bessel beams with orders l = 1 to 4. The radius of
the inner ring of the generated first-order Bessel beam was only rm = 21.2 ~tm,
and it propagated about Zma• = 29 cm without any spread. This should be
compared with an LG beam with I = 1 and the same ring size at its waist, which
would have a Rayleigh range of only about 4 mm. The conversion efficiency was
almost 100%, limited only by the CGHs used to produce the LG beams.
166 H.-R. Noh et al. [III
FIG. 5. Generation of a high-order Bessel beam within the shaded region by illuminating an
axicon with an LG mode (from Arlt et al., 2000, Opt. Commun. 177, 297, Fig. 1, reprinted with
permission).
J
0')
(/) soo
t'~ 2o0
100
0 ~,,. t .... t .... i, ~., 1 .... I , ,
~
0 2oo 4oo 000 Boo 1000
Z(mm)
700 (b)
~eoo
E=1 r~o~ M - 4 0 X Objective
CO
IZI z~0
lO0
Z(mm)
FIG. 6. The relationship between the DSS and the propagation distance Z of the HLB measured
with (a) M-20• and (b) M-40• objective lens.
z 1 exp(ikp)
E(x,y,z) = - ~ ~ ~ E~ P - ik p2 clxo dyo, (28)
168 H.-R. Noh et al. [III
10 0 r (~tm) 10 0 r (~tm)
where (r, 0) are the cylindrical coordinates of (x, y). Here U)~ that is, the Fourier
transform of Et~ can be obtained analytically as described in Ref. [54].
Figure 7a explains how the LP01 mode diffracts in free space near the HOF: the
two peaks at z - 0, representing a cross section of ring-shaped mode, diminish
away while an additional central peak grows. In Fig. 7b one can find that the
peaks of LPll also diminish whereas another pair of peaks grow. In this case,
however, there still does exist a dark column along the central axis. A doughnut-
shaped HLB can then be produced as follows. For a given propagation constant,
there are four degenerate LPll modes, whose respective polarizations and angular
variations are described by ~ sin(0 + q~),)3 cos(0 + q~),~ cos(0 + r and)3 sin(0 + q~)
[58]. One can easily find that superposition of the first two or the last two modes
can produce an azimuthally symmetric mode. The output beam then forms a
doughnut-shaped HLB since it is just a superposition of the output fields of two
orthogonal LPll modes. The resulting combined beam in front of the HOF may
look like a single linear-polarized beam with its plane of polarization rotated
by 45 ~ with respect to the horizontal plane. One should note, however, that each
beam can be adjusted separately, which is important in exciting modes that differ
from one another.
The first two images in Fig. 8 represent the independent mode patterns of
two perpendicular modes at z = 0 before they are merged, and the last image
III] MANIPULATION OF COLD ATOMS IN HLBs 169
Fie. 8. Superposition of two orthogonal LPll modes to obtain HLB. Transverse intensity profiles
at z = 0 are shown: (a) and (b) present the images before superposition, (c) shows the superposed
image. Polarization and angular variation of the corresponding electric field can be described by, for
example, (a) ~ sin(0 + r and (b) ~ cos(0 + r
Fl~. 9. Characteristic dimensions of the diffraction-limited dark hollow spot, measured in terms
of the dark-spot radius Rmax and the halfwidth w, which is in good agreement with the numerical
simulation.
shows their combined pattern, which is similar to that of the LP01 mode. At a
distance z = 250 ~m, the peak-to-peak distance is about 17 ~tm and the dark spot
size is about 8.2 ~tm. Its azimuthal isotropy was checked by measuring the beam
profiles along eight different radial axes and they showed good uniformity within
the maximum uncertainty of about 7%.
In a later experiment, the same group [59] also obtained the diffraction-limited
dark spot near the HOF facet. Figure 9 shows the development of the radial
intensity and the size of the dark hollow region, which is equivalent to the
calculations presented in Fig. 7b. The minimum size of the dark spot, Rmax, is
about 2 txm, the halfwidth of the dark spot, w, is under 1 ~tm, and the inner peaks
are diverging with a 40-mrad diffraction angle. The experimental results were
in good agreement with the numerical calculations obtained by the Rayleigh-
Sommerfeld theory and the weak guiding approximation. The small dark spot
may be applicable as an atomic lens which focuses atoms to a small spot or as
an optical dipole-force microtrap by combining several beams.
170 H.-R. Noh et al. [IV
0- 9 Copropagating
~..~ Counterpropagating
"~ 40-
30,
20,
.-~ 10.
(-9 O
-4-~_ o 2 ~, 6 8 io i2 i4 i6
Detuning~i2(GHz)
FIc. 11. Guiding efficiency as a function of the detuning 62 in the (a) copropagating and (b)
counterpropagating schemes. The solid curves represent numerical simulation results.
with higher power, larger detuning, and colder atoms. For example, simulation
shows that when the HLB has 500 mW power and 220 GHz detuning, more than
30% of the atoms at 2 ~tK temperature can be guided over a distance of 30 cm
without any spontaneous emission and with an average photon scattering rate
much less than 1 s-1.
Schiffer et al. [ 10,60] have demonstrated guiding and focusing of atoms in the
dark region of a holographically generated HLB. They performed experiments
with metastable neon atoms. A laser-decelerated and compressed atomic beam,
having a high brightness of 5• 1012/sr/s [61], is injected into the dark region
of a blue-detuned doughnut mode. The longitudinal velocity is 28 rn/s with a
rms width of 4 m/s. The atoms are injected into the doughnut mode through
a 30-mm-radius hole in a dielectric mirror at 45 ~ Behind the mirror, the flux
is 1.4 • 10 6 atoms per second with a transverse Gaussian velocity distribution,
having the spread a. = 7.8 cm/s=2.5Vrec, where Ure c = hk/m is the photon
recoil velocity. They used a computer-designed blazed phase hologram that was
produced by a direct laser-writing technique [62].
Figure 12 shows the normalized atomic intensity in the focal plane as a
function of the doughnut-mode well depth for a waist w0 of 50 ~tm and a power
of 300mW. For a shallow potential, only a minor part of the atomic beam
was captured by the guiding potential when entering the doughnut mode. By
increasing potential height, however, a growing number of atoms was trapped
and guided. The experimental curve in Fig. 12 provides slightly lower guiding
1/ [1/OHz]
0.00 0.02 0.04 0.06 0.08
,,
| i !
I-, I
2000
1500
0 50 I00
o
N
I000
Q 500
z
Urnax[ 103Eree]
FIG. 12. The dependence of the atomic intensity enhancement on the maximum light shift for
atom guiding in a blue-detuned doughnut-mode HLB (open circles) and in a red-detuned Gaussian
mode (solid circles). The dashed and solid curves present the results of the numerical simulation.
The plot for a wider range is shown in the inset (from Schiffer et al., 1998, Appl. Phys. B 67, 705,
Fig. 2, reprinted with permission).
IV] MANIPULATION OF COLD ATOMS IN HLBs 173
Fie. 13. Atoms loaded into a HLB waveguide from a Rb BEC with different evolution times
inside the waveguide (from Bongs et al., 2001, Phys. Rev. A 63(3), 031602, Fig. 4, reprinted with
permission).
efficiency compared to the simulation result. For Umo~ - 8500Eree, the atomic
intensity is enhanced by a factor of 1600. In this case, (60+ 10)% of all atoms
injected into the doughnut mode are captured and guided. The inset of Fig. 12
shows that for high Umo~ the enhancement factor is expected to reach values
well above 3000. For Uma~ = 2000Erec, the flux is 8 • 105 atoms/s, the density is
2 • 108 cm -3, and the intensity is 6 • 1011 (cm -2 s -1). In particular, they achieved
a factor of 10 improvement in atomic flux by using the doughnut mode, and a
factor of 80 with a TEM~)5 mode.
Recently, the transfer of Bose-Einstein condensate (BEC) into a quasi-lD
waveguide created by a blue-detuned HLB was also demonstrated by the same
group [63]. The combined optical dipole and magnetic (DM) trap consists of a
waveguide added to the 3D potential of a Ioffe-type magnetic trap. It allows for a
natural connection between the magnetic trap and a pure 1D waveguide geometry
created by an LG (TEMPI) laser beam. With a power of P = 1 W at 532 nm
and a beam waist of r0 ~ 10 ~tm, a dipole potential at the focal plane with a
maximum value of ~120~tK and a transverse oscillation frequency of ~6 kHz
(corresponding to 570nK) for 87Rb atoms can be realized. They investigated
the transfer process of BEC into a blue-detuned dipole waveguide and studied
the subsequent evolution of the ensemble in a quasi-lD waveguide. Figure 13
shows guiding for evolution times up to 500 ms. On time scales above 40 ms,
the conversion of mean-field energy into kinetic energy is nearly complete and
the ensemble is expected to expand with constant velocity, keeping its parabolic
density distribution. In these experiments they demonstrated that a fully coherent
transfer is possible, and they observed a mean-field-dominated expansion of the
ensemble for adiabatic loading conditions.
1.5
x
v
1.0
0.5
o.o . . . . . I ~ c~|
0 50 100 150
UKE (=,)
Fl6. 14. Number of atoms in the HLB tunnel as a function of time, measured from longitudinal
images (squares) with the repumper, those without the repumper (diamonds), and those in the
presence of the repumper but with the kicking beam placed 10 cm below the MOT (triangles) (from
Song et al., 1999, Opt. Lett. 24(24), 1805, Fig. 4, reprinted with permission).
described in Sect. III.D. The source of cold atoms was a vapor-loaded Cs MOT
containing - 1 0 9 atoms. The guide beam and the major axis of the MOT were
aligned and oriented in the vertical direction. The atoms are transferred to the
tunnel by turning the MOT beams off. They then monitored the evolution of the
cloud of atoms (size, location, and density) by the absorption shadow the cloud
of atoms casts on a CCD camera.
They showed that the center of mass of the cloud in the transverse
direction has an acceleration o f - 1 5 m / s 2, appreciably larger than the gravita-
tion g ( ~ 9.8 m/s2). They also found that when the guide beam is directed against
gravity and detuned by less than 1 GHz, it is possible to levitate the center of
mass of the cloud. In the one-dimensional case, in which the atoms are restricted
to radial motion, they find that the average acceleration /asc)ensemble ~ 1/V/A
to first order, in qualitative agreement with the observations (A is the laser
detuning). They also measured the number of atoms in the tunnel for times well
beyond 35 ms by taking images in the longitudinal direction (Fig. 14). With the
r e p u m p e r , - 1 0 s atoms make it to the bottom of the chamber, whereas without
the repumper, they detect no atoms at the bottom. As the triangles in Fig. 14
show, nearly all the atoms are kicked out of the beam before hitting the window.
Although only 3% of the atoms go through the tunnel as shown in Fig. 14
(A ~ 1.5 GHz), the efficiency was about 10% when they reduced the detuning
to increase the atomic speed.
IV] M A N I P U L A T I O N OF C O L D ATOMS IN HLBs 175
FiG. 15. (a) CCD image of the low-velocity rubidium beam split and guided by the HLB.
(c) Spatial profile of the rubidium beam taken at the place indicated by the arrow. (b) and (d)
show the corresponding image and the spatial profile without the HLB (from Yan et al., 2000,
J. Opt. Soc. Am. B 17(11), 1817, Fig. 4, reprinted with permission).
A. 4. H L B s p l i t t i n g o f Rb
Yan et al. [64] guided a continuous low-velocity atomic beam and achieved
incoherent splitting of the atomic beam with the HLB. A low-velocity intense
source of atoms (LVIS) was generated by the method demonstrated by Lu
et al. [65]. An HLB was generated by an axicon setup that converts a Gaussian
beam from a Ti:sapphire laser into the HLB as explained in Sect. III.D [28].
A convergent HLB with a full convergence angle o f 5 ~ was generated from a
collimated HLB with a dark center diameter o f ~1 cm.
With the intercepting angle a = 0, they investigated the effect o f the HLB for
the guiding. The result was that, owing to the HLB guiding and collimating or
focusing, the rubidium flux was increased by ~20% and the spatial width was
reduced from 0.9 mm to 0.7 mm. Figure 15a shows the CCD image of the LVIS
split and guided by an HLB with a convergence angle o f ~ 5 ~ and intercepting the
LVIS at a ~ 8 ~ The top of the image was about 4 m m below the center o f the
MOT. Spatial separation of the LVIS is observed: one atomic beam is propagating
downward and a second atomic beam is produced by the atoms guided by the
HLB along the propagating direction of the HLB. This effectively realizes an
incoherent atomic beam splitter. For comparison, Fig. 15b shows the CCD image
of the LVIS without the HLB. Figures 15c and 15d plot the cross-sectional spatial
profiles of the rubidium atomic beams taken at a distance o f 9 m m below the
MOT. The maximum atomic flux guided by the HLB is 50% o f the flux intensity
of the free-traveling rubidium beam without the HLB.
176 H.-R. Noh et al. [IV
The development of an atomic fountain based on laser-cooled atoms [66, 67] has
created prospects for an improved accuracy and stability of frequency standards.
In such a clock, one approach to solve the line shift due to cold collisions is to
use laser light for guiding the upward-launched atoms [68]. This is because the
guiding can enhance the number of atoms which come back into the microcavity
without increasing the atomic densities.
Optical guiding of an atomic fountain by using a cylindrical HLB was recently
demonstrated by Kim et al. [69]. They generated an HLB by using the micro-
imaging method described in Sect. III.E. It was collimated by the objective lens
and propagated downwards toward the center of the Rb MOT. The power of
the guiding laser was 250 mW and the beam waist was 3 mm. The HLB was
nearly collimated in order to remove the dipole force of the guiding direction,
which can cause broadening of the spatial distribution of guided atoms. With an
intensity of 3 mW/cm 2 in each beam, the typical diameter of an atomic cloud
in the MOT was about 1 mm, and the number of trapped atoms was typically
2 • 107. Cold atoms were then launched upwards in a rather simple way by rapidly
varying the vertical magnetic field, resulting in the atomic Zeeman shift. After
1-ms acceleration, the detuning of the laser beams was changed from -2.5F to
-70F, lowering the atomic temperature to 33.7 ~tK in the frame moving upwards.
A typical launching velocity of ascending atoms was 1.4 m/s and the atoms were
launched up to 10 cm.
The number of guided atoms was detected by observing with a photomultiplier
tube the fluorescence induced by a horizontally placed probe laser at 10.5 cm
below the center of the MOT. They observed that 0.5% of the launched atoms
were detected without the HLB. On the other hand, a tenfold enhancement
of the HLB-guided atomic fountain was clearly obtained without appreciable
heating. In Fig. 16, curve (a) is the time-of-flight (TOF) signal of atoms
launched without the HLB, while curve (b) is the TOF signal with the HLB
at a detuning of 19 GHz. From this TOF signal, one can deduce the guiding
efficiency of atoms and the temperature. Without the HLB, the temperature was
about 33.7 (-+-2.1) ~tK; with the HLB it was about 34.4 (• ~K.
To characterize the enhancement due to the guiding HLB, they introduced the
enhancement factor, defined as the ratio of the number of atoms guided with
the HLB to that without HLB. In Fig. 17, the curve with solid squares shows
the relationship between the enhancement factor and the detuning measured
with respect to the 5S1/2,F = 2 ~ 5/93/2 transition line. The inset shows
the enhancement of the guiding efficiency for larger detuning. The curve with
open circles shows how the number of scatterings, or the heating, is changed
with the detuning. They observe that for small detuning the enhancement factor
is more than 35, but there is serious heating. As the detuning increases, the
enhancement factor as well as the heating decrease. Note that the number
IV] MANIPULATION OF COLD ATOMS IN HLBs 177
10
P = 250 mW
.~,08
6z = 19 G H z
.I=I
Vlaunch---- 1.4 m / s
5
HLB
"r - " 0 6
1:1 04
Q
HLB ~{j~~
9 o2
O0 _ .~' . _ ~ _.. ~ ,, _, . . . 7 . . . ,,. _ l.~.-. ,, ,.._ ,_ T , - ~ , ....... ~._~L I ' " "I
0 05 010 015 0 20 0 25 0 30 0 35 0 40 0 45
FIG. 16. TOF signals in the HLB-guided atomic fountain experiment: (a) without the HLB;
(b) with the HLB.
The first optical dipole trap consisted of a strongly focused Gaussian laser
beam, detuned to the red side of the atomic resonance line [72]. Since then,
several schemes have been realized to reduce the scattering rate that limits the
trap lifetime [73], such as a far-off-resonance trap (FORT)[74] and far-detuned
traps operating with Nd:YAG [75] or CO2 [76] lasers. Since the large scattering
rate or the ac-Stark energy shift is a serious obstacle to precision spectroscopy,
blue-detuned optical dipole traps have been designed to provide lower scattering
rate and less energy shift by using the fact that atoms mostly remain in the region
of low laser intensity.
Before the advent of HLB, Davidson et al. [70] at Stanford demonstrated
the first blue-detuned dipole trap by using two sheets of Ar + laser beams. The
beams intersect at 90 ~ forming a V-shaped cross section, and provide a strong
confinement perpendicular to the beam propagation axis. Confinement along the
laser propagation axis is provided by the divergence of the focused light sheets.
In this trap, a 1/e coherence decay time of 4.4 s was obtained. A linewidth of
0.125 Hz and a Ramsey fringe contrast of 43% were also obtained. The coherence
time was 300 times longer than that achieved in a red-detuned Nd:YAG laser
dipole trap with a comparable trap depth. In a later experiment, they used two
pairs of light-sheets, forming an inverted pyramid [77]. After Raman cooling,
4.5• 105 atoms were loaded at a temperature of 1.0~tK to a final density of
4 • 10 ll cm -3 with 1/e lifetime 7.0 s. In this subsection, we discuss several types
of atom traps that use blue-detuned hollow laser beams.
C. 1. Single-HLB trap of Rb
Kuga et al. [8] have demonstrated a novel optical dipole trap using an LG laser
beam. Precooled Rb atoms were trapped in the dark core of the doughnut beam
(2D trap). Because there was no restoring force along the axial direction, they
IV] MANIPULATION OF COLD ATOMS IN HLBs 179
, - 9 . ,,,
10 a
o
L..
i1)
.io
E
r 107
, ! | i ~ , t
FIG. 18. Decay of atoms from the 2D (circles) and 3D (squares) trap (from Kuga et al., 1997,
Phys. Rev. Lett. 78(25), 4713, Fig. 4, reprinted with permission).
loaded in the dipole trap to be 2x 108 (loading efficiency from the MOT to the
dipole trap was 30%). The time constant of r = 1.5 s was consistent with losses
due to collisions with background gas. This indicates that the trap loss due to
heating could be efficiently suppressed by pulsed PGC. The temperature of the
trapped atoms was 13 gK, close to the temperature of 10 ~tK achieved by PGC
just before the dipole trap was turned on.
e , , , ,
e -1 o ~
Zo e -2
~- e-S
e -4
-5 I I
I
e o 5 lo 15 20 25
time (s)
FIG. 19. Number of atoms in the GOST versus storage time at a rest gas pressure of
4.2x 10 - l ~ mbar (solid circles) and 7.6x 10 - l ~ mbar (open circles). The solid lines are exponential
fits (from Ovchinnikov et al., 1997, Phys. Rev. Lett. 79(12), 2225, Fig. 3, reprinted with permission).
IV] MANIPULATION OF COLD ATOMS IN HLBs 181
and p = 7.6 • 10-l~ mbar). In about 1 s, the decay is found to be exponential with
1/e lifetimes of (6.0-+-0.1)s and (3.2• respectively. These results suggest
that, besides small transfer losses of ~30% observed in the first second, losses
from the GOST are essentially due to rest-gas collisions. From the TOF method,
they obtained the vertical and horizontal temperatures To = (3.0+0.1) ~tK and
Th = (3.1-+-0.3) ~tK after 4 s of storage and cooling in the GOST. Both have equal
values within experimental uncertainty. In order to study the cooling dynamics,
they also performed a series of measurements on the temperatures To and Th as
a function of the storage time in the GOST. They obtained the EW cooling rate
to be 1/fi = (380-+-20)ms, which is in good agreement with the predicted value
of 1/fl = (400• ms [16].
Ovchinnikov et al. also demonstrated a gravito-optical dipole trap, which
used an intense blue-detuned conical HLB together with gravity to confine an
ensemble of cesium atoms in a dark spatial region, producing a conical atom trap
(CAT) [79]. The conical trapping beam with an opening angle of 0 ~ 150 mrad
is generated by using two identical axicons: in a telescope-like arrangement, a
Gaussian laser beam is transformed into a collimated HLB. This tubular beam
is then focused with a spherical lens to generate the conical HLB with its
apex located in the focal plane. In the focal plane, the beats profile is roughly
Gaussian with a diameter of about 100 ~tm. Within a few millimeters, the beam
profile evolves into a ring shape in resemblance to a higher-order LG mode [8].
Along the symmetry axis, the intensity distribution is approximately Gaussian
and decreases to 1/e of its peak value (maximum optical potential of ~50 mK at
3 GHz detuning) within an estimated distance of ~700 ~tm.
They have demonstrated the storage of Cs atoms in the CAT with a lifetime
of several seconds, limited only by collisions with the residual gas in the
vacuum chamber. After a variable storage time in the CAT, atoms were retrapped
into the MOT and a fluorescence image was taken with a CCD camera. The
corresponding experimental results are shown in Fig. 20 for two different values
of the residual gas pressure in the vacuum chamber (p - 2.5 x 10-1~ mbar and
6.9• 10-1~ mbar). An exponential decay is observed with lifetimes of 7.8s and
2.8 s, respectively. This indicates that collision with the residual gas is also
the predominant loss mechanism of atoms in the CAT. The measurement also
demonstrates a very high transfer efficiency from the MOT into the CAT of
about 80%. This corresponds to an absolute number of ~8 • 105 atoms initially
stored in the CAT. The atoms in the CAT are cigar shaped, with the diameter of
about 100 ~tm and the length of about 1 mm. The peak density is on the order
of 1011 cm -3 with about 10 6 atoms in the CAT.
Webster et al. [80] demonstrated a dipole trap by using a blue-detuned
LG-mode HLB based on the geometry proposed by Morsch and Meacher [81 ].
An LG-mode doughnut-shaped beam was produced by a mode converter
(Sect. III.A) from an HG beam emitted by an argon-ion laser. The doughnut-
182 H.-R. Noh et al. [IV
! | ! |
-!
e
e -2
z
e -B
-4 i 9
e
o 5 10 15 20 25
t i m e (s)
FIG. 20. Measurement of the storage time in the CAT as a function of storage time. The measured
lifetime is 7.8 s at a background pressure of 2.5 • 10-1~ mbar (solid circles). At 6.9x 10-l~ mbar (open
circles), a lifetime of 2.8 s is observed (from Ovchinnikov et al., 1998, Europhys. Lett. 43(5), 510,
Fig. 2, reprinted with permission).
shaped beam was expanded by a telescope to a beam waist of 3.5 m m and then
focused by a lens of focal length 25 mm, located one focal length from the centre
of the trap. To make the temperature o f the atomic cloud less than the height o f
the potential barrier, and to make the cloud small enough to fit inside the cone,
the cesium atoms were evaporatively cooled in a magnetic trap [82] to give a
temperature of 1 ~tK and a cloud diameter in the horizontal plane of 150 ~tm.
The size of the trapped cloud was roughly 100 ~tm radially and 200 ~tm axially,
elongated in the direction of the beam axis. To increase the trap depth, they
noted that a better method for achieving a higher dipole potential would be to
use a holographic technique for producing the HLB, since holography enables
one to reproduce an arbitrary waveform from a Gaussian laser beam with an
efficiency greater than 90% [60]. In particular, they demonstrated application to
a rubidium BEC. A condensate was formed in a magnetic trap positioned above
the apex of a focused doughnut-mode HLB and then released so that, falling
downwards, it would be funnelled towards the focused region, which thus realizes
a condensate propagating through a small orifice. This may permit investigation
of the superfluid flow in Bose condensates produced by evaporative cooling in
the magnetic trap.
C.3. C r o s s e d - H L B trap o f Rb
o~ 100.
",~176
or 8O
] 9 Experimental data
--
9 6o
o "., .... S i m u l a t i o n result
a::
4O
t:D "-..
c
~.
9 20 "-J[.,
D. ...
tO "" . . . . . . . . ;b'" "e. . . . . . .
'- 0
2'o 4'o 8'o ~oo
9 , 9
0 60
Trapping time (ms)
FIG. 21. The trapping efficiency of a crossed-HLB trap as a function of the trapping time. The
two horizontal HLBs have powers of 200 and 400 roW, the detuning of each HLB is 20 GHz, and
the initial temperature of atoms is 16 gK.
They estimated that 60% of the atoms in the MOT were initially loaded in the
HLB trap.
The number of atoms trapped, and their temperature, could be deduced by
TOF measurements. They found that the temperature of the trapped atoms was
about 7 gK and this value was close to the minimum height of potential barrier of
10 gK, where about 105 atoms stayed inside the trap for 100 ms and the lifetime
of trapped atoms was about 20ms as shown in Fig. 21. Figure 21 also shows
the trapping efficiency as a function of the trapping time. For comparison, the
simulation results based on Eqs. 6 - 9 in Sect. II.A are also shown as the dotted
curve in Fig. 21. Since the detuning was much larger than the splitting between
the hyperfine-structure levels of the excited state, the three-level interaction mode
was quite good for the simulation.
400-
350.
9 I
300
0 II
r
250
E
200 84 101 . . . . . . .
E
;:; 150
100 "6
50. 103 .......... . .
0 200 4O0 6OO 8OO 1000
time (rnsec)
u 9 i 9 i 9 9 i ' " ' 9 ! 9
0 5 10 ~'~ ~o ~'~ ~o 35
detuning (nm)
FIG. 22. Lifetime versus detuning. The inset shows a typical lifetime measurement for
6 = 5 nm (dots). The exponential fit (solid line) gives the lifetime of 340ms (from Ozeri e t a l . ,
1999, P h y s . Reu. A 59(3), R1750, Fig. 3, reprinted with permission).
coating should be d = ~,/[2(n- 1)] = 676.3 nm for ~, = 514.5 nm. The darkness
factor, defined as the ratio between the light intensity at the center of the trap
and the light intensity at the first surrounding ring, was measured to be 1/750.
A TEM00 Gaussian laser beam was magnified into a collimated Gaussian beam
with w0 = 6 mm, passed through the :r-phase plate, and was focused with a
f - 250-mm lens into the vacuum chamber.
Figure 22 shows the measured lifetime for various trapping beam wavelengths.
For detunings 6 > 0.5 nm the 1/e trap lifetime is nearly independent of 65 at
around 300ms and is inversely proportional to the background pressure in the
vacuum chamber. This indicates that the trap lifetime is governed by collisions
with background atoms. For 6 > 0.5 nm, the trap lifetime is approximately
proportional to 6. This is consistent with a heating-induced lifetime, since the
heating rate is proportional to 0 -2, whereas the trap depth is approximately
proportional to 6 -1. The peak density was measured to be 6.8• l0 II atoms/cm 3.
In a later experiment [85], they made a similar dipole trap with a much larger
volume and a more symmetric shape than before. They achieved this by
simultaneously exploiting two diffraction orders of a properly designed binary
phase element (BPE)[86], which was composed of concentric phase rings with
a phase difference of ;r between subsequent rings, thus creating a radial grating
with uniform spacing. Figure 23 depicts the 1st a n d - l s t diffraction orders from
the radial grating, each having a diffraction efficiency of 40.5%, which together
form an outgoing cone of light. When focused, the cone appears in the focal
plane as a narrow ring. The ring closes upon itself in both sides of the focal plane
owing to the beam divergence to form a dark region completely surrounded by
light.
Zem~nek and Foot [87] proposed a blue-detuned dipole trap by using two
IV] MANIPULATION OF COLD ATOMS IN HLBs 185
FIG.23. Generation of a dark, hollowoptical trap by a binary phase element (BPE). The 1st (grey)
and-lst (dashed) diffracted beams are focused and generate a dark region around the focal plane
(from Ozeri et al., 2000, J. Opt. Soc. Am. B 17(7), 1113, Fig. 1, reprinted with permission).
focal length of the second lens f l = 10.0 cm, and distance between the axicon
and the second lens d I = 93 cm. As a result, they observed a ring radius of
43 gm in the image plane, which is in qualitative agreement with the theoretical
prediction of 90 gm.
750"
@
9 o o
e' ~ 5O0 o
o
9 o
l
.z 250
o o 9 r=67p m
o o r=32~m
" O --
O
|~ , i 9 i 9 | "~ i , , , i 9 i 9
FIG. 24. Atomic lifetime in ROBOT as a function of the frequency of the trapping beam (from
Friedman et al., 2000, Phys. Rec. A 61(3), 031403, Fig. 2, reprinted with permission).
IV] MANIPULATION OF COLD ATOMS IN HLBs 187
400
300 "'.,.,
CO
E "~" .,..,"~" '~"..,
200 ."1 ss "I
O3 ,," 1 so
,r ." , 1.45 ~ ~.
E~4o
100
~ ."
1.35
1 .all
1.zs
1'2~ 5-1"0-1'5 2'0 2"5 3"o 35 4"0 45
' Idetunin~ (OHz I
lb
"IV B,
0 20 30 40 50
detuning (GHz)
Ff6. 25. Number of atoms captured by RODiO as a function of trap radius (from Rudy et al.,
2001, Opt. Exp. 8(2), 159, Fig. 3, reprinted with permission).
85Rb atoms using an extremely weak (25 gW) probe laser beam. The measured
transition rate was as small as 0.09 s-~. Note that the striking feature was the
long spin-relaxation times combined with tight confinement of the atoms in a
dark, hollow optical dipole trap.
Rudy et al. [93,94] demonstrated a Rotating Off-resonant Dipole Optical
(RODiO) trap, a similar all-optical dynamical dark trap. A circular scan of radius
1-5 mm was created by using two perpendicular linear scans phase-shifted by
90 ~ In this way, they created an average trap potential with a spatially averaged
height of ~< 240 gK. After the RODiO trap was loaded, it was left on for a
variable time duration, At. Figure 25 shows the atomic confinement at different
scan radii taken after 30 ms at A - 30 GHz. For small radii, the averaged potential
well was deep, but the trap beam cut into the initial trapped atoms, expelling
many atoms. As shown in the inset, the decay time is faster in this regime because
the interaction time with the light is significant. When the radius is increased,
since the interaction time as well as the time-averaged scattering force decrease,
the number of trapped atoms rises sharply.
They also examined the dependence of confinement time rRoDio on the scan
rate by implementing a two-dimensional RODiO at 2, 5 and 11 kHz scan rates.
For the 11-kHz case, they found rRODiO ~ 40ms at the optimum conditions
of A = 30GHz. At 5kHz, rRODiO ~ 13 ms and retention was observed
beyond 25 ms. At 2 kHz, rRODiO ~ 6 ms and finite retention was found well
beyond 10 ms. In particular, they discussed the merits of RODiO over other blue-
188 H.-R. Noh et al. [VI
detuned dipole traps, such as the flexibility with respect to the number of laser
beams, the realization of an arbitrarily sized dark region, and the completely dark
interior.
V. A c k n o w l e d g m e n t
The authors acknowledge the support of the Creative Research Initiatives of the
Korean Ministry of Science and Technology.
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A D V A N C E S IN A T O M I C , M O L E C U L A R , A N D O P T I C A L P H Y S I C S , VOL. 48
CONTINUOUS STERN-GERLACH
EFFECT ON ATOMIC IONS
G(J/NTHER WERTH l, H A R T M U T Hf4"FFNER l and WOLFGANG Q U I N T 2
l Johannes Gutenberg University, Department of Physics, 55099 Mainz, Germany,"
2Gesellschaft fiir Schwerionenforschung, 64291 Darmstadt, Germany
I. I n t r o d u c t i o n . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 191
II. A Single Ion in a P e n n i n g Trap . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 195
III. C o n t i n u o u s S t e r n - G e r l a c h Effect ................................. 206
IV. D o u b l e - T r a p Technique . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 209
V. C o r r e c t i o n s and S y s t e m a t i c Line Shifts ............................. 212
VI. C o n c l u s i o n s . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 213
VII. O u t l o o k . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 214
VIII. A c k n o w l e d g e m e n t s . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 216
IX. R e f e r e n c e s ................................................ 216
I. I n t r o d u c t i o n
= gskts, (1)
--~,1017
10TM
,,,,"."'.".'".'".""'.". . . . . . . . . . . . . . . . . . . .
W"1012101310141015
1011 /
10lo
109
10 20 30 40 50 60 70 80 90
nuclearchargeZ
Fie. 1. Calculated expectation values for the electric field strength for hydrogen-like ions of
different nuclear charge Z. (Courtesy Thomas Beier.)
gBreit = (5)
20 40 60 80 100
10 0 100
10 -1 10 -1
o 10 .3 10 .3
9;'~ AgBsQED 1. order in ot 9 . ~" 9
' 104 : /. 9
9 )r
10 -4
~o )r
o
.~ 10 -s )r 10 -~
hue.
+ + + +
0 10 .6 + 10 .6
10 .7 +
+~ AgBs QF.D2. order in a (estimate~ 10 .7
E
o
tJ
lO-S
10 .9
10-1o
+
+
Y 10 ~
10 .9
10-1o
+
1 0 -11 10-~1
I , I , I , I , I
0 20 40 60 80 100
nuclear charge Z
FIG. 2. Contributions to the g-factor of a bound electron in hydrogen-like ions for different nuclear
charges Z. (Courtesy Thomas Beier.)
Table I
Theoretical contributions to the g-factor in 12C5+
of the Dirac equation and deviates from the value g = 2 for the free electron
(Breit, 1928). The next-largest part is the well-known QED contribution for the
free electron (Hughes and Kinoshita, 1999). The bound-state contributions of
order a (calculated to all orders in Z a) are given with error bars which represent
the numerical uncertainty of the calculations. The quoted uncertainty of the
aZ(za) 2 term is an estimate of the contribution from non-calculated higher-
order terms. Finally, nuclear recoil contributions have been calculated to lowest
order in Z a by Grotch (1970b), Faustov (1970) and Close and Osborn (1971).
Recently, Shabaev (2001) presented formulas for a non-perturbative calculation
(in Za), and Yelkovsky (2001) presented further numerical results. The nuclear-
shape correction was considered numerically by Beier et al. (2000), and recently
(for low Z) also analytically by Glazov and Shabaev (2001). The sum of the
different contributions leads to a theoretical value for the g-factor in hydrogen-
like carbon of
gtheor(12C5+) = 2.001 041 590 1 (3). (6)
FIc. 3. Sketch of the electrode structure and potential distribution of the double trap.
Uo ~ (~); (7)
(~)( r , I.~q) : -~- Z Ci -~ Pi(COS L~),
i=0
Uo z 2 - r2/2
,I, - (8)
2 d2
We optimize the trap by changing the voltages on the correction electrodes until
the ion oscillation frequency is independent of the ion's oscillation amplitude
as characteristic for a harmonic oscillator. With this method we can reduce the
II] CONTINUOUS STERN-GERLACH EFFECT ON ATOMIC IONS 197
axial
motion
magnetron
m
T-B
cyclotron
motion
FIG. 4. Ion oscillation in a Penning trap.
dominant high-order term C4, the octupole contribution, to less than 10-5. The
ion's frequency in the harmonic approximation is then given by
qUo
O)z = Md 2 . (9)
o)~ = q B (10)
M
of a free particle with charge q and mass M because of the presence of the
electric trapping field, and is given by
where (-/)mis the magnetron frequency, a slow drift of the cyclotron orbit around
the trap center, given by
For calibration of the magnetic field we use the cyclotron frequency of the
trapped ion. It can be derived either from Eq. (12) or more reliably from the
relation
since this equation is independent of trap misalignments to first order (Brown and
Gabrielse, 1986). In this case the measurement of the magnetron frequency (_gm
is required in addition to a measurement of to~ and COz.
The traps are enclosed in a vacuum chamber placed at the bottom of a helium
cryostat at a temperature of 4 K and located at the center of a superconducting
NMR solenoid. The helium cryostat provides efficient cryopumping. As an upper
limit we estimate the vacuum in the container to be below 10 -16 mbar. The
estimation was derived from the measurements on a cloud of highly charged
ions, whose storage time would be limited by charge exchange in collisions with
neutral background particles. We observed no ion loss in a cloud of 30 hydrogen-
like carbon ions stored for 4 weeks. Together with the known cross section for
charge exchange with helium as the most likely background gas at 4 K we obtain
an upper limit of 10 -16 mbar for the background gas pressure. The magnetic
field of the superconducting magnet is chosen to be 3.8 T. At this field strength
the precession frequency of the electron spin is 104 GHz. Microwave sources of
sufficient power and spectral purity are commercially available at this frequency.
We load the trap by bombarding a carbon-covered surface with electrons. This
process releases ions and neutrals of the element under investigation as well as
of other elements present on the surface. Higher charge states are obtained by
consecutive ionisation by the electron beam. We detect the ions by picking up
the current induced by the ion motions in the trap electrodes. For this purpose
superconducting resonant circuits and amplifiers are attached to the electrodes.
Upon sweeping the voltage of the trap, and thus the ions' axial frequencies, the
ions get in resonance with the circuit and their signal is detected. Figure 5 shows
such a spectrum, where we identified different elements and charge states. We
eliminate unwanted ion species by exciting their axial oscillation amplitude with
an rf field until the ions are driven out of the trap.
Ions of the same species have different perturbed cyclotron frequencies in
the slightly inhomogeneous magnetic field of the precision trap, because they
have different orbits. Therefore, for small ion numbers, single ions can be
distinguished by their different cyclotron frequencies. Figure 6 shows a Fourier
transform of the induced current from 6 stored ions. We excite the ions' cyclotron
motion individually and thus eliminate them from the trap until a single ion is
left. Typical cyclotron energies for signals as shown in Fig. 6 are of the order of
several eV.
In order to reduce the ion's kinetic energy we use the method of "resistive
cooling" which was first applied by Dehmelt and collaborators (Wineland and
Dehmelt, 1975; Dehmelt 1986). The ion's oscillation is brought into resonance
II] CONTINUOUS S T E R N - G E R L A C H EFFECT ON ATOMIC IONS 199
= 0,3
"~ 0,2
0,0 l : I , I , I , I , I , I , I ,
"~ 0,2
r
,w
~ o,1
0,0_ 14
trapping potential [Volt]
FIG. 5. Mass spectrum of trapped ions after electron bombardment of a carbon surface showing
different charge states of carbon ions as well as impurity ions (a) before and (b) after removal of
unwanted species.
with the circuits attached to the electrodes. The induced current through the
impedance of the circuit leads to heating of the resonance circuit, and the ion's
kinetic energy is dissipated to the surrounding liquid helium bath (Fig. 7). This
leads to an exponentially decreasing energy with a time constant r given by
q2
r -1 - R, (15)
Md 2
where R is the resonance impedance of the circuit.
For the axial motion we use superconducting high-quality circuits (Q = 1000 at
1 MHz in the precision trap and Q = 2500 at 365 kHz in the analysis trap).
With the resonance impedances of R = 23 M ~ (analysis trap) and 10 Mr2
(precision trap) the cooling time constants are 8 0 m s and 235 ms, respectively.
For cooling the cyclotron motion we employ a normal-conducting circuit at
24 MHz (Q = 400) with a resonance impedance of 80 kf~. Here we reach cooling
time constants of a few minutes. Figure 8 shows the exponential decrease of the
induced currents from the ion oscillations as the result of axial cooling.
200 G. Werth et al. [II
.~ 30
"f~ 25
6 C 5+ions I
~ o
, i
J , I , I ~ I
| Superc0nductang
l Cryogenic
Ion trap GaAsamphfier
I
FIG. 7. Principle of resistive cooling.
t--
~
ms
t',-
T =4 K ~~,..,__....~
_
yields that the quantum numbers tend to equalize. This leads to the expectation
value (Em) for the magnetron energy,
_ 1 (-Om (16)
o)m h ooz ( <kz ) -k- ~ ) = --~z ( Ez ) .
r
The axial oscillation is continuously kept in equilibrium with the cooling circuit
and we thus reduce the magnetron orbit to about 10 ~tm.
The mean kinetic energy of a single ion is often expressed in terms of
temperature. This is justified by the statistical equilibrium of the ion and the
resonant circuit. The statistical motion of the electrons in the resonance circuit
causes Johnson noise in the trap-electrode voltages, which in turn leads to
varying energies of the ion as a function of time (Fig. 9). Extracting a histogram
of the cyclotron energies results in a Boltzmann distribution (Fig. 10) with a
temperature of 4.9 K close to the temperature of the environment. Calculating
the temporal autocorrelation function of the energy gives, as expected, an
exponential (Fig. 11) with a time constant well in agreement with the measured
cooling time constant.
In order to calibrate the magnetic field at the ion's position with high precision
from Eq. (14) the three oscillation frequencies have to be measured. Because
of their different orders of magnitude (~Oc~/2;r = 24 MHz, Ogz/2:r = 1 MHz,
O)m/2~ 18 kHz) the required precision is different, o~ is determined from the
=
FIG. 9. Noise power of the induced voltage in a trap electrode from the cyclotron oscillation of
a single trapped ion while its frequency is continuously kept in resonance with an attached tank
circuit.
FIG. 10. Histogram of the probabilities for cyclotron energies. The curve can be well fitted to a
Boltzmann distribution, giving a temperature of 4.9(1) K.
II] CONTINUOUS STERN-GERLACH EFFECT ON ATOMIC IONS 203
%,
%,
%, C(t) = C o exp(-th:)
%,
%,
%,
".%
-c = 5.40 + 0.07 min
%,
%
"~,
-%
%
,~,
%
4
%.
".,,
%. e.
1~0
I ' I ' [ ' ' I '
0 2 4 15 8
Time [min]
FIG. 11. The time-correlation function of the noise in fig. 10 shows an exponential decrease. The
time constant o f 5 . 4 0 ( 7 ) m i n corresponds to the time constant for resistive cooling of the cyclotron
motion.
~
.,... 30
~ 25
2O
.,,..
~ lO
5
0
-- ' i 7 - - - 1 - , - - - ~ . . . . . . -w--- - T - - - "T~ ...... 1 i 1
FIG. 12. High-resolution Fourier transform of the induced noise at the perturbed cyclotron
frequency. A Lorentzian fit gives a fractional width o f 1.4>< 10 -9.
magnetic field this changes the mean field strength along the cyclotron orbit.
This has to be considered in the final evaluation of the measurements.
The axial frequency OJz is determined while the ion is in thermal equilibrium
with the resonance circuit. At a given temperature the thermal noise voltage in
the impedance Z(e)) of the axial circuit, given by
excites the ion motion within the frequency range 6v of the ion's axial resonance.
This motion in turn induces a voltage in the endcap electrodes, however at a
phase difference of 180 ~ as can been shown by modeling the system as a driven
harmonic oscillator. Consequently the sum of the thermal noise voltage and
204 G. Werth et al. [II
FIG. 13. Axial resonance of a single trapped C5+ ion. The noise voltage across a tank circuit
shows a minimum at the ion's oscillation frequency.
FIG. 14. High-resolution Fourier transform of the axial noise near the center of the resonance
frequency of the axial detection circuit.
the induced voltage leads to a reduced total power around the axial frequency
of the ion. This appears as a m i n i m u m in the Fourier transform of the axial
noise as shown in Fig. 13. A spectrum with a resolution of 1 0 m H z (Fig. 14)
shows that the center frequency can be determined to about 24 mHz. A different
approach to explain the appearance of a m i n i m u m in the axial noise spectrum
was taken by Wineland and Dehmelt (1975) considering the equivalent electric
circuit of an oscillating ion in the trap. The magnetron frequency tOm is
measured by sideband coupling to the axial motion. If the ion is excited at
the difference between the axial and magnetron frequencies, the ion's axial
II] CONTINUOUS STERN-GERLACH EFFECT ON ATOMIC IONS 205
A6Oct-
tO,c C4~ 1 (~cc)2[-3Ez + -~3 (~cc)2Ec - 6Era] (19)
Ez, Ee and Em are the energies in the axial, cyclotron and magnetron degrees
of freedom. The tuning of the trap potential results in a coefficient C4
as small as 10-5 . For the energies of the motions in thermal equilibrium the
corresponding frequency shifts are below 10-l~ and need not be considered here.
The coefficient C6 of the dodekapole contribution to the trapping potential has
been calculated to an accuracy of 10-3 for our trap geometry. The frequency
shifts arising from this perturbation scale with (E/qUo) 2 and are negligible here.
The residual inhomogeneity of the magnetic field in the precision trap arising
from the nickel ring electrode in the analysis trap 2.7 cm away changes the value
of the oscillation frequencies of an ion with finite kinetic energy as compared
to the ion at rest. A series expansion of the B-field in axial direction,
Am~_ 1 B2 1
mtO2z Bo hoOc
- ~ Ec+Ez+2E~j (22)
ACOz 1 B2 1
[Ee -Em], (23)
~Oz mm2z Bo hoe
Ao)m 1 B2 1
[2Ec - Ez - 2Era]. (24)
(Dm mm 2 Bo hmc
The g-factor of the bound electron as defined by Eq. (1) can be determined by
a measurement of the energy difference between the two spin directions in a
magnetic field B:
A E = hVL = g ~ s B , (25)
The nickel ring in the analysis trap creates a bottle-like magnetic field distortion
which can be described in first approximation by
The odd terms vanish in the expansion because of mirror symmetry of the field.
The corresponding force on the magnetic moment in axial direction is
F= = - 2 1 z z B 2 z , (28)
which is linear in the axial coordinate. It adds to the electric force from the
quadrupole trapping field acting on the particle's charge. Since both forces are
linear in the axial coordinate the ion motion is still described by a harmonic
oscillator (Fig. 15). The axial frequency, however, depends on the direction of
the magnetic moment/t with respect to the magnetic field:
ltzB2
~ 6COz = % 0 + 9 (29)
% = %0 + ~ M (OzO
The value of B2 in our set-up was calculated using the known geometry and
magnetic susceptibility of the nickel ring electrode. We also determined it
III] C O N T I N U O U S S T E R N - G E R L A C H E F F E C T ON ATOMIC IONS 207
z-a~s
FIo. 15. Axial parabola potential for an ion in a quadrupole trap including the magnetic potential
for the spin-magnetic moment in a bottle-like magnetic field. The strength of the potential depends
on the spin direction. Upper curve: spin down; lower curve: spin up.
spin up
,~ ~ J , ---- ~---0.7Hz , r
, ,
i
i
_.
-10 ,
-5 ~ ,
0
I '
5
r , 1~0
FIG. 16. Axial frequencies of a single C5+ ion for different spin directions. The averaging time
for each resonance line was 1 min.
)" 1,0
quantum jumps
i u~
down
oo
~ -1,o~
FI6. 17. Center of the axial frequency for a single C 5+ ion when irradiated continuously with
microwaves at the Larmor precession frequency showing two distinct values which correspond to
the two spin directions of the bound electron.
3O
E
E 20
2~
~L_
lO
E
m m m m
m m m m
I I I I I
-5 0 5 10 15
Larmor precession frequency- 103 958 [MHz]
FIG. 18. Number of observed spin flips per unit time vs. the frequency of the inducing field. The
solid line is a fit according to Eq. (29).
by Brown (1985) as a complex function of the trap parameters, the ion's energy
and the field inhomogeneity. However, assuming that the ion's amplitude z(t) is
IV] CONTINUOUS STERN-GERLACH EFFECT ON ATOMIC IONS 209
constant during the time 1/AwL, the line profile is given by a 6-function averaged
over the Boltzmann distribution of the energy:
Z ( ~~ ) =
io (
dE 6 ~oL - O)Lo
( '"))".-""
1 + m---~z
(30)
-- O(O)L
{ A--O09LO)
) L exp - (-OL--O')LO}Ao)L"
Here O(~oL - coL0) is the step function, which is 0 for o)L < coL0 and 1 for col > cot0,
and e is a linewidth parameter so that the Larmor frequency depends as
ooL = ~Oo(1 + ez 2) on the axial coordinate. A least-squares fit of this function
to the data points of Fig. 18 yields the Larmor frequency with a relative
uncertainty of 10-6 (Hermanspahn et al., 2000). This is sufficient to measure
the binding correction to the g-factor in C 5+. The bound-state QED corrections
for C 5+, however, are 4 • 10-7 and were not observed in this measurement.
0,2
~" 0,0
~ 0,4
-0,2
(D :' ~.~
", ,' =I 0,2
: :' ~r ~
o -0,4 ',, :,
, % 0,0 -
)$
..~
-0,6
-0,2
-0,8
i i i I i I I i i 1 i i 1 1 i
0 1 2 3 4 5 6 7 0 l 2 3 4 5 6 7
m i c r o w a v e excitations m i c r o w a v e excitations
FIG. 19. D e t e r m i n a t i o n o f the spin direction in the analysis trap after transport from the precision
trap. A change in axial frequency o f about 0.7 Hz indicates that the spin was up (left) or d o w n (right)
when the ion left the precision trap.
we induce an additional spin flip in the analysis trap to determine without doubt
the spin direction after return to the analysis trap. Figure 19 shows several cycles
for a spin analysis. The total time for a complete cycle is about 30 min.
While the ion is in the precision trap its cyclotron frequency COc = ( q / M ) B
is measured simultaneously with the interaction with the microwaves. This
ensures that the magnetic field is calibrated at the same time as the possible
spin flip is induced. The field of a superconducting solenoid fluctuates at the
level of 10-8-10 -9 on the time scale of several minutes. Figure 20 shows a
measurement of the cyclotron frequency of the ion in the precision trap over
a time span of several hours. Every 2 min the center frequency of the cyclotron
resonance was determined. The change in cyclotron frequency has approximately
a Gaussian distribution with a full-width-at-half-maximum of 1.2x 10 -8. This
may impose a serious limit on the precision of measurements as in the case of
high-precision mass spectrometry using Penning traps (Van Dyck et al., 1993;
Natarajan et al., 1993). However, the simultaneous measurement of cyclotron and
Larmor frequencies eliminates most of this broadening. Using Eqs. (10) and (25)
we obtain the g-factor as the ratio of the two measured frequencies
(DL m
g=2~--. (31)
mc M
The mass ratio of the electron to the ion can be taken from the literature. In our
case of 12C5+, Van Dyck and coworkers (Farnham et al., 1995) measured it with
high accuracy using a Penning trap mass spectrometer.
We measure the induced spin flip rate for a given frequency ratio of the
microwave field and the simultaneously measured cyclotron frequency. When we
IV] CONTINUOUS STERN-GERLACH EFFECT ON ATOMIC IONS 211
80-
7O
6O
e--
-I~ 50
.~.
._~ 4o
v/v = 1.2. 10-8I
30
Q.
20
10
FIG. 20. Distribution of magnetic field values measured by the cyclotron frequency of a trapped
ion in a period of several hours. Data were taken every 2 min. The distribution is fitted by a Gaussian
with a full width of 1.2 x 10-8.
35
,-, 3O
~>' 25
.m
-0
.0 20
o
r
i,..
15
.m
.~ 10
Wmw/We - 4 3 7 6 . 2 1 0 499
Fie. 21. Measured spin-flip probability vs. ratio of Larmor and cyclotron frequencies. The data
are least-squares fitted to a Gaussian.
plot the spin flip probability, i.e. the n u m b e r o f successful at t empt s to c h a n g e the
spin direction d i v i d e d by the total n u m b e r o f attempts, we obtain a r e s o n a n c e line
as s h o w n in Fig. 21. The m a x i m u m attainable p r o b a b i l i t y is 50% w h e n the
a m p l i t u d e o f the m i c r o w a v e field is high e n o u g h . To avoid those saturation effects
we take care to k e e p the a m p l i t u d e o f the m i c r o w a v e field at a level that the
m a x i m u m p r o b a b i l i t y for a spin flip at r e s o n a n c e f r e q u e n c y is b e l o w 30%. In
addition we can take saturation into a c c o u n t using a s i m p l e r a t e - e q u a t i o n m o d e l .
212 G. Werth et al. [V
0',
-10-
0
c-q -20-
t~
~" -30-
-40-
2 4 6 8 10 1 14 16
Table II
Systematic uncertainties (in relative units) in the g-factor determination of 12C5+
From the residual imperfection of the electric trapping field (C4 - l0 -5) we
calculate a shift of the cyclotron frequency of 1 x 10 -10. O f the same order of
magnitude are frequency shifts caused by changes of the trapping potential due
to ground loops when the computer controls are activated. The interaction of
the ion with its image charges changes the frequencies by 3 x 10-1~ but can be
calculated with an accuracy of 10%. Relativistic shifts are of the order of 10-l~ at
typical ion energies, but do not contribute to the uncertainty at the extrapolation
to zero energy. A list of uncertainties of these corrections is given in Table II.
The quadrature sum of all systematic uncertainties amounts to 3x 10-~~ The
final experimental value for the frequency ratio WL/OOCin 12C5+ is
COL
- 4376.2104989(19)(13). (32)
O9C
The first number in parentheses is the statistical uncertainty from the extrap-
olation to vanishing cyclotron energy, the second is the quadrature sum of the
systematical uncertainties. Taking the value for the electron mass in atomic units
(M(12C) = 12) from the most recent CODATA compilation (Mohr and Taylor,
1999) we arrive at a g-factor for the bound electron in 12C5+ of
Here the first number in parentheses is the total uncertainty of our experiment,
and the second reflects the uncertainty in the electron mass.
VI. Conclusions
This is in agreement with the CODATA electron mass (Mohr and Taylor, 1999)
based on a direct determination by the comparison of its cyclotron frequency to
that of a carbon ion in a Penning trap (Farnham et al., 1995):
VII. Outlook
2,8
2,4
2,o
rn--,I
t'q
1,6
N
<3
1,2
0,8
0,4
4He + 12C5+ 1607+ 9 9 9 9
t
9 9 n uu 9
o,o , t, ,t ,
; 8 ,'2 ' ,'6 2'0 ' 2'4 ' 2'8
(q * m)'/2
FIG. 23. Difference in axial frequency for two spin directions in a bottle-like magnetic field for
various hydrogen-like ions. The parameters B0 = 3.8T, B2 = I T/cm2, and tOz/2ar = 365kHz
are those of our experiment. The frequency difference scales linear with the magnetic field
inhomogeneity B2.
frequency difference for the two spin states significantly. This would also have
the advantage that it reduces the amount of ferromagnetic material placed in the
analysis trap, and so helps to improve the homogeneity in the precision trap. To
further improve the homogeneity in the precision trap the distance between the
two traps can be increased. Finally, shim coils may be used to make the field
in the precision trap more homogeneous. We believe that we can maintain the
presently achieved precision with other ions as well, and hope to even increase
it when we apply some of the measures for improvement. This would result in a
more significant test of higher-order bound-state QED contributions since they
increase quadratically with the nuclear charge (see Fig. 2).
The method can also be applied to more complicated systems: a measurement
of the electronic g-factor in lithium-like ions would test not only the QED cor-
rections in these systems but also correlation effects with the remaining electrons
which change the g-factor significantly. When applied to hydrogen-like ions with
non-zero nuclear spin the transition frequencies between spin states depend on
the nuclear magnetic moment. Measuring the different transition frequencies
yields the magnetic moment of the nucleus. This would be of special interest,
because all nuclear magnetic moments so far have been determined using neutral
atoms or singly ionized ions. The effective magnetic field seen by the nucleus in
these systems differs from the applied magnetic field by shielding effects of the
electron cloud. In a measurement on hydrogen-like ions this shielding is strongly
216 G. Werth et al. [IX
reduced, and comparison with data obtained on neutral systems would, for the
first time, test atomic-physics calculations on electron shielding.
VIII. Acknowledgements
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A D V A N C E S IN ATOMIC, M O L E C U L A R , A N D O P T I C A L PHYSICS, VOL. 48
I. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 219
II. Fundamental Nature of Chirality . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 219
III. True and False Chirality . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 230
IV. Galaxies, Plants, and Pharmaceuticals . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 233
V. Plausible Origins of Homochirality . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 236
VI. A s y m m e t r y in Beta Radiolysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 243
A. Amplification and Degradation M e c h a n i s m s . . . . . . . . . . . . . . . . . . . . . . . 247
VII. Possible Effects of the Parity-Violating Energy Difference (PVED) in
Extended Molecular Systems . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 252
VIII. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 257
IX. Acknowledgment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 257
X. References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 258
I. Introduction
It is often said that the feature that distinguishes the physical sciences from the
biological sciences is the precision with which the terms and concepts in each
field are defined and measured. Terms in the physical sciences are precisely
defined while those in the biological sciences are often much less so. Even the
definition of life, which is the sine qua non of biology, is difficult to pin down in
all cases. Is a virus or a prion living, for example? Nonetheless, there are features
that all living things have in common. Most of the molecules that serve structural
and functional roles in all living systems exist in only one of two seemingly
identical forms. This property is called homochirality, and the molecules that
possess it are said to be optically active. This chapter will investigate the present
state of understanding of how homochirality in living systems may have come
to be on the earth. We refer to the fact that overwhelmingly only one of these
identical forms is found in life. Before doing this, however, it will be necessary to
find out what homochirality means and what are the properties of the molecules
that potentially posses it.
A more detailed discussion may be found in the excellent book on the subject
by Eliel et al. (1994).
The English word chirality is derived from the Greek word Zetp (kheir)
meaning hand, and refers to an interesting geometrical property of left and right
hands (and feet) and other three-dimensional objects. Neither the left nor the
right hand has any internal symmetry but both are related to each other via a
mirror plane. If you take your left hand and reflect it into a mirror, what you
see in the mirror is an image of your right hand (Fig. 1). Likewise, reflection
of your right hand into the mirror also yields an image of your left hand. All
objects (except vampires) have a mirror image. In most cases, such as with
spheres (balls) and planes (pieces of papers), the mirror image is superposable
or congruent with the original object. This means that the mirror image object
is identical in every respect (constituents and geometry) to the original. What
makes the relationship of the left and right hands different is the fact that they
cannot be superposed one on top of the other even though the connectivities of
the fingers to the palms are the same in both cases. No matter how hard one
tries to attain the superposition, there will always be mismatches. The left and
right h a n d s - and any other objects with non-superposable mirror i m a g e s - are
said to be chiral.
There are myriad objects in the physical world that are chiral. Coils, screws
and springs exist in chiral forms (right- and left-handed helices), for example.
Perhaps the most well-known of these is the alpha (right-handed) helix of DNA.
II] THE CHIRALITY OF BIOMOLECULES 221
H H
H\ .... H
CH4 HmC--H
H / C "~H
I
H
On a larger scale, vines coil up (twine) trees and shrubs in one of the two
mirror image forms whose direction of coiling (helicity) is species dependent.
When only one of the two mirror image forms exists, the system is said to be
homochiral. Homochirality at all size scales is a hallmark of biology. Many
seashells also coil in only one direction, with the direction of coiling being
species dependent. Spiral staircases are chiral as well. The massless photon with
a unit spin and moving in a straight line at the speed of light carries a spin
angular momentum (+h). Thus, a single photon can be thought of as "right-" or
"left-" handed. Linearly polarized light is an equal mixture (racemic) mixture of
these photons. Electrons also have one-half integer spin, but at rest the electron
and its mirror image are superposable. When electrons are in motion, their
mirror images are not superposable, thus yielding spin-polarized particles if the
z component of the spin angular momentum can be along or against the direction
of propagation of the electron. Thus, for elementary particles such as photons
and electrons, it is the combination of spin and translation that is responsible for
their chirality (physicists speak of helicity) and circular polarization.
Many molecules, including biological ones, are chiral. To see how this is possi-
ble, consider first the structure and properties of the simplest organic molecule,
methane (CH4) (Fig. 2). This molecule consists of a central carbon atom (C)
connected or bonded to four hydrogen atoms (H). Each bond connecting a carbon
atom to a hydrogen atom is represented by a straight line. When a carbon atom
is bonded to four other atoms, it exists in a tetrahedral environment in which the
carbon resides in the center of an imaginary Platonic tetrahedron and the four hy-
drogen atoms reside at apices of the tetrahedron. This yields a three-dimensional
structure with four identical carbon-hydrogen bond lengths and six identical
hydrogen to carbon to hydrogen bond angles, in agreement with experiment.
Rather than draw a cumbersome tetrahedron every time a structure contains a
tetrahedral carbon atom, it is convenient to draw it in a different, simplified
manner: In this picture of methane two straight lines from C to H represent bonds
in the plane of the paper, while a solid triangle represents a carbon-hydrogen
bond projecting from the paper, where the carbon resides, to the hydrogen in front
of the paper and a dashed triangle represents a C - H bond projecting behind the
paper. Methane is thus a highly symmetric molecule with Td symmetry. It should
222 R.N. Compton and R.M. Pagni [II
i _ i / c "~H H~'~C ~ H
H H H H
I I I I
HmC ~H ~ H~G ~F H--CmF ~ Br--CmF
I / I I
H H CI C1
CHIRAL
be noted, however, that the picture of methane with Ta symmetry represents the
time-averaged or equilibrium structure. As the bonds in molecules are constantly
vibrating, an instantaneous picture of methane would be of lower symmetry.
Now consider methane as was done above for left and right hands, i.e., reflect
the image of methane into a mirror (Fig. 3). It is not difficult to see, either in
one's mind or with models, that the mirror image object is superposed exactly
on the original methane molecule. Methane thus lacks chirality and is said to be
achiral.
What happens when one of the hydrogen atoms in methane is replaced with a
different atom (or a group of atoms)? Consider fluoromethane, CH3F, where the
replacement is a fluorine atom (Fig. 4). This molecule also contains a tetrahedron
carbon atom at its center but with C3~ symmetry has lower symmetry than
methane. Nonetheless, CH3F and its mirror image are superposable on one
another and the molecule is achiral. Likewise, when a second atom is replaced
with a still different atom (or a group of atoms), an achiral molecule results. For
example, chlorofluoromethane (CHzC1F), where the second replacement is with
a chlorine atom (C1), is also achiral.
When a third replacement is made with a still different substituent, a chiral
molecule is formed. Bromochlorofluoromethane, CHBrC1F, where the third
substituent is a bromine atom (Br), is a fascinating example of such a molecule
(Fig. 5). Here the mirror image molecule cannot be superposed on the original.
It is always possible to match up the carbon and two of its attached atoms (and
their bonds) in the two structures, but the other two attached atoms (and their
bonds) will always be out of alignment. Thus CHBrC1F is chiral.
II] THE CHIRALITY OF BIOMOLECULES 223
H\ F/,..... / H
J C -,.~ICI CIw~'" C ~ B r
Br~
It is worth noting that the achiral CH4, CH3F and CH2FC1 all have one or more
planes of symmetry while the chiral CHBrC1F does not. It can be shown that
all achiral molecules have at least one improper axis of symmetry Sn, defined
as rotation by 2sr/n radians followed by reflection in a plane perpendicular to
the rotation axis. A plane of symmetry is thus equivalent to S I and a center of
symmetry is equivalent to $2.
The two forms of CHBrC1F are stereoisomers of one another, i.e., they have
the same connectivities of atoms and yet the very same atoms are oriented
differently in space. The carbon atoms in the stereoisomers of CHBrC1F are
called stereogenic centers. Stereoisomers such as the two forms of CHBrC1F
that are also mirror images of one another are called enantiomers. Interestingly,
enantiomers have identical chemical properties except when they react with other
molecules which are also enantiomeric; reaction or interaction with chiral forces
may also yield a difference in behavior. Enantiomers also have identical physical
properties except in the way they interact with plane-polarized or circularly
polarized light or other chiral objects. From this observation it would appear to
be difficult to separate, i.e., resolve, mixtures of enantiomers into their individual
forms. Fortunately, as described below, there are methods to accomplish this
task.
If one has samples of each pure enantiomer, one enantiomer would rotate
the plane of monochromatic plane-polarized light a given number of degrees
in the clockwise direction while the other enantiomer would rotate the light
the same number of degrees but in the counterclockwise direction. The device
in which these measurements are made is called a polarimeter. Molecules that
rotate plane-polarized light are said to be optically active, and the wavelength
dependence of the optical activity is called optical rotary dispersion (ORD).
A collection of achiral molecules does not rotate light and is thus said to be
optically inactive. An individual achiral molecule can also rotate the plane of
polarization, but the rotation averaged over many non-oriented molecules goes
to zero. A 1:1 mixture of two enantiomers, which is called a racemic mixture,
also is optically inactive because the rotation of one enantiomer is canceled by
224 R.N. Compton and R.M. Pagni [II
the opposite rotation of the other enantiomer. The enatiomeric excess is defined
as the difference in amounts of the two enantiomers in a sample divided by their
sum times 100. A pure enantiomer will have an enatiomeric excess of 100% and
is thus homochiral; a racemic mixture will have an enantiomeric excess of 0%.
Enantiomeric excess is often abbreviated as ee.
CHBrC1F is prepared in racemic form by the reaction of achiral CHBrzC1 with
achiral HgF2 (Hine et al., 1956):
Generally speaking when achiral or racemic compounds react with one another,
the resulting chiral products will be racemic. Only when a r e a g e n t - or
c a t a l y s t - is optically active will a chiral product be optically active as well.
Chiral forces such as circularly polarized light may also induce optical activity
(enantiomeric excess) in the product as well. Chiral reagents, chiral catalysts
or chiral forces are required to bring about enantiomeric excess in reaction
products. Thus, at first glance it is difficult to see how optically active biological
compounds such as amino acids and carbohydrates came to be on the earth
when they resulted in the first place from the chemical combination of achiral
molecules.
CHBrC1F can be prepared in optically active or resolved form in two ways:
(1) by the reaction of a precursor that is already optically active (Doyle and
Vogl, 1989) and (2) by the reaction of a chiral but optically inactive precursor
in a chiral, optically active environment (Wilen et al., 1985). It always takes an
optically active molecule or chiral force to produce a product that is optically
active.
There is nothing unique about CHBrC1E Any molecule containing a tetrahe-
dral carbon or other central atom such as silicon (Si) bonded to four different
substituents, regardless of their nature, will exist in enatiomeric forms. Thus the
property of chirality, which is manifested in chemical compounds, is in reality
geometric in nature. Many other geometric orientations of molecules in space
also yield enantiomeric forms.
CHBrC1F (and like molecules) has permanent chirality because its stereogenic,
tetrahedral carbon atom is attached to four different substituents. The innate
chirality of CHBrC1F does not depend on the lengths of its four bonds or
the fact that the lengths are constantly changing due to molecular vibrations.
CH4, on the other hand, behaves differently. It is achiral because its averaged
equilibrium structure of Td symmetry possesses six planes of symmetry and
six $4 axes of symmetry as well. Because it is vibrating, any instantaneous
structure of CH4 lacks Td symmetry and may be chiral if all four bond lengths are
different. In another moment this chiral structure will disappear and be replaced
by another, perhaps with a mirror-image relationship to the first. This constantly
shifting chirality will disappear when averaged through an ensemble of methane
II] THE CHIRALITY OF BIOMOLECULES 225
molecules, thus yielding a net optical rotation of zero degrees. Even crystals and
liquids made up of achiral molecules may display instantaneous chirality which
averages to zero.
Monochromatic, linearly polarized light (LPL) may be viewed as a su-
perposition of left-handed and right-handed circularly polarized light (CPL)
(Michl and Thulstrup, 1986). Alternately, one could describe LPL as a racemic
mixture of photons with spin angular momentum oriented along and against the
direction of propagation. When LPL passes through a sample of enantiomers,
one circular component of the light passes through the medium faster than the
other component because the real parts of the refractive indices, nL and ne,
of the left-handed and right-handed CPL through the molecule are different
(Atkins, 1978). This is the origin of optical activity. The angle of rotation
is equal to ( n L - nR)Jrl/~,, where l is the length of the sample and Jl is the
wavelength of the light. If the rotation of the plane of polarization is clockwise
as seen by an observer looking at the source of light, this is designated in
two ways: (1) with a + sign or (2) with a lower case "d" which stands for
dextrorotatory. Counterclockwise rotation is designated with a - sign or with
a lower case 'T' which stands for levorotatory. One enantiomer of CHBrC1F
will thus be (+)-CHBrC1F and the other (-)-CHBrC1F or d-CHBrC1F and
1-CHBrC1E Unfortunately, there is no simple method to relate the direction of
the optical rotation that the ensemble of enantiomers generates with the absolute
configuration of the enantiomer. Absolute configuration is the property of the
enantiomer that distinguishes the orientation of its substituents in space from
that of its mirror image partner.
Amino acids are the building blocks of peptides, proteins and enzymes which
serve an extraordinary number of structural and catalytic roles in cells. Enzymes,
for example, are the biological agents that catalyze virtually all cellular reactions,
most often with amazing speed and selectivity. Structurally, an amino acid that
is used biologically consists of an amino group NH2, consisting of a nitrogen
atom N bonded to two hydrogen atoms, and a carboxylic acid group COOH,
consisting of a carbon atom b o n d e d - actually double-bonded- to one oxygen
atom O and a hydroxyl group OH, and to a central CHR group, where R varies
in structure. As there are 20 amino acids commonly used in cellular chemistry,
there are 20 different R groups. All of the amino acids except glycine with R = H
contain a stereogenic center at the CHR carbon atom. Two of the amino acids,
isoleucine and threonine, contain a second stereogenic center in the R group
itself.
H
I H2N~CHR~COOH
H2N~ l ~COOH
R
AMINO ACID
226 R.N. Compton and R.M. Pagni [II
..... //COOH
H l, HOOC ....,,\H
CH3W~"C ~ H2N/C "~CH3
NH2
one enantiomer of alanine other enantiomer of alanine
I rotate rotate
structure structure
COOH COOH
_
H2ND-- C ~ H H~ ' - C ~ N H 2
_
CH3
_
CH3
I project I project
into paper into paper
COOH COOH
H2N~
I
C ~H
I
H~ C ~NH2
I
CH3 I
CH3
L-alanine D-alanine
To see the consequences of the amino acids having a stereogenic center at the
CHR group, consider alanine with R = CH3 (methyl group, where a carbon atom
is bonded to three hydrogen atoms) (Fig. 6). With one stereogenic center alanine
exists in two enantiomeric forms, as shown in Fig. 6. It is common to draw the
enantiomers of the amino acids in the so-called Fischer projection, named after
Emil Fischer, the great German chemist. Here the COOH and CH3 groups of
one of the enantiomers are aligned vertically with the COOH group at the top.
This forces the hydrogen and NH2 group attached to the stereogenic center to
occupy horizontal positions. If one imagines the stereogenic carbon to be in the
plane of the paper, the two vertical groups lie behind the paper and the two
horizontal groups lie in front. At this point the vertical and horizontal groups
and their bonds are projected onto the plane of the paper, resulting in the Fischer
projection of one of the enantiomers of alanine. The enantiomer which places the
NH2 group to the left of the vertical axis in the Fischer projection is assigned the
L absolute configuration. The other enantiomer, with the NH2 group to the right
of the vertical axis, is assigned the D absolute configuration. All 19 amino acids
with a stereogenic center at the CHR carbon thus have L and D enantiomers. It
II] THE CHIRALITY OF BIOMOLECULES 227
is important to note that the upper case D and L refer to absolute configuration
while the lower case "d" and "1" refer to the clockwise/counterclockwise rotation
of plane polarized light through the enantiomers; knowing one quantity does
not tell you anything about the other. A strange fact of living material is the
almost exclusive use of L-amino acids in cellular chemistry. The origin of this
homochirality is difficult to understand if one assumes that the amino acids were
synthesized on the primitive earth from achiral and racemic compounds without
any apparent intervening chiral force. Chiral products generated from achiral
or racemic compounds are themselves racemic. Homochirality is an accepted
tenant in any theory involving the origins of life. Science continues to ponder
the seemingly mystical question of the origins of specific homochirality: Did it
occur by chance or some fundamental bias?
Carbohydrates or sugars are a second class of important biological molecules.
Most people are familiar at least with the names of the carbohydrates glucose,
fructose, lactose, and sucrose (table sugar). Although they generally serve as
energy sources in cells, they have other functions as well. Glucose, for example,
is the building block for both cellulose, the fibrous material of plants, and
starch. Other carbohydrates can be found in cell walls. Ribose and deoxyribose,
two other carbohydrates, are building blocks of the nucleic acids which are
responsible for the genetic code and ultimately for all of the chemistry that takes
place in cells.
The name carbohydrate is a misnomer as it implies a hydrated form of carbon,
i.e., a compound in which carbon is bonded to water. This arises because sugars
have formulas of the type Cn(HzO)m, where H20 is the formula for water, and
n and m are integers. Instead, most carbohydrates are polyhydroxyaldehydes;
here hydroxy implies an OH group and aldehyde a CHO group, which can
only occur at the terminus of a molecule. Thus carbohydrates are aldehydes
containing two or more, thus poly, OH groups, one at each of the non-aldehydic
carbons: HOCHz(CHOH)nCHO. Because most carbohydrates contain more than
one stereogenic center, it is important to see what stereochemical consequences
there are for such molecules.
Consider the two stereoisomers of the carbohydrate 2,3,4-trihydroxybutanal
(HOCHzCHOHCHOHCHO) in Fischer projection: D-erythrose and L-erythrose,
each with stereogenic centers at carbons 2 and 3 (Fig. 7). These mirror-image
isomers are enantiomeric because they are non-superimposable. The enantiomer
at the left has the D absolute configuration because its OH group at carbon 3
(the one attached to the stereogenic center farthest removed from the aldehyde
group) is to the right of the vertical axis of carbon atoms, while its partner to
the right has the L absolute configuration because its carbon-3 OH group is to
the left of the vertical axis. As D- erythrose and L-erythrose are enantiomeric,
their properties and relationships are identical to those described above for
enantiomers with one stereogenic center.
228 R.N. Compton and R.M. Pagni [II
CHO OHC
I I
H-- C2 --OH HO-- C2--H
I I
H--C3--OH HO-- ~3--H
I
CH2OH HOH2C
D-erythrose ~L-erythrose
CHO OHC
[ I
HO-- C2--H H-- C2--OH
I I
H--~3--OH HO-- ~3--H
CH2OH HOH2C
D-threose L-threose
There are two other stereoisomers that have the same bonding pattern as
D-erythrose and L-erythrose (Fig. 8). One can imagine forming them from the
erythrose enantiomers by interchanging the H and OH groups at carbon 2. The
resulting structures, which are called D-threose and L-threose, are enantiomeric
with one another because, even in Fischer projection, it is easy to see that the
molecules are mirror images of one another and yet are not superimposable.
As with D-erythrose, D-threose has the D absolute configuration because its
OH group at carbon 3 is to the right of the vertical axis of carbon atoms, while
its mirror image partner has the L absolute configuration because its carbon-3
OH group is to the left of the axis.
What is new for molecules that have two stereogenic centers is the relationship
of the erythrose enantiomers to the threose enantiomers. They are clearly
stereoisomers of one another because the bond connectivities in the erythrose
isomers are the same as those in the threose isomers but the atoms are oriented
differently in space. Furthermore, neither erythrose isomer is superposable
on or has a mirror-image relationship with the threose enantiomers and vice
versa. Stereoisomers that do not have a mirror-image relationship are called
II] THE CHIRALITY OF BIOMOLECULES 229
reflection involves spatial inversion) plus a rotation through Jr, Rn, about an
axis perpendicular to the mirror plane. This is illustrated by the S-(-) and R-(+)
enantiomers of bromochlorofluromethane"
F Mirror Reflection F
.,,,~ Br Brm,.... /
C "'~H SI + R~ . . . . C
H"" \
Cl
Classical time reversal, T, represents the reversal of the motions of all the
particles in the system. Barron presented a vivid picture of the distinction
between "true" and "false" chirality by considering two rotating cones, one in a
state of linear translation and the other rotating but translationally at rest (Barron,
1986a,b). A stationary rotating cone exists as two mirror image states which are
interconverted by SI. Since P plus R:r also interconverts these two cones, the
object exhibits "false chirality." However, a spinning cone translating along the
axis of the cone, although interconverted by SI, is not interconverted by T and R
and thus is said to possess "true chirality." This is further illustrated by replacing
the spinning cones with rotating ammonia molecules:
FALSE CHIRALITY
,,, H H
TRUE CHIRALITY
Thus the instantaneous snapshot (i.e., time short compared to the tunneling time)
of a translating and rotating ammonia molecule represents a truly chiral system.
However, the fact that ammonia is rapidly converting (tunneling) from one form
to the other, requires that the two states would have definite chirality but not
definite parity. The two true eigenstates of definite parity are described by the
symmetric or antisymmetric combination of the two mirror-image forms of the
ammonia molecule. If the molecule is in one state, after a time r it will exist in
the other state. Thus, if observed over a time long compared to r, the probability
of being in either state is equal (racemization). This also illustrates the so-called
Hund's paradox (Hund, 1927), where a quantum-mechanical chiral molecule is
232 R.N. Compton and R.M. Pagni [III
E SI E ~ E T E
.,,q_..............~
~ D , ~ ~ D . - -" Y
B B B
g = kL + k D 9
Neither a static magnetic field (SMF), static electric field (SEF) or their
combinations are chiral. Gravitational fields (GF) are also achiral. However,
certain combinations of these fields together with rotations are chiral, as seen
in Table I. All of the advantage factors shown are dependent upon a molecular
factor, Z, determined by the structure of the molecule under consideration. The
chiral influence of longitudinally polarized [3 particles also depends upon the
electron helicity h, and the relative difference in the spin-polarized electron
scattering cross section ((yL _ ( j D ) / / ( o L _+_ (yD).
A report of asymmetric induction/resolution occurring in static magnetic
fields (Zadel et al., 1994) has been retracted (Breitmaier, 1994) and was shown
IV] THE CHIRALITY OF BIOMOLECULES 233
Table I
Chirality of field combination with rotation
Advantage factors
Local
Circularly polarized light 10-4 to I 0 -1
Global
Weak neutral currents IO-20ZrZ5kBT~ 10-13 to 10-17
Beta particles Xqh3A(oL-oD)/(OL +oD)~ 10-9 to 10-11
Many plants also exhibit handedness. Charles Darwin, the father of the theory
of evolution, made detailed observations of the "twining" of certain climbing
plants, that is, their propensity to grow in a spiral or corkscrew manner (Darwin,
1906). In nature, twining plants are homochiral; honeysuckle twines to the left
and morning glory twines exclusively to the right. Most other plants grow in a
right-handed spiral and most seashells also exhibit a right-handed helicity. The
human umbilical cord, on the other hand, twists in either direction. The left tusks
of the Narwhal, a species of toothed whale, twist in a counterclockwise direction.
Figure 10 shows the right-hand twist exhibited by a large Blue Gum tree (genus
Eucalyptus) located in the Botanical Gardens of Christchurch, New Zealand.
IV] THE CHIRALITY OF BIOMOLECULES 235
i
_
i
~cg3 3 ~"CH3 H3
OH
,I
O H OCH2CHCH2NHCH(CH3)2
II ,I
H2NCCH2m C mCOOH
I
NH2
asparagine propranolol
O O
OH
I,
HOCH2CCH2CI
I
H
FIG. 11.
naturally occurring D-glucose and the unnatural L-glucose are equally sweet. If
an inexpensive synthesis of it were available, L-glucose would be an ideal non-
nutritive sweetener.
Enantiomerically pure drugs are becoming increasingly important even though
they are generally more expensive to prepare than their racemic counterparts
(Deutsch, 1991; Stinson, 1995, 1998, 2000, 2001). The world-wide market
for single-enantiomers drugs already exceeds $120 billion per year. Often
one enantiomer is therapeutic while the other is benign or even harmful.
Separate enantiomers of barbituric acid derivatives can function as a narcotic
or anticonvulsant. (-)-Propranolol acts as a beta blocker for heart disease while
its enantiomer acts as a contraceptive. The S form of 1-chloro-2,3-propanediol is
a pharmaceutical while the R form is poisonous. One enantiomer of the steroid
estrone is a sex hormone while the other is inactive.
Thalidomide, which possesses one stereogenic center (at the starred position),
is undoubtedly the most notorious compound where one enantiomer is reported
to be therapeutic while the other is harmful. The R enantiomer of this
compound has been used to alleviate the effects of morning sickness of pregnant
women while the S enantiomer gives rise to teratoidism, i.e., birth defects, in
developing fetuses. It has been estimated that 12 000 children have been born
with thalidomide-induced birth defects in the 1950s, primarily in Europe and
South America. This molecule was not approved for use in the United States
except for research purposes. It had been presumed that if enantiomerically pure
(R)-thalidomide were given to pregnant women the problem of birth defects
would be avoided. However, it is now known that thalidomide racemizes rapidly
in blood plasma so that providing an enantiomerically pure form of thalidomide
would not alleviate the problem of teratoidism. Thalidomide may still prove
useful in certain circumstances. The compound suppresses the growth of blood
vessels (angiogenesis) which may prove useful in the treatment of certain cancers
and AIDS-related conditions. Research is now underway on the development of
resolved derivatives of thalidomide which are therapeutic but do not racemize
easily.
Approximately 530 synthetic chiral drugs are now marketed worldwide.
Because of the technical difficulties and corresponding expense of making
enantiomerically pure drugs, only about 60 of these compounds are marketed
in their enantiomerically pure form. Increasing pressure from the scientific
community along with tighter restrictions imposed by the U.S. Food and Drug
Administration means that more enantiomerically pure pharmaceuticals will
become available in the near future.
that carbohydrates, which are found in starch, cellulose, and the nucleic acids,
exist in nature exclusively with the D absolute configuration. Most amino acids,
which are the building blocks of proteins and enzymes, have the L absolute
configuration. This is true regardless of the type or complexity of the organism,
be they found in a bacterium, betel (palm or pepper), beetle, beagle, or
the Beatles. Thus specific homochirality of biomolecules is a fundamental
characteristic of life. Any plausible theory of the origins of life on earth must take
this fact into account. Two general types of theories have been invoked to explain
the origin of homochirality on the earth: (1) those involving a chance or random
selection of the homochiral molecules that were incorporated into the first living
organisms; and (2) those that require an internal or external chiral force to bring
about the asymmetric synthesis of the homochiral molecules. As will be seen in
due course, many theories in the second grouping also have a random quality
about them because the chiral influence itself may appear randomly. Leaving
aside the accidental "chance scenario," theories have concentrated on how chiral
forces may influence the prebiotic asymmetric synthesis of biological molecules
in nature.
Ideas that specific homochirality has resulted from some prebiotic asymmetric
synthesis have become more credible in recent years following the analysis
of organic compounds brought to the earth in meteors. Cronin and Pizzarello
(1997) for example, found a 7 to 9% excess of L amino acids in the Murchison
meteorite found in Australia. It is believed that this enantiomeric excess did not
arise by terrestrial contamination because some of the amino acids found in the
meteorite do not exist in the biosphere. The Murchison meteorite, a carbonaceous
chondrite, was created about 4.5 billion years ago in the asteroid belt, strongly
suggesting an asymmetric prebiotic chemical synthesis of the carbon-containing
molecules in the universe. The "normal" laboratory synthesis of amino acids, of
course, yields a racemic mixture. For example, an electric discharge (a mimic
of lightning) in a mixture of methane, nitrogen, ammonia, and water produced
racemic mixtures of the amino acids, alanine (1.7% yield), asparagine (0.024%),
and glutamine (0.051%); achiral glycine was found in 2.1% yield (Miller, 1959).
Assuming an extraterrestrial asymmetric synthesis of the amino acids found in
the Murchison meteorite, some chiral influence has been at work on the meteorite
when it was first synthesized or during the intervening 4.5 billion years. It is
plausible that the source of homochiral molecules necessary for the formation
of life on the earth has an extraterrestrial origin. Even if this be true, the
question remains as to how the asymmetric synthesis occurred. Several possible
explanations follow.
Circularly polarized light is a plausible chiral influence. It is well known that
the photochemistry of racemic mixtures of molecules initiated with circularly
polarized light can lead to an excess of one enantiomer over the other, either
in product or recovered reactant (Feringa and van Delden, 1999; Bonner,
238 R.N. Compton and R.M. Pagni [V
1996; Rau, 1983; Balavoine et al., 1974). This photochemistry can occur
by photoequilibration of a racemic mixture of molecules without any loss of
reactant or by the selective destruction of one enantiomer over the other. Both
processes take advantage of the fact that enantiomers have different absorptivities
(cross sections) when exposed to LCPL and RCPL. Both methods, however,
have serious drawbacks. In the first instance enantiomeric excesses tend to
be low because differences in absorptivities usually are very small while the
absorptivities are generally large. In the second case, very high enantiomeric
excesses can be obtained but only at the expense of destroying most of the
reactant. There are several notable photoreactions in the literature initiated by
CPL. Shimizu and Kawanishi have studied the two-photon photochemistry of
D,L, i.e., racemic tartaric acid with 351-nm CPL from a XeF excimer laser
(Shimizu and Kawanishi, 1996a,b; Shimizu, 1997). Irradiation with RCPL led
to a selective destruction of the L enantiomer while the concentration of the
D enantiomers changed little; this led to a maximum enantiomeric excess of
recovered tartaric acid of 7.5%. Irradiation with LCPL was unfortunately not
carried out.
COOH
I COOH
~HOH 351-nm RCPL from
XeF excimer laser
r
HO H
+ CO2, CO, H 2
CHOH H OH
I
COOH COOH
CPL
R enantiomer S enantiomer
trans-cyclooctene cis-cyclooctene
Although enantiomeric enrichment was found, the effect was small. Photolysis of
the racemic amino acid, D,L-leucine, with RCPL and LCPL in aqueous solution
(in water) at 212.8 nm also afforded small, but meaningful enantiomeric excesses
V] THE CHIRALITY OF BIOMOLECULES 239
type observed for atoms have not been reported. Instead, research in P-odd effect
in molecules has concentrated on the prediction and detection of PVED between
R and S enantiomers. Rein (1974) and Letokhov (1975) first suggested that the
electroweak interaction would lift the degeneracy between enantiomers predicted
by normal quantum electrodynamics. A number of calculations of the PVED for
small molecules have been published (Hegstrom et al., 1980; Zel'dovich et al.,
1977; Mason, 1984; Mason and Tranter, 1984; MacDermott et al., 1992; Bakusov
et al., 1998; Lazzeretti and Zanasi, 1997; Zanasi et al., 1999; Laerdahl and
Schwerdtfeger, 1999; Laerdahl et al., 2002; Berger et al., 2001). The Hamiltonian
operator describing the PVED for a molecule containing i electrons and n nuclei
is given by
where N11 and Z11 are the numbers of neutrons and protons, respectively, and
0w is the Weinberg mixing angle. An excellent review of the state of affairs
of the theoretical calculations of the parity-violating energy difference for small
molecules has been published by Buschmann, Thede and Heller (2000). In the
1980s, ab initio calculations gave PVED values on the order of 10-14 J/mol
and, interestingly, concluded that the L-amino acids and D-sugars were lower
in energy. Until recently, this stabilization energy was believed to be too small
to be of significance to prebiotic asymmetric synthesis. Although autocatalytic
processes such as those evoked by Kondepudi and Nelson (1983, 1984a,b, 1985)
could play a role in providing enantiomeric excesses over long times, the small
energy differences expected did not encourage further speculation. However,
more recent calculations, particularly those by Quack and co-workers (see Berger
and Quack, 2000 and others contained therein) and Schwerdtfeger et al. (see
Laerdahl, Wesendrup and Schwerdtfeger, 2000) are about an order of magnitude
larger and give new interest to possible PVED effects in prebiotic asymmetric
chemistry. However, both of these groups have shown that the magnitude and
indeed the sign of the PVED for alanine depend upon its exact molecular
conformation (shape that may change by rotating atoms or group of atoms
242 R.N. Compton and R.M. Pagni [V
around single bonds) and therefore may not lead to a preferential stabilization
of one enantiomer over the other. There is an obvious critical need for an
experimental measurement of the PVED. Unfortunately, a measurement on the
order of 10- 1 4 J/mol is beyond any present experimental technique. Fortunately,
the PVED increases with the magnitude of the atomic number. Specifically, the
PVED scales with Z 6 (Laerdahl and Schwerdtfeger, 1999). Thus, molecules with
atoms having large atomic numbers will show the largest PVED and may provide
an experimental test for PVED.
There have been a number of experimental attempts to measure PVED. Most
notably, high-resolution infrared absorption spectroscopy has been used on two
occasions. Arimondo, Glorieux and Oka (1977) observed inverted Lamb-dip
ro-vibrational transitions for the two enantiomers of camphor and found them to
agree to within 10-8. Recently, Daussy et al. (1999) demonstrated that the C - F
stretching mode of the two CHFBrC1 enantiomers agreed to within 13 Hz. This
places an upper limit on AEpv/E of <4x 10 -13. Although these measurements
are five orders of magnitude more sensitive than the results for camphor, they
are still not sensitive enough. Theoretical studies on CHFBrC1 give an energy
difference of only 2 mHz, (-8 x 10-18 eV) for the C - F frequency (Laerdahl et al.,
2002).
Keszthelyi (1994) used M6ssbauer spectroscopy to establish an upper limit
of 4x 10 -9 for the energy difference of 1- and d-tris(1,2-ethanediamine)iridium
complexes. A Z 6 scaling was used to estimate the energy difference of
1.1 x 10-12 eV between the two enantiomers. Thus the measured upper limit is
three orders of magnitude higher than the expected Z-scaling result. This report
contains very few details on the experimental procedures used, and no M6ssbauer
spectra were shown.
Although all of the L amino acids are predicted to lie lower in energy than
the corresponding D amino acids, the differences are so small that it is hard to
envision how this could lead to a dominance of the L amino acids in biology. A
large amplification mechanism would be required. However, the PVED scales
with Z 6, as noted earlier. Thus, for larger molecules containing atoms with
larger atomic numbers, the energy differences between enantiomers should
be sufficiently large to be observable with currently available spectroscopic
techniques such as nuclear magnetic resonance, M6ssbauer and perhaps infrared
spectroscopies. Lahamer et al. (2000), for instance, reported an energy difference
between enantiomers of an iron complex using M6ssbauer spectroscopy. Due to
the fact that these experiments were performed on crystalline material, the energy
difference may be due to crystalline effects, although the difference in energy
(-10 -l~ eV) is close to that predicted by scaling the PVED with atomic number.
In 1991 Abdus Salam (1991), who along with Glashow and Weinberg
united the electromagnetic and weak force theory into one electroweak theory,
speculated that the Z ~ interactions might provide an explanation of the
VI] THE CHIRALITY OF BIOMOLECULES 243
H
,I
HzN~C~COOH
I
R
R
O
(+)-camphor tyrosine H O ~ H 2 ~
J
CH 2
] tryptophan
CH3CH2~COOH
H
FIG. 12.
positive results (Ulbricht and Vester, 1962). Garay (1968), on the other
hand, found D-tyrosine, an amino acid (Fig. 12), to degrade more rapidly
in water containing radioactive strontium chloride (9~ than the naturally
occurring L-tyrosine enantiomer. Unfortunately, the method of analysis that
Garay u s e d - UV spectroscopy- is not definitive. Darge et al. (1976), likewise,
found positive results. In these experiments a frozen aqueous solution of
racemic D,L-tryptophan, another amino acid, and radioactive phosphate (32po43)
underwent self-radiolysis for 12 months; an astounding 19% enantiomeric excess
of the D enantiomer was reported. As with the Garay experiments, the methods
of analysis- UV spectroscopy and polarimetry- are not definitive. When the
Garay and Darge experiments were repeated (with considerable modification)
on D,L-tyrosine, D,L-tryptophan, and other amino acids by Bonner (Bonner,
1974; Bonner and Flores, 1975, Bonner et al., 1979) using gas chromatography,
where the enantiomers are separated and quantitated, as the analytical tool, no
asymmetric degradation of any amino acid was found even though extensive
overall degradation of the amino acids had occurred. Calvin and colleagues
(Bernstein et al., 1972) and then Bonner (Bonner et al., 1978) also examined
the internal beta radiolysis of several 14C-labeled amino acids (14C is a beta-
particle emitter), Calvin by polarimetry and Bonner by gas chromatography;
no positive results were obtained. Bonner did have success, however, with
polarized electrons not from beta decay but using longitudinally polarized
electrons (120 KeV) from a linear accelerator (Bonner et al., 1975, 1976/77).
VI] THE CHIRALITY OF BIOMOLECULES 245
The target was a solid sample of racemic leucine, a still different amino acid.
Antiparallel electrons afforded a slight excess of L-leucine (~1% enantiomeric
excess) after about 50% degradation of the sample, while parallel electrons
afforded a slight excess of the D enantiomer (~0.9% enantiomeric excess) after
about 75% degradation. More recently, Akaboshi et al. (1999) looked for the
asymmetric decomposition of the racemic amino acid, D,L-aspartic acid, in
tritiated water (3H20 , 3H--tritium, a beta emitter). When the recovered amino
acid was examined by HPLC, another technique that separates and quantitates
the enantiomers, no enantiomeric excess was detected.
Except for Bonner's results using polarized electrons generated in a linear
accelerator, none of the other experiments involving amino acids, all of
which involved beta radiolysis, led to asymmetric degradation. Several related
experiments did give positive results. Beta radiolysis of polycrystalline amino
acids yields free radicals (species with one unpaired electron) which are detected
by electron-spin resonance spectroscopy, a very sensitive technique. Irradiation
of D- and L-alanine with internal or external beta radiation affords an excess
of radicals from the D enantiomer (Akaboshi et al., 1978, 1981, 1982; Conte
et al., 1986). Beta particles passing through the liquid enantiomers, R- and
S-2-phenylbutyric acid scatter differently as evidenced by emitted Cerenkov
radiation (Garay and Ahlgren-Beckendorf, 1990). The scattering of polarized,
low-energy electrons from enantiomers such as D- and L-camphor also occurs
asymmetrically (Campbell and Farago, 1985; Blum and Thompson, 1998).
To date there is no unambiguous evidence that the beta radiolysis of amino
acids leads to the faster degradation of one enantiomer as compared to the other,
i.e. deracemization. There is evidence, on the other hand, for the racemization of
enantiomers of amino acids by beta radiation. The self beta radiolysis of optically
pure 14C-labeled amino acids over the course of decades led to the compounds'
partial racemization. (Bonner, 1996). Radiolysis of L-alanine, D-2-aminobutyric
acid, L-norvaline, L-norleucine, and D- and L-leucine, all amino acids, with
y-rays from a cobalt source (6~ results in partial racemization of the amino
acids in all cases (Bonner and Lemmon, 1978a,b). Thus any mechanism
involving radiolysis that builds up enantiomeric excess in recovered amino acid
would also provide a mechanism for its loss.
There is a way in which beta radiolysis has led to significant amplification of
enantiomeric excess. This involves the behavior of sodium chlorate (NaC103) in
water, for which relevant background material will now be presented.
NaC103 is an achiral molecule consisting of a spherical sodium cation (Na +)
and a chlorate anion (C103) of C3v symmetry. Solutions of this compound in
water are likewise achiral and thus optically inactive. The colorless, transparent
crystals of this molecule, on the other hand, are chiral because they belong to the
chiral P213 space group. Crystals of NaC103 thus exist in enantiomeric forms
which are easily distinguished by polarimetry (Pagni and Compton, 2002).
246 R.N. Compton and R.M. Pagni [VI
If the physics and chemistry described above generally yield enantiomers with
very small enantiomeric excesses, a large amplification mechanism is required to
attain the homochirality of the biological world. This is particularly true if PVED
was the initial source of asymmetry because its effect is exceedingly small.
Where crystallization and aggregation phenomena are concerned, however, the
initial enantiomeric excesses may be substantial and only a modest amplification
may be required to attain homochirality.
The crystallization effect is best exemplified with sodium chlorate. Seeding
of an evaporating aqueous sodium chlorate solution with (+) and (-) crystals
yields (+) or (-) crystals, exclusively. Stirring has the same effect but the
direction of the induced homochirality is random. Circularly polarized electrons
and positrons generated from radioactive nuclei, as noted above, have a similar
effect on the distribution of (+) and (-) sodium chlorate crystals.
Although it is difficult to see how sodium chlorate crystals could have played
a role in the origin of biological homochirality because they are synthetic,
naturally occurring quartz, which exists in enantiomeric forms, could have played
such a role. Unfortunately, there is essentially no excess of one enantiomeric
form of quartz over the other on the earth although local excesses may exist
(Frondel, 1978; McBride, 2001). Interestingly, asymmetric adsorption of the
alanine enantiomers onto (+) and (-) quartz has been demonstrated by Bonner
(Bonner et al., 1974). Until the recent work of Soai, which will be described
below, quartz had not served as a medium for an asymmetric chemical reaction.
248 R.N. Compton and R.M. Pagni [VI
CO2CH(CH3)2
(CH3)2CHO2C~ (CH3)2CHO2C CO2CH(CH3)2
hv
dibenzobarrelene dibenzosemibullvalene
give enantiomeric products R and S, each of which catalyzes its own formation
reversibly and with each other irreversibly to produce a product P:
A + B ~,-~--R, A+B~----S,
A + B + R ~,-~-2R, A + B + R ~,-~--2S, R + S--,P.
This system is open because A and B are continually added while P is continually
removed. As with Frank's model, this one becomes unstable under certain
conditions, thus yielding one enantiomeric product in excess. If this system is
biased, however, with an initial excess of R or S, even ever so slightly due to
PVED, one pathway becomes dominant. If R is in excess initially, the pathway
leading to production of R will be favored, and vice versa if S is in excess
initially. Calculations show that in periods as small as tens of thousands of years,
the initial very small enantiomeric excess due to PVED can be amplified to
enantiomeric excesses close to 100% favoring the L-amino acid. It is unfortunate
that there is no possibility of testing this mechanism.
Soai and coworkers have developed in recent years a remarkable autocatalytic
reaction which also results in significant amplification of chirality. (Shibata et al.,
1996, 1998; Soai et al., 1999, 2000; Soai and Shibata, 1999; Sato et al., 2000a,
2000b.) In this chemistry the chiral product also functions as a catalyst for its
own production. Although this chemistry could not have occurred in the prebiotic
world, prebiotic chemistry based on the model of this chemistry could have
played a role in the origin of homochirality. Let us begin by examining the
reaction under consideration.
Treatment of achiral pyrimidine-5-carboxaldehyde which contains a carbon-
oxygen double bond (carbonyl group) with achiral diisopropylzinc [isopropyl =
-CH(CH3)2] affords a zinc alkoxide product. Treatment of the zinc alkoxide
in turn with water yields an alcohol product. The initial reaction involves the
transfer of an isopropyl group from the zinc reagent to the carbonyl carbon of
the pyrimidine reagent. Both the initially formed zinc alkoxide and the isolated
alcohol contain a single stereogenic center. Because there are no chiral forces or
optically active reagent involved in the chemistry, both products are racemic.
0 OZnCH(CH3)2
~ ~ "- ~ Jc"CH(CH3)2
H + [(CH3)2CH]2Z
n ...- -~- ~
N "N
pyrimidine-5- diisopropylzinc zinc alkoxide
carboxaldehyde /
OH
] ~ H CH(CH3)2
~
N
alcohol
250 R.N. Compton and R.M. Pagni [VI
The zinc alkoxide still has a reactive isopropyl group which also adds to the
carbonyl group of the pyrimide-5-carboxaldehyde to yield a zinc dialkoxide with
a second stereogenic center. Recall that a product with two stereogenic centers
yields a maximum of 4 stereoisomers. In this instance a pair of enantiomers
(RR and SS) in racemic form, and a meso compound (RS=SR) are generated
in unequal amounts. On treatment with water this mixture of zinc dialkoxide
stereoisomers yields the same alcohol as shown above in racemic form.
CH(CH3)2 CH(CH3) 2
,I ,I
Ar--- C ~ O ~ Z n ~ O ~ C ~Ar Ar = pyrimidine ring
I I
H H
zinc dialkoxide
RS = SR (meso)
RR and SS (enantiomeric pair)
The system becomes very interesting when a small amount of optically
active alcohol is added to diisopropylzinc before addition of the carboxaldehyde.
The added alcohol reacts with the zinc reagent to yield the optically active
(S)-zinc alkoxide. If the added alcohol has the S absolute configuration, so
does the zinc alkoxide. Before addition of the carboxaldehyde, the system
contains mostly achiral diisopropylzinc and a little (S)-zinc alkoxide. When
the carboxaldehyde is then added, it reacts preferentially with the optically
active zinc alkoxide. This can happen in two ways, creating either an S
or an R stereogenic center in the zinc dialkoxide. For steric reasons, the
second addition yields the S absolute configuration at the new center. By a
disproportionation reaction the (S)-zinc dialkoxide reacts with diisopropylzinc
to generate more (S)-zinc alkoxide which is then used to add to still more
pyrimidine-5-carboxaldehyde. Overall then, the addition of a little (S)-alcohol
to the systems yields lots of (S)-alcohol.
(CH3)2CHx (CH3)2CHx
Ar,, .)C -- OH + [(CH3)2CH]2Zn ~ Ar,,')C--OZnCH(CH3)2 + Propane
H H
(S)-alcohol (S)-zinc alkoxide
(CH3)2CHx,
...._ (CH3)2CHN /QCH3)2CH
Ar,"~C --OZnCH(CH3)2
"- ~C_O_ZnOC~,,H~....x
O
[ (S,S)-zinc dialkoxide I
Ar H original ~ new
S center J S center
J
~ [(CH3)2CH]2Zn
2 (S)-zinc alkoxide
VI] THE CHIRALITY OF BIOMOLECULES 251
Table II
Amplification of chirality in the Soai reactions
Even more amazing results are obtained when the added alcohol is only
slightly enriched in one enantiomer (2% enantiomeric excess). After one
reaction, the alcohol has enantiomeric excess = 10%. If this alcohol in turn
is used to initiate a second reaction, the resultant alcohol has enantiomeric
excess = 57%. After 4 such cycles, the original 2% enantiomeric excess has
become 88%, a 44-fold amplification of chirality.
Similar but even more spectacular results are also obtained on the reaction
of pyrimidine carboxaldehydes using the amino acids leucine (2% enantiomeric
excess favoring D or L) and valine (1% D or L), alcohols (0.1% enantiomeric
excess R or S), (+) and (-) quartz and (+) and (-)-NaC103 as initiators (Table II).
Amplifications of close to a thousand have been obtained after one reaction cycle
in some cases.
The results discussed above provide clear theoretical and experimental
evidence that autocatalysts can lead to enantioamplification. Autocata|ysis is,
however, not the only mechanism by which enantiomer enrichment may have
occurred in the prebiotic world. Yamagata has proposed that amplification may
have occurred by an accumulation of small enrichments during each step of
the synthesis of a polymer such as a protein or nucleic acid (Yamagata, 1966;
Yamagata et al., 1980). The starting material in this scheme is a racemic mixture
of a monomer to be incorporated into the polymer; the monomer will be called
R-M and L-M. Now allow R-M to react with itself to make a dimer (R-M)2.
A similar reaction converts L-M into (L-M)2, the enantiomer of (R-M)2. Because
of PVED, the two reactions occur at minutely different rates. Repeat the reactions
again to form (R-M)3 and (L-M)3. These also occur at slightly different rates.
252 R.N. Compton and R.M. Pagni [VII
Thus, if homopolymers (R-M)n and (L-M)n are ultimately formed, the PVED
kinetic effect will have been amplified n - 1 times. Although this amplification
would occur several thousand times in forming a protein, it would occur tens of
millions of times to form DNA. In forming the protein the PVED kinetic effect
occurs within the D- and L-amino acids, 20 of which are commonly used in life,
whereas for DNA, the differences occur in cyclic forms of the carbohydrates D-
and L-deoxyribose.
The simple scheme involving the build-up of a polymer from a single pair of
enantiomers is too simple because R-M and L-M can also react with one another
although at rates different from the R-M + R-M and L-M + L-M reactions. This
produces a pair of dimer enantiomers, (R-M)(L-M) and (L-M)(R-M). The PVED
kinetic effect will also operate when R-M and L-M react with one another. If
this "random" polymerization continues, one will obtain in theory 2 n pairs of
enantiomers for a polymer with n monomeric units. Each pair of enantiomers
will be subject to the cumulative PVED effect; each pair of enantiomers will be
formed in unequal amounts.
If the starting pool of reactants consists of 20 different racemic molecules, as
would be the case for the amino acids, the chemistry becomes incredibly complex
because each of the 40 reactants can react to form 1600 dimeric products
consisting of 800 pairs of enantiomers. The dimers would then yield 64000
trimeric products.
does not result in amplification. Thus, eeproduct= (eeo)(eeligand), where eeo is the
maximum enantiomeric excess that is attainable for the reaction of interest.
kR ke
M + LR ~ MLR---+ PR, M + Ls ~ MLs ' Ps.
On the other hand, if the metal contains two ligands, three catalysts, MLRLR,
MLsLs and MLsLR, are possible, each of which catalyzes the asymmetric
reaction to yield, respectively, PR, Ps and racemic product, each at its own
distinctive rate. The expression relating eeproduct to eeligand is now more complex
in that it contains/3, which is the ratio of the amount of meso complex, MLRLs,
to the sum of the homochiral complexes, MLRLR and MLsLs, and g, which is
the ratio of the rate constant for the reaction of the meso complex, kRs, to that
of the homochiral complex MLRLR, kRR (kRR = kss):
When /3 = 0, i.e., the meso complex is not present, or g = l, i.e., the meso
and homochiral complexes have the same rate of reactivity, the new equation for
eeproduct reverts to the original one where a linear response is anticipated. When
g < 1, a positive non-linear effect (amplification) is expected which reaches
its maximum effect at g = 0, where the meso complex MLRLs is unreactive.
Values of g > 1 result in a negative non-linear or deamplification effect. In order
to calculate the exact positive, zero or negative non-linear effect it is necessary
to know K = (MLRLs)2/(MLRLR)(MLsLs), the equilibrium distribution of the
complexes. If the complexes are formed randomly, K = 4, for example. It should
be noted here that the chemistry of Soai described in detail above is almost
certainly an example of a positive non-linear amplification of chirality involving
a diastereomeric zinc complex of unknown structure. Diastereomeric catalysts
are required for this behavior to occur; enantiomeric complexes are excluded.
As seen above, there is significant theoretical speculation and experimental
evidence for enantioamplification. What is not always appreciated is that
racemization chemistry will always compete. Degradation chemistry will also
remove the substrate from the racemic pool being amplified. As seen earlier in
256 R.N. Compton and R.M. Pagni [VII
the article, beta radiation racemizes amino acids. Amino acids also racemize in
water with a half-life of about 6000 years, the exact value depending on the
structure of the amino acid (Bada, 1972).
COOH COOH
I water I
H2N - C --H -... H-- C --NH 2 1;1/2- 6000 years
I /
R R
L amino acid D amino acid
It is possible to date bone and teeth in archaeological samples using this fact.
Dating is difficult, however, because the half-life of racemization is environment
dependent. The optically active amino acids in the Murchison meteorite, for
example, may have remained that way for 109 years.
Carbohydrates, as noted near the beginning of the article, are polyhydroxy-
aldehydes and ketones. As is the case with all aldehydes and ketones with
similar structure, they readily form enols and enolates reversibly in the presence
of acid and base, respectively. In so doing the stereogenic center next to the
carbonyl group (C=O) is lost initially and reformed in two ways: with the original
absolute configuration or with the other absolute configuration. By such facile
pathways, D-glyceraldehyde is converted into L-glyceraldehyde, thus racemizing
the molecule. The enol and enolate also react to give an isomeric ketone,
2,3-dihydroxy-2-propanone, with no stereogenic centers. The racemization of
amino acids in waters also occurs through intermediate enols and enolates:
H\ /OH
C
II
CHO
aci
~ HO/ C \ CH2OH ~ . ~ d CHO
I enol I
H-- C --OH HO-- C --H
I I
CH2OH ~ CH2OH
D-glyceraldehyde ~ H\ /O- L-glyceraldehyde
C
II
/C\
HO CH2OH
enolate
HOCH2\
enol, enolate /c=o
HOCH2
regenerates the center, and an isomeric compound if the center is not regenerated.
D-glucose, for example, yields the diastereomer D-mannose and the isomer
D-fructose when treated with base in water.
CHO CHO
I I HOCH2~ //O
H - - ~ --OH HO-- ~ - - H
HO-- C --H base HO-- C --H HO-- C --H
I ~ I + I
H--C --OH H--C --OH H--C --OH
I I J
H - - C --OH H - - C --OH H - - C --OH
I I I
CH2OH CH2OH CH2OH
D-glucose D-mannose D-fructose
Thus most carbohydrates will not racemize but will quite readily be converted
into diastereomeric and isomeric compounds. How such chemistry would affect
the amplification of chirality is unclear but important.
Interestingly, the carbohydrates, ribose and deoxyribose, that exist in nucleic
acids are not susceptible to the above chemistry because they exist in cyclic
forms that mask the carbonyl group. Under such circumstances enols and
enolates cannot form.
In conclusion it is fair to say that any mechanism that amplifies a small
enantiomeric excess into a larger one must do so at rates faster than mechanisms
that racemize or degrade the compound of interest.
VIII. Conclusions
Considerable progress has been made in the last few decades in understanding the
origin and evolution of the molecules of life (Brack, 1998; Mason, 1991). This
cannot be said about the origins of specific homochirality. As this article attests,
the field is active and many interesting results have been obtained, but there are
still a very large number of plausible explanations for specific homochirality.
Hopefully future research will reject some explanations and refine others to the
point where a likely cause is found. This may never occur, however, because the
time scales of some theories are vast and thereby difficult to study experimentally.
The origin may have arisen from a random event and is thus not explainable by
any theory or testable by experiment, because of our inability to go back and
see it transpire in the first place. Thus, the origins of specific homochirality may
remain one of the many mysteries of life.
IX. Acknowledgment
The authors thank the National Science Foundation for support of this work, and
graduate student Rodney Sullivan for his assistance.
258 R.N. C o m p t o n a n d R . M . P a g n i [X
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ADVANCES IN ATOMIC, M O L E C U L A R , A N D O P T I C A L P H Y S I C S , VOL. 48
JOHANNES DENSCHLA G
Institut fiir Experimentalphysik, Universita't Innsbruck, 6020 Innsbruck, Austria
CARSTEN HENKEL
Institut fiir Physik, Universitdt Potsdam, 14469 Potsdam, Germany
I. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 263
II. Designing Microscopic Atom Optics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 265
A. Magnetic Interaction ....................................... 265
B. Electric Interaction ........................................ 283
C. Traps and Guides formed by C o m b i n i n g the Interactions . . . . . . . . . . . . . . . 286
D. Miniaturization and Technological Considerations . . . . . . . . . . . . . . . . . . . . 289
III. Experiments with Free-Standing Structures . . . . . . . . . . . . . . . . . . . . . . . . . . . 292
A. Magnetic Interaction ....................................... 292
B. Charged Wire Experiments ................................... 300
IV. Surface-Mounted Structures: The Atom Chip ......................... 303
A. Fabrication . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 304
B. Loading the Chip . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 307
C. Atom Chip Experiments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 314
V. Loss, Heating and Decoherence .................................. 324
A. Loss Mechanisms ......................................... 324
B. Heating ................................................ 330
C. Decoherence . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 335
VI. Vision and Outlook . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 342
A. Integrating the Atom Chip . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 343
B. Mesoscopic Physics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 346
C. Q u a n t u m Information . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 348
VII. Conclusion ................................................ 351
viii. Acknowledgement ........................................... 351
IX. References ................................................ 352
I. I n t r o d u c t i o n
Scientific and technological progress in the last decades has proven that
miniaturization and integration are important steps towards the robust application
of fundamental physics, be it electronics and semiconductor physics in integrated
circuits, or optics in micro-optical devices and sensors. The experimental effort
described in this work aims at achieving the same for matter wave optics.
A. MAGNETIC INTERACTION
A particle with total spin F and magnetic moment/u = gFttBF experiences the
potential Vmag = - / ~ " B = --gFktBmFB, (1)
where /re is the Bohr magneton, gF the Land6 factor of the atomic hyperfine
state, and mF the magnetic quantum number. In general, the vector coupling/u. B
results in a complicated motion of the atom. However, if the Larmor precession
(mL = ItBB/h) of the magnetic moment is much faster than the apparent change of
direction of the magnetic field in the rest frame of the moving atom, an adiabatic
approximation can be applied. The magnetic moment then follows the direction
of the field adiabatically, mF is a constant of motion, and the atom is moving in
a potential proportional to the modulus of the magnetic field B = ]B].
Depending on the orientation of/u relative to the direction of a static magnetic
field, one distinguishes two cases:
(1) If the magnetic moment is pointing in the same direction as the magnetic
field (Vmag < 0), an atom is drawn towards increasing fields, therefore it is in
a strong-field seeking state. This state is the lowest energy state of the system.
266 R. Folman et al. [II
Minima o f the potential energy are found at maxima of the field. Maxima of the
magnetic field in free space are, however, forbidden by the Earnshaw theorem 1.
This means that for trapping atoms in the strong-field-seeking state, a source
of the magnetic field, such as a current-carrying material object or an electron
beam, has to be located inside the trapping region.
(2) If the magnetic moment of an atom is pointing in the direction opposite
to the magnetic field (Vmag > 0), the atom is repelled from regions with high
magnetic fields; it is then in the metastable weak-field seeking state. In this case,
minima o f the modulus of the field correspond to potential minima. Because a
minimum of the modulus of the magnetic field in free space is not forbidden
by the Earnshaw theorem, traps of this type are most c o m m o n for neutral atom
trapping. Losses from the traps are a potential problem (see Sect. V), especially
when non-adiabatic transitions to the energetically lower high-field-seeking states
become likely in regions of low or even vanishing fields.
A. 1. Kepler guide
A possible realization of a trap for an atom in the strong-field-seeking state is
a current-carrying wire with the atom orbiting around it (Vladimirskii, 1961;
Schmiedmayer, 1992, 1995a,b; Schmiedmayer and Scrinzi, 1996a,b; Denschlag,
1998; Denschlag et al., 1999b). The interaction potential is given by 2
1
Vmag = - / I / - B = - ~ Iw-%'la,r (2)
where Iw is the current through the wire, % is the azimuthal unit vector in
cylindrical coordinates, and /z0 = 4 ; r m m G / A is the vacuum permeability.
This potential has the 1/r form of a Coulomb potential, but the coupling
/ u - B is vectorial. Using the adiabatic approximation, Vmag corresponds to a
2-dimensional scalar ( l / r ) potential, in which atoms move in Kepler orbits 3.
In the quantum regime, the system looks like a 2-dimensional hydrogen atom
in a (nearly circular) Rydberg state. The wire resembles the "nucleus" and
l The Earnshaw theorem can be generalized to any combination of electric, magnetic and
gravitational fields (Wing, 1984; Ketterle and Pritchard, 1992).
2 This and all other expressions for magnetic and electric fields in this section are given in the limit
of an infinitely thin wire, unless stated otherwise.
3 From corrections to the adiabatic approximation to the next order, we obtain an effective
Hamiltonian for the orbital motion of the atom where the Coulomb-like binding potential is corrected
by a small repulsive 1/r2 interaction (Shapere and Wilczek, 1989; Aharonov and Stern, 1992; Stern,
1992; Littlejohn and Weigert, 1993; Schmiedmayer and Scrinzi, 1996a,b). As a result, the Kepler-
like orbits show an additional precession around the wire. A very similar potential can be realized
for small polar molecules with a permanent dipole moment interacting with the electric field of a
charged wire (Sekatskii and Schmiedmayer, 1996).
II] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 267
FIG. 1. Guiding neutral atoms using a current carrying wire. (a) Guiding the atoms in their strong
.field seeking state as they circle around the wire. (b) Atoms in the weakfield seeking state can be
held in a 2-dimensional magnetic quadrupole field which is created by adding a constant bias field
to the wire field. Typical trajectories of atoms are shown on the right-hand side of the figure.
the atom takes the place of the "electron ". Considerable theoretical work has
been published on the quantum mechanical treatment of this system showing
a hydrogen-like energy spectrum (Pron'kov and Stroganov, 1977; Blfimel and
Dietrich, 1989, 1991; Voronin, 1991 ; Hau et al., 1995; Burke et al., 1996; Berg-
Sorensen et al., 1996) with a characteristic quantum defect (Schmiedmayer and
Scrinzi, 1996a,b).
The magnetic field, the potential, and typical classical trajectories are
presented in Fig. la.
r0 = ~-~)
{ ~to s
Bb
(3)
Around this line the modulus of the magnetic field increases in all directions and
forms a tube with a magnetic field minimum at its center. Atoms in the weak-
field seeking state can be trapped in this 2-dimensional quadrupole field and can
268 R. Folman et al. [II
| | |
| | | | | | |
Fie. 2. Upper left: potential for a side guide generated by one wire and an external bias field
perpendicular to the wire direction. The external bias field can be replaced by two extra wires (lower
left). Upper right: field configuration for a two-wire guide with an external bias field perpendicular
to the plane containing the wires. This external bias field may also be replaced by surface mounted
wires (lower right).
be guided along the side of the wire, i.e. in a side guide. At the center of the
trap the magnetic field gradient is
(4)
dr ro Iw ro
As long as the bias field is orthogonal to the wire, the two fields cancel exactly,
and trapped atoms can be lost due to Majorana transitions between trapped and
untrapped spin states (see Sect. V.A). This problem can be circumvented by
adding a small B-field component Bip along the wire direction which lifts the
energetic degeneracy between the trapped and untrapped states. This potential is
conventionally called a Ioffe-Pritchard trap (Gott et al., 1962; Pritchard, 1983;
Bagnato et al., 1987). At the same time, the potential form of the guide near the
minimum changes from linear to harmonic. The guide is then characterized by
the curvature in the transverse directions
where d is the distance between the two wires. When Bb > 2~Iw/Jrd, the field
from the wires is not capable of compensating the bias field. Two side guides
are then obtained, one along each wire in the plane of the wires.
In the case Bb < 2ltolw/:rd, the gradient in the confining directions is given
by dB r0
d r ro = --~ Iw d (8)
If there is a field component Bip along the wire, the position of the guide is
unchanged. However, the shape of the potential near its minimum is parabolic:
the curvature in the radial direction is given by
d2B
dr 2 r0 = BipI2 de. (91
In the special case of r0 = d/2, the gradient and, for the case of a non-vanishing
Bip, the curvature of the potential at the minimum position, are exactly equal to
the corresponding magnitudes for the single-wire guide.
FIG. 3. Atoms are guided in a two-wire guide that is self-sufficient without external bias fields.
Insets (a), (b) and (c) show the magnetic field contour lines for no bias, horizontal bias, and vertical
bias fields, respectively. Courtesy E. Cornell.
FIG. 4. Potential for a two-wire guide formed by copropagating currents. The plots show from
left to right the equipotential lines for increasing bias fields. As the field is raised, two (quadrupole)
minima approach each other in the vertical direction and merge at the characteristic bias field denoted
by B = 1 into a harmonic (hexapole) minimum. At higher bias fields this minimum splits into a
double (quadrupole) well again; this time the splitting occurs in the horizontal direction.
/
dsplit =
\
5-~)
Ito Iw
Bb
(lO)
one observes three different cases (Fig. 4): (i) If d/2 < dsplit, two minima are
created one above the other on the axis between the wires. In the limit of d
going to zero, the barrier potential between the two minima goes to infinity and
the minimum closer to the wire plane falls onto it; (ii) if d/2 = dsplit, the two
minima fuse into one, forming a harmonic guide; (iii) if d/2 > dsplit, t w o minima
are created, one above each wire. Splitting and recombination can be achieved
by simply increasing and lowering the bias field (Denschlag, 1998; Zokay and
Garraway, 2000; Hinds et al., 2001).
II] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 271
Table I
Typical potential parameters for wire guides, based on tested atom chip componentsa
Side guide b
Li 1000 80 2 5.4 25 32 100 120 > 1000
Li 500 200 10 13 5 400 570 50 > 1000
Li 200 400 30 27 1 4000 3300 21 7
Rb 1000 80 1 5.4 25 32 41 53 >1000
Rb 500 200 4 13 5 400 250 21 > 1000
Rb 200 400 20 27 1 4000 1100 10 > 1000
Rb 1000 2000 50 130 1 20000 3600 6 > 1000
a The parameters are given for the two different atoms lithium and rubidium, both assumed to be
in the (internal) ground state with the strongest confinement (F = 2, m F = 2). For both types
of guide, small bias-field components Bip pointing along the guide were added in order to get a
harmonic bottom of the potential and to enhance the trap life time that is limited by Majorana
spin flip transitions (see Eq. 18 in Sect. V). It was confirmed in a separate calculation that the
trap ground state is always small enough to fully lie in the harmonic region of the Ioffe-Pritchard
potential. See also Fig. 2.
b Side guide created by a thin current-carrying wire mounted on a surface with an added bias field
parallel to the surface but orthogonal to the wire.
c Two-wire guide created by two thin current-carrying wires mounted on a surface with an added
bias field orthogonal to the plane of the wires. In these examples the two wires are 10 ~tm apart.
currents and bias fields. The guided atoms are then located a few ~tm from the
wire (above the surface).
FIG. 5. Creating wire traps: The upper row shows the geometry of various trapping wires,
the currents and the bias fields. The lower column shows the corresponding radial and axial
trapping potential. (a) A straight wire on the axis of a quadrupole bias field creates a ring-shaped
3-dimensional non-zero trap minimum. (b) A "U"-shaped wire creates a field configuration similar
to a 3-dimensional quadrupole field with a zero in the trapping center. (c) For a "Z"-shaped wire a
Ioffe-Pritchard type trap is obtained.
II] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 273
A.4.2. Bent wire traps: the U- and Z-trap. 3-dimensional magnetic traps can be
created by bending the current-carrying wire of the side guide (Cassettari et al.,
1999; Reichel et al., 1999; Haase et al., 2001). The magnetic field from the bent
leads creates endcaps for the wire guide, confining the atoms along the central
part of the wire. The size of the trap along this axis is then given by the distance
between the endcaps. Here we describe two different geometries:
(1) Bending the wire into a "U"-shape (Fig. 5b) creates a magnetic field
that in combination with a homogeneous bias field forms a 3-dimensional
quadrupole trap 4. The geometry of the bent leads results in a field
configuration where a rotation of the bias field displaces the trap minimum
but the field always vanishes completely at this position.
(2) A magnetic field zero can be avoided by bending the wire ends to form a
"Z" (Fig. 5c). Here, one can find directions of the external bias field where
there are no zeros in the trapping potential, for example when the bias field is
parallel to the leads. This configuration creates a Ioffe-Pritchard type trap.
The potentials for the U- and the Z-trap scale similarly as for the side guide,
but the finite length of the central bar and the directions of the leads have to
be accounted for. Simple scaling laws only hold as long as the distance of the
trap from the central wire is small compared to the length of the central bar
(Cassettari et al., 1999; Reichel et al., 1999; Haase et al., 2001). Bending both
Z leads once more results in 3 parallel wires. This supplies the bias field for a
self-sufficient Z-trap.
4 The minimum of the U-trap is displaced from the central point of the bar, in a direction opposite
to the bent wire leads. A more symmetric quadrupole can be created by using 3 wires in an
H configuration. There the side guide is closed by the two parallel wires crossing the central wire
orthogonally. The trap is then in between the two wires, along the side guide wire.
274 R. Folman et al. [II
Flo. 6. Two geometries of crossed-wire traps: different cuts through the potential are displayed
without and with a longitudinal bias field component in the left and right column, respectively. The
1-dimensional plots show the potential along the direction of the side guide; in the contour plots
the wire configuration is illustrated by light gray bars. Courtesy J. Reichel.
Even more elaborate designs for traps than those described previously can be
envisioned. For example, Weinstein and Libbrecht (1995) describe planar current
geometries for constructing microscopic magnetic traps (multipole traps, Ioffe-
Pritchard traps and dynamical traps). We focus here on the Ioffe-Pritchard trap
proposals. Figure 7 shows four possible geometries: (a) three concentric half
loops; (b) two half loops with an external bias field; (c) one half loop, one full
loop and a bias field; (d) two full loops with a bias field and external Ioffe
II] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 275
a) 111 b) I1
111 1!
cl 111 d]
| |
| |
111
FIG. 7. Four planar (and pseudoplanar) Ioffe trap configurations, as described in the text. Courtesy
J. Weinstein/K. Libbrecht.
bars. The first of these (a) is essentially a planar analog of the nonplanar Ioffe-
Pritchard trap with two loops and four bars. Configuration (b) replaces one of the
loops with a bias field. Configuration (c) is similar to (b) but provides a steeper
trapping potential on-axis and weaker trapping in the perpendicular directions;
this makes an overall deeper trap with greater energy-level splitting for given
current and size. (d) is a hybrid configuration, which uses external (macroscopic)
|offe bars to produce the 2-dimensional quadrupole field, while deriving the on-
axis trapping fields from two loops and a bias field. Typical energy splittings
in the range of 1 MHz are achievable using experimentally realistic parameters
(Drndi6 et al., 1998).
A. 7. Moving potentials
Introducing time-dependent potentials facilitates arbitrary movement of atoms
from one location to another. There are different proposals for possible
276 R. Folman et al. [II
Yl
IH2
FIG. 8. Magnetic 'conveyor belt': The wires are configured in a way that allows to transport atoms
from one trap to another along a side guide. Together with a homogeneous time-independent bias
field, the currents IQ, IH1, and /H2 are used for the confining fields of the source and collecting
traps, I0 is the current through the side guide wire. The currents IM1 and IM2 alternate sinusoidally
with a phase difference of Jr/2 and provide the moving potential. Courtesy J. Reichel.
A. 8. Beam splitters
By combining two of the guides described above, it is possible to design
potentials where at some point two different paths are available for the atom.
This can be realized using different configurations (examples are shown in Fig. 9)
some of which have already been demonstrated experimentally (see Sect. IV).
5 The Y-configuration has been studied in quantum electronics by Palm and Thyl6n (1992) and
Wesstr6m (1999).
II] M I C R O S C O P I C ATOM OPTICS: F R O M WIRES TO ATOM CHIP 277
FIG. 9. Different wire geometries for a beam splitting potential: The plots show the wire
arrangement on the surface of an atom chip, and the directions of current flow and the additional bias
field. Each picture also shows a typical equipotential surface to illustrate the shape of the resulting
potential. (a) A simple Y-beam splitter consisting of a single wire that is split into two: The output
side guides are tighter and closer to the surface than the input guide. Note that a second minimum
closer to the chip surface occurs in the region between the wire splitting and the actual split point
of the potential; (b) a two-wire guide split into two single-wire guides does not exhibit this 'loss
channel'. (c) Here, the output guides have the same characteristics as the input guide, minimizing
the backscattered amplitude. The vertical orientation of the bias field ensures exact symmetry of
the two output guides. (d) In an X-shaped wire pattern the splitting occurs because of tunneling
between two side guides in the region of close approach of the two wires.
incoming and outgoing wires lead to a change o f field strength at the guide
minimum and can cause backscattering from the splitting point. (2) In the Ioffe-
Pritchard configuration (i.e. with an added longitudinal bias field), the splitting
is not fully symmetric due to different angles of the outgoing guides relative to
the bias field. (3) A fourth guide leads from the splitting point to the wire plane,
i.e. to the surface of the chip.
The backscattering and the inaccessible fourth guide o f the Y-beam splitter
may be overcome, at least partially, by using different beam splitter designs,
like those shown in Fig. 9b,c. The configuration in Fig. 9b has two wires which
run parallel up to a given point and then separate. If the bias field is chosen
so that the height of the incoming guide is equal to the half distance d/2 o f
the wires (d/2 = dsplit as defined in Eq. 10 in Sect. II.A.3), the height o f the
potential m i n i m u m above the chip surface is maintained throughout the device
(in the limit of a small opening angle) and no fourth port appears in the splitting
region. The remaining problem o f the possible reflections from the potential in
the splitting region can be overcome by the design presented in Fig. 9c. Here, a
guide is realized with two parallel wires with currents in opposite directions and
a bias field perpendicular to the plane of the wires. This type of design creates a
truly symmetric beam splitter where input and output guides have fully identical
characteristics.
278 R. Folman et al. [II
A.9. Interferometers
FIG. 10. Basic properties of the guided matter wave interferometer: (a) Two Y-beam splitters are
joined together to form the interferometer. (b) Transverse eigenfunctions of the guiding potentials
in various places along the first beam splitter. When the two outgoing guides are separated far
enough, i.e. no tunnelling between left and right occurs, the symmetric and antisymmetric states
become degenerate. (c) Energy eigenvalues for the lowest transverse modes as they evolve along the
interferometer. One clearly sees that pairs of transverse eigenstates form disjunct interferometers.
(d) The wavefunction of a cold atom cloud starts out in the vibrational ground state of a guide or
trap. The wavefunction splits when the guide divides, leaving a part of the wavefunction in each
arm of the interferometer. If the phases of the two parts evolve identically on each side, then the
original ground state is recovered when the two parts of the wavefunction are recombined. But if a
phase difference of Jr accumulates between the two parts (for example due to different gravitational
fields acting on them), then recombination generates the first excited state of the guide with a node
in the center. Courtesy E. Hinds. (e) 2-dimensional plots of a wave packet propagating through a
guided matter wave interferometer for 10) and 11) incoming transverse modes, calculated by solving
the time-dependent Schr6dinger equation in two spatial dimensions (x, z, t) for realistic guiding
potentials, where z is the longitudinal propagation axis. The probability density of the wave function
just before entering, right after exiting the interferometer, and after a rephasing time t are shown
for a phase shift of ~ . One clearly sees the separation of the two outgoing packets due to the
energy conservation in the guide, e.g. for n = 0 the first excited outgoing state is slower than the
ground state.
280 R. Folman et al. [II
2-dimensional geometry 6 are depicted in Fig. 10c. From the transverse mode
structure one can see that there are many disjunct interferometers in Fock space.
Each of them has two transverse input modes (]2n) and [2n + 1), n being the
energy quantum number of the harmonic oscillator) and two output modes. In
between the two Y-beam splitters, the waves propagate in a superposition o f
]n)l and ]n)r in the left and right arm, respectively. With adiabaticity fulfilled,
the disjunct interferometers are identical.
Considering any one of these interferometers, an incoming transverse state
evolves after the interferometer into a superposition o f the same and the
neighboring transverse outgoing state (Fig. 10c), depending on the phase
difference acquired between [n)l and In)r during the spatial separation o f the
wave function 7. While the propagation remains unchanged if the emerging
transverse state is the same as the incoming state, a transverse excitation
or de-excitation translates into an altered longitudinal propagation velocity
(Ao _~ +oo/k where hk is the m o m e n t u m o f a wave packet moving through
the interferometer and to/2:r is the transverse trapping frequency), since
transverse oscillation energy is transferred to longitudinal kinetic energy, and
vice versa.
As presented in Fig. 10e, integrating over the transverse coordinate results in a
longitudinal interference pattern observable as an atomic density modulation. As
all interferometers are identical, an incoherent sum over the interference patterns
of all interferometers does not smear out the visibility of the fringes.
A.9.2. Interferometers in the time domain. Two different proposals are based
on time-dependent potentials (Hinds et al., 2001 ; Hfinsel et al., 2001c). These
proposals differ from the interferometer in the spatial domain in several ways:
(1) The adiabaticity of the process may be controlled to a better extent due to
easier variation of the splitting and recombination time. (2) The interferometers
are based on a population of only the ground state. (3) The interference signal
amounts to different transverse state populations in the recombined single
minimum trap, whereas the above proposal anticipates a spatial interference
pattern which may be easier to detect.
The first proposal (Hinds et al., 2001) is based on a two parallel wire
configuration with co-propagating currents (see Sect. II.A.3). Changing the bias
field in this configuration as a function of time produces cases (i), (ii), and (iii)
discussed in Sect. II.A.3 depending on the strength of the bias field as compared
6 In 2-dimensional confinement the out of plane transverse dimension is either subject to a much
stronger confinement or can be separated out. For experimental realization see Gauck et al. (1998),
Spreeuw et al. (2000), Hinds et al. (2001), Pfau (2001).
7 The relative phase shift Aq~between the two spatial arms of the interferometer can be introduced
by a path length difference or by adjusting the potentials to be slightly different in the two arms. In
general, Ar is a function of the longitudinal momentum k.
II] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 281
B, G
(a) (b)
/ ~ 2so
200
150
100
50
Z, m
0.5 1 1.5 2 2.5 3 3.5
I B, G
25o~ (c)
X
0.5 1 1.5 2
FIc. 11. (a) Two pairs of differently sized magnetic sheets (bottom) are magnetized using
current-carrying wires wound around them. The choice of the direction of current flow in these
wires establishes the direction of magnetization: the arrows show a possible configuration for which
the equipotential lines are plotted (top). (b) The field produced by the sheet pairs measured in the
symmetry plane. (c) Scaling of the field due to the combined inner and outer pair of sheets in the
plane of symmetry. Courtesy M. Prentiss.
B. ELECTRIC INTERACTION
1 ) 2 2aq2
Vp~ = - 4n'e0 r2 (12)
is attractive. It has exactly the same radial form ( 1/r 2) as the centrifugal potential
barrier (VL = LZ/2Mr 2) created by an angular momentum Lz. VL is repulsive. The
total Hamiltonian for the radial motion is
12 - "" 60 2101
8 56- 206
6 "
; . ~
54 It" 204
0 48 ' 198
0 1i 2, 3i 4i 5 25 21 6 2 1 7 2I8 2t9 30 ,
100 ,
101 ,
102 ,
103 ,
104 105
Line charge q in units of mcrit
FIG. 12. Theoretical absorption cross section for a charged wire. The calculations are made for
several different relative thicknesses (kRw) of the wire; the charge is given in units of the angular
momentum mcrit = Lcrit/h.
where A and B are constants that depend on specifics of the optical fiber as
well as on light power, wavelength and atomic properties (Batelaan et al., 1994).
K0 is the modified Bessel function of the second kind. Figure 13 shows a typical
example of such a potential. Cold atoms are bound in radial direction by the
effective potential but free along the z-direction, the direction of the charged
optical fiber.
2 ~ T 1
g o
~ -2 -
FIG. 13. Typical radial potential for a neutral lithium atom trapped around a charged (5 V) optical
quartz fiber (diameter 0.5 ~tm) with 1-mW light and a detuning of A/F = 3 • 105. The attractive
potential (1/r 2) is created by the interaction of the induced dipole moment with the electric field of
the charged fiber. The repulsion is due to the evanescent wave from blue-detuned light propagating
in the fiber. Close to the wire surface the Van der Waals interaction becomes important.
286 R. Folman et al. [II
Vguid(r)=Vm(Z)--( 1 ) 22~
4;re0 r2 , (16)
where z is the height above the mirror and r the distance from the wire. This
creates a potential tube for the atoms as shown in Fig. 14 which can be viewed
as a wave guide for neutral atoms.
Typical parameters for guides f o r m e d by a magnetic mirror and a charged wire
are given by Schmiedmayer (1998). They can be very similar to the magnetic
guides discussed in Sect. II.A. Using typical mirror parameters (Roach et al.,
1995; Sidorov et al., 1996), one can easily achieve deep and narrow guides with
transverse level spacings in the kHz range for both light (Li) and heavy (Rb)
atoms.
In a similar fashion microscopic traps can be created by mounting a charged
tip (point) at or close beneath the atom mirror surface. A point charge on the
surface o f an atom mirror creates an attractive 1/r 4 interaction potential:
1 ) 2aq 2
Vpol(r) = - 8yt60 r4 (17)
where q is the tip charge. Together with the atomic mirror it forms a microscopic
cell for the atoms. It can be viewed as the atom-optical analog to a quantum dot
(Schmiedmayer, 1998; Sekatskii et al., 2001).
This approach o f combining a charged structure with an atom mirror is
compatible with well-developed nanofabrication techniques. This opens up
8 There are two main types of atom mirrors: The first type utilizes evanescent waves (e.g. above
the surface of a reflecting prism) of blue-detuned light which repels the atoms. Here the potential
takes the form Vm(z) = VOexp(-tCmZ) where trm is of the order of the light wave number and z is
the distance from the mirror (Cook and Hill, 1982). The second type is based on a surface with
alternating magnetic fields. Here, ~ = 2;r/lcm is the periodicity of the alternating magnetic field.
The approaching atom experiences an exponentially increasing field, and consequently the weak-
field seekers are repelled (Opat et al., 1992; Roach et al., 1995; Sidorov et al., 1996; Hinds and
Hughes, 1999).
II] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 287
10 // - - ,
.Eo. 5 _ .
/'-'\ 1 -
-
-10 _ "~ _
-50 0 50 [! ' . . . . ]
potential [ne_V]50~ 1
=X -5 __...~
/'i......
5 10 15 20 25 30
distance from mirror [gm]
Flo. 14. Typical potential for a neutral atom guide. The attractive potential (1/r 2) is created by the
interaction of the induced dipole moment in the electric field of the charged wire mounted directly
on the surface of an atomic mirror. The action of the atomic mirror (evanescent wave or magnetic
mirror) prevents the atom from reaching the surface and creates a potential tube close to the surface
illustrated by the contour graph. The two adjacent plots give the potential in a direction orthogonal
to the charged wire and orthogonal to the mirror surface. Distances are given from the location of
the charged wire and the surface of the atom mirror.
FIG. 15. State-dependent potential: (a) top view of an actual chip design; the wire in the center
is used as a side guide wire, the additional electrodes create a spatially oscillating electric field
providing confinement also along the wire. The contour plot shows a typical potential configuration
for 7Li a t o m s in the IF = 2, m F = 2) magnetic substate using experimentally accessible parameters.
Dark areas correspond to attractive potentials, the trap minima are located 50 gm above the surface.
(b,c) The side views show that only one state (IF = 2, m F = 2)) is trapped in the combined
potential (b), while the other (IF = 1, m F = - 1 ) ) is not, because the weaker magnetic barrier to the
surface is compensated by the attractive electric potential (c). The parameters used in a simulation
with the electromagnetic field solver MAFIA were lw = 500 mA, B b = 20 G for the side guide and
a voltage of 600 V on the electrodes.
C.3. The e l e c t r i c m o t o r
FIG. 16. Two-wire guide configuration with currents of 1 A running in opposite directions with a
vertical bias field of 150 G. The combined magnetic and electric potential is shown in contour plots
perpendicular to the wire and along the wire at the minimum height (inset). The parabolic potential
shape offers the possibility to drive the atoms (87Rb) along the wire. In the example, the voltages
applied to the wires are chosen to be 0 V with respect to ground in the wire center.
can be neglected. However, for micron-sized wires, one finds that if the current-
carrying wire becomes long, at some point the voltage is strong enough to create
a significant driving force for the atoms or even to destroy the traps.
On the other hand, one can actually exploit this effect and turn it into an
'electric motor' by using the electric potential gradient inside the magnetic
minimum to accelerate and decelerate the atoms at will. Figure 16 illustrates
the mechanism used for the motor for the example of a two-wire guide with a
vertical bias field. The wires carry counter-propagating currents, and the electric
interaction is zero in the middle of the guide (see inset) where both wires have
the same voltage. By adding a homogeneous electric potential relative to ground,
the zero electric field point may be moved at will to achieve any acceleration or
deceleration rate. A constant acceleration is obtained when the zero electric field
point is maintained at a constant distance from the position of the atoms.
To achieve very robust and highly controlled atom manipulation one would like
to localize atoms in steep traps or guides which can be fabricated with high
precision. The large technological advances in precise nanofabrication, with the
290 R. Folman et al. [II
achievable size limit on chips smaller than 100 nm, makes the adaptation of these
processes for mounting the wires onto surfaces very attractive.
D. 1. Miniaturization
The formulae presented in Sects. II.A to II.C are exact only for infinitely small
wire cross sections. In the case of a physical wire with a finite cross section,
they are a good approximation only as long as the height above the wire is
greater than the width of the wire. For experiments requiring a trap height smaller
than the width of the wire, finite size effects have to be taken into account. In
Fig. 17, we present examples of calculations showing how the trap gradient is
limited by finite size wires. One clearly sees that at trap heights of the order of
the width of the wire the resulting gradient starts to deviate from the expected
value. The effect is small for wires with a square cross section, while it becomes
considerably more important when rectangular wires with high ratios of width
to thickness are used.
The Van der Waals interaction becomes important at distances of the order
of a few 100nm from the surface. The interaction can be strong enough to
II] M I C R O S C O P I C ATOM OPTICS: F R O M W I R E S TO ATOM CHIP 291
0 30 , lar
025
0 20
-- 015
82
0 05
, i , i
1 2 3 4
FIG. l 7. Deviations from the field of an infinitely thin wire become important as the surface of
a physical wire is approached. The plot shows the trap gradient for a side guide (see Sect. II.A.2)
when differently shaped wires are used. The solid line corresponds to a circular cross section as a
reference since the field outside the wire equals that of an infinitely thin wire at the wire center.
A wire with a square cross section (dotted line) shows very small deviations, while broad and thin
wires (dashed lines) deviate more and more as the thickness/width ratio decreases. Here, all wires
are chosen to have the same cross section d 2. Therefore, the widths of the rectangular wires are
2d and x/]--dd = 3.2d for the ratios 1:4 and 1:10, respectively.
significantly alter the trapping potentials (Grimm et al., 2000). Traps much
closer than 100 nm from the surface will be very hard to achieve since the Van
der Waals potential attracts the atoms to the surface and increases with 1/d 3
(in the non-retarded regime where the distance d is smaller than the optical
wavelength).
D. 4. Current densities
A limiting factor in creating steep traps and guides is the maximally tolerable
current density of a current-carrying structure. Considering a side guide potential
created by a wire with finite width d and a constant thickness, the highest
possible gradient is achieved at a distance from the wire comparable with d. The
bias field needed for such a trap is given by the ratio of the m a x i m u m current
that can be pushed through the wire and d; therefore the bias field is proportional
to the m a x i m u m current density j. This leads to the conclusion that the highest
possible gradient is given by j / d which favors smaller wires. If a square wire
cross section d 2 is assumed, the m a x i m u m gradient is proportional to j . Even in
this case, smaller d will allow for larger gradients b e c a u s e j has been observed to
increase with smaller wire cross sections. The drive for smaller width is stopped
292 R. Folman et al. [III
The basic principles of microscopic atom optics have been demonstrated using
free-standing structures: current-carrying and charged wires. The interaction
potentials are in general shallow, typically only a few mK deep. Hence
experiments use cold atoms from a MOT or a well collimated atom beam
(even the moderate collimation of 1 mm over 1 m results in a typical transverse
temperature of <1 mK).
Free-standing wire structures can be installed close to a standard six beam
MOT without significantly disturbing its operation (as long as the wire is thin
enough), and offer large optical access which has advantages when probing the
dynamics of the atoms and their spatial distribution within the wire potentials.
They have the disadvantages that they are not very sturdy, they deform easily
due to external forces, and they cannot be cooled efficiently to dissipate energy
from ohmic heating. This limits the achievable confinement and the potential
complexity of wire networks. Nevertheless there are some special potentials
which can only be realized with free-standing wires.
A. MAGNETIC INTERACTION
As discussed in Sect. II.A there are two possibilities for magnetically trapping a
particle with a magnetic moment: traps for strong field seekers and traps for
weak field seekers. In the following we describe experiments with magnetic
microtraps which are based on small, free-standing wires or other magnetic
structures. Typical wire sizes range from 10 ~tm to a few mm and the wires
carry electrical currents of up to 20 A. All experiments but the first example
start with a conventional MOT of alkali atoms (lithium or rubidium) which is
initially situated a few mm away from the magnetic field producing structures.
This distance prevents the atoms in the MOT from coming into contact with the
III] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 293
structure surface where they would be adsorbed. It also provides the necessary
optical access for the MOT laser beams.
To load the magnetic wire traps and guides, the MOT laser light is simply
switched off and the magnetic trap fields are turned on. The loading rate into the
miniature magnetic traps has been enhanced in some experiments (a) by optically
pumping the unpolarized MOT atoms to the right trapping state (Key et al.,
2000); (b) by first loading the MOT atoms in a size-matched magnetic trap which
is then further adiabatically compressed (Vuletic et al., 1996, 1998; Key et al.,
2000; Fortagh et al., 1998; Haase et al., 2001); (c) by moving the MOT closer
to the trapping region shortly before the light is turned off, which can be done
with an additional magnetic bias field (Denschlag et al., 1999b). In this way the
efficiency of transferring the atoms into the miniature magnetic traps reached
between 1 and 40 %. In general the spatial distribution of the trapped atoms was
imaged with a CCD camera by shining a resonant laser beam onto the atoms and
detecting its absorption or the atomic fluorescence.
FIG. 18. (a) Experimental setup: The schematics at the bottom show in detail the relative geometric
arrangement between the apertures, the movable beam shutter used to bend the wire, and how the
wire is mounted. (b) Guiding of Na atoms along the 1-m long, 150-~tm diameter tungsten wire
(at detector position 0 indicated by the vertical line). Experimental count rates, n(I)- n(O) (left),
and Monte Carlo simulations (right), are shown for 0.0, 0.50 and 1.00mrad bends in the wire.
The different symbols represent currents of 0.5 A (circles), 1.0 A (diamonds), 1.5 A (crosses) and
2.0 A (triangles) through the wire. The thick line shows the fraction of atoms of the direct beam
that gets to the detector when no current is on (right-hand vertical axis). Its form corresponds to
the shadow of the bender that is cast onto the detector.
Fig. 19). For long guiding times the bound atoms leave the field of view, and the
fluorescence signal of the atoms decreases. The top left view images of Fig. 19
show a round atom cloud that is centered on the wire suggesting that atoms circle
around it.
By studying the ballistic expansion of the bound atoms after switching off
the guiding potentials, the m o m e n t u m distribution of the guided atoms can be
extracted. The center panel of Fig. 19 shows a picture sequence demonstrating
how the atomic cloud expands as a function of time. Starting from a well-
localized cylindrical cloud of guided atoms at t = 0 the spatial atomic distribution
transforms into a doughnut-like shape. This shows that there are no zero-velocity
atoms in the Kepler guide. In order to be trapped in stable orbits around the wire
the atoms need sufficient angular m o m e n t u m and therefore velocity. Atoms with
too little angular m o m e n t u m hit the wire and are lost.
Guiding in the Kepler guide is very sensitive to the presence of uncompensated
bias fields. Such additional magnetic bias fields, even if homogeneous, destroy
the rotational symmetry of the Kepler potential and angular m o m e n t u m is
not conserved anymore. Over the course of time, the Kepler orbits become
increasingly eccentric and thus finally hit the current-carrying wire leading to
loss, which was confirmed by Monte Carlo calculations. The right-hand panel
of Fig. 19 shows the results of an experiment investigating the dependence of the
III] M I C R O S C O P I C ATOM OPTICS: FROM WIRES TO ATOM CHIP 295
FIG. 19. Left: guiding of atoms along a current-carrying wire in their strong field seeking state
(Kepler guide). Pictures of the atomic clouds are shown, taken in axial and transverse directions with
respect to the wire. For times shorter than 15 ms the expanding cloud of untrapped atoms is also
visible. The location of the wire is indicated by a line (dot). The pictures show a 2-cm long section
of the wire that is illuminated by the laser beams. Center: Atomic distribution after free expansion
of 0 to 9 ms for atoms that have been guided in Kepler orbits around the wire. The expanded cloud
is doughnut-shaped due to the orbital motion of the atoms around the wire. Right: Experimentally
measured stability of the Kepler guide as a function of the magnitude of bias fields. The signal is
proportional to the number of atoms trapped in the guide after an interaction time of 20 ms.
magnetic trap stability on the magnetic bias field. The remaining atom number in
the Kepler guide was measured after 20 ms interaction time. It clearly decreases
with increasing bias field strength: the larger the bias field, the faster the atoms
get lost (Denschlag, 1998). In case of a weak disturbance the orbits can be
stabilized by an additional 1/r 2 potential which leads to a precession of the
orbits.
FIG. 20. Three realizations of magnetic quadrupole traps with straight wires. (a) Trap realized
by Fortagh et al. (1998) with a thin wire (50~tm) glued onto a thick wire (1 mm). The current
through both wires flows in opposite directions. (b) A homogeneous bias field is combined with
a single straight wire (Denschlag, 1998; Denschlag et al., 1999b). (c) Four wires with alternating
current direction produce a quadrupole field minimum in the center. In the experiment the four wires
were embedded in a silica fiber (Key et al., 2000). (d) Images of atoms in guide (b).
FIG. 21. Atomic beam switch for guided atoms using a "Y"-shaped current-carrying wire. By
controlling the current through the arms, one can send cold lithium atoms along either arm or split
the beam in two. The images here show the switch operated in the Kepler guide mode and the
"weak-field-seeker" mode.
Experiments with free-standing wires that are bent in shape of a "U" or "Z" have
been reported by Denschlag et al. (1999a), Haase (2000) and Haase et al. (2001).
Bending the wire has the effect of putting potential endcaps on the wire guide,
which turns it into a 3-dimensional weak-field-seeker trap (see Sect. II.A.4.2).
A simple Z-wire trap achieves trapping parameters similar to the ones currently
used in BEC production, here, however, with moderate currents and very low
power consumption (see Sect. IV.C.4). In their experiment, Haase et al. used
a 1-mm thick copper wire, with the central bar being about 6 mm long. The
wire can carry 25 A without any sign of heating. Figure 22c shows the scaling
298 R. Folman et al. [III
FIG. 22. (a) Schematic description of the experiment. Camera 1 is looking along the central bar
of the magnetic trap and camera 2 along the leads. In addition to the two laser beams shown in the
figure, there is the third MOT beam parallel to the central bar. (b) The Z-wire held by two Macor
blocks is mounted on a flange. (c) The cloud of trapped atoms monitored by camera 1. By changing
the bias field Bb from 5 to 52 G, the trap size and position change. Also, the trap frequency increases
from 30 to 1600Hz. The experiment confirms the predicted scaling laws concerning trap distance,
frequency and bias field.
properties of the Z-trap. The atomic cloud can be compressed by raising the bias
field or by lowering the wire current.
J .................
. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .J. . . / / / x ~ 8 ~ .... J 3"105
2.105
..~ ~p. 21 mm mm
] lCm 1.101t
I ~1" I=- permanentmagnet
J with steelpin -2 ' (~ " :~ ' ~, " 6 ' 8 " 1()' 1'2' 1 ' 4 ' 1 6
distance of light sheet from pin tip [ram]
FIG. 23. Left: Setup of the tip trap ofVuletic e t a l . . A sharp steel pin is magnetized by a permanent
magnet and exposed to a variable magnetic field that is generated by two electromagnets. Right:
Observed shape of the atomic cloud (a) in the shallow field after loading from a magneto-optical
trap and (b) after compression in the steep potential of the tip trap at a current in the tip coil of
1.2 A. Courtesy V. Vuletic.
factor of 6.5 within 100 ms. A total of 3% of the MOT atoms could be transferred
to the microtrap at moderate currents of 3 A through the tip trap coils.
30 i , ,-, , 9 , , , 9 , , , 9 , 9 , 9 ,, , , ' |
20 ~
..l'..
trap 4
v ent into page)
~= o
~5 - l o
~ 20
30 ,,m mF - ". .
-40
-8 -6 .4 -2 0 2 4 s 8 10 12 14
horizontal distance (mm)
FIG. 24. Computer simulation of trajectories of cesium atoms deflected by the magnetic field from
a wire carrying 20 A. The solid lines indicate the trajectories for atoms in the nine possible magnetic
substates, assuming zero initial velocity. The broken lines are for atoms in the m F = + F substates
with initial transverse velocities of-t-1 cm/s. Courtesy P. Hannaford.
300 R. Folman et al. [III
With currents of up to 45 A through the wire, the positions of the atoms in the
individual magnetic substates are resolved and deflection angles as large as 25 ~
are observed. State preparation of the atoms using optical pumping increases the
number of atoms deflected through essentially the same angle.
Very recently Sauer et al. (2001) have demonstrated a storage ring for neutral
atoms using a two-wire guide (Sect. II.A.3). A pair of wires (separation-840 gm)
which forms a ring of 2cm diameter, produces a 2-dimensional quadrupole
magnetic field (see Fig. 25). The wires carry currents of 8 A in the same direction
which produces a field minimum between the two wires with a field gradient
of 1800 G/cm and a trap depth of 2.5 mK for the F = 1, mF = -1 ground
state of 87Rb (weak-field seeker). The ring is loaded from a MOT via a similar
second two-wire waveguide. The MOT is turned off and the second waveguide is
ramped up in 5 ms. Approximately 106 laser-cooled rubidium atoms (longitudinal
temperature 3 ~tK) fall 4 cm under gravity along the guide after which they enter
the storage ring with a velocity of about 1 m/s. To transfer the atoms to the ring,
the current in the guide is ramped off while simultaneously increasing the current
in the ring. Using fluorescence imaging the position and the number of the atom
cloud can be probed. Up to seven revolutions of the atoms in the ring have been
observed.
FIG. 25. (a) Schematic of the storage ring. (b) Cross section of the overlap region. The trap
minimum is shifted from between the guide wires to the ring wires by adjusting the current.
(c) Contour plot of a two-wire potential. The contours are drawn every 0.5 mK for the wire distance
d = 0.84mm and I = 8 A. (d) Successive revolutions in the storage ring. The points represent
experimental data, the curve is a theoretical model. Courtesy M. Chapman.
Two types of experiments have used the 1/r 2 potential (Eq. 12) of a charged
III] M I C R O S C O P I C ATOM OPTICS: FROM WIRES TO ATOM CHIP 301
wire. One investigated the effect of a charged wire in atom interferometry. The
other investigated atomic motion in the singularity of the 1/r 2 potential. Here,
laser cooled atoms fall into the attractive singularity and are lost as they hit the
charged wire.
Shimizu et al. (1992) used a straight charged wire to shift (deflect) the
interference patterns of a matter wave interferometer in a Young's double slit
configuration. In a recent experiment of the same group (Fujita et al., 2000)
(Fig. 26, at right), this work is expanded by combining a binary matter wave
FIG. 26. Experimental set-ups and data for interferometry and holography experiments with
charged wires. Left: charged-wire interferometerfor metastable helium. Different voltages applied to
the electrodes: the data sets are plotted with a vertical offset. The dotted horizontal lines indicate the
zero level for the respective measurements. Courtesy J. Mlynek. Right: Selective atom holography:
switching between atomic images "r and "~". For the upper figure the wire array is uncharged,
whereas for the lower figure it is electrically charged. The squares in the lower part of each figure
are nondiffracted atom patterns. Courtesy E Shimizu.
9 Similarly it was suggested by Ekstrom et al. (1992) that charged patches on a grating can be used
to modify the diffraction properties.
302 R. Folman et al. [III
FIG. 27. (a) Two classical trajectories: An atom falls into the 1/r2 singularity of an electrically
charged wire if the atomic angular momentum Lz < Lcrit. If Lz > Lcrit it scatters and escapes from
the singularity. (b) When moved onto the wire the atom trap decays exponentially, as can be seen
by monitoring the atomic fluorescence signal. Charging the wire (100 V ~ 6.4 pC/cm) creates an
attractive 1/r2 potential and enhances the decay rate. Inset: experimental steps. Loading of the trap,
shifting it onto the wire and observing its decay. (c) Dependence of the trap decay rates on the wire
charge for different wire thicknesses. The decay rate for uncharged wires is proportional to their
actual diameters. For increasing charges the absorption rate becomes a linear function of the charge,
a characteristic of the 1/r2 singularity. The slope is independent of the wire diameter.
a terminal. The width and the spacing of each wire was 0.5 ~tm and the holes for
the binary hologram in between the wires were 0.5 ~tm • 0.5 ~tm in size. The
electric field E generated between two wires shifted the energy of the neon atom
b y - o t E 2 / 2 . When two adjacent electrodes had the same potential, the atoms in
the gap were unaffected. If they had different potentials, the atoms accumulated
an additional phase while passing through the hole.
In an experiment in Konstanz, Nowak et al. (1998) sent a collimated thermal
beam of metastable helium atoms onto a charged wire (tungsten, 4 ~tm diameter)
where it was diffracted (see Fig. 26, left). 1.3 m further downstream they
observed an interferometric fringe pattern which depended on the wire charge
and on the de Broglie wavelength. The data agreed well with the theoretical
predictions for scattering polarizable particles off a 1/r 2 potential.
The motion in a 1/r 2 singularity can be studied by placing a cloud of cold atoms
in the potential of a charged wire. In this experiment the n u m b e r of cold lithium
atoms of a M O T is monitored while the atoms move in the 1/r 2 potential of the
wire (Denschlag et al., 1998). At extremely low light levels the M O T acts as a
box holding a gas o f atoms. Atoms falling into the attractive 1/r 2 singularity are
lost as they hit the wire. This loss m e c h a n i s m leads to an exponential decay of
the trapped atom n u m b e r (see Fig. 27b).
The corresponding loss rate is characteristic for the 1/r 2 singularity and its
IV] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 303
strength. Atoms with angular momentum Lz < Lcrit (see Eq. (14) in Sect. II.B)
fall into the singularity. The loss rate is a linear function of q because Lcrit is
proportional to the line charge q and the atoms are uniformly distributed over
angular momentum states (see Fig. 27c). This is actually true only for high
charges, since for lower q, the finite thickness of the charged wire becomes
apparent. The MOT decay rate for an uncharged wire is proportional to its actual
diameter. The radii of the wires in the experiments ranged between 0.7 ~tm and
5 ~tm. A detailed analysis of the absorption data reveals that Van der Waals forces
also contribute to the atomic absorption rate (Denschlag, 1998). This effect was
found to be important for thin wires with diameters of less than 1 ~tm. Hence
this system should allow for detailed future studies of Van der Waals interaction
and retardation in nontrivial boundary conditions.
The 1/r 2 potential would be especially interesting to study in the quantum
regime where the de Broglie wavelength of the atoms is much larger than the di-
ameter of the charged wire; the quantization of angular momentum then begins to
play a role (Denschlag and Schmiedmayer, 1997). This can be used for example
in order to build an angular momentum filter for atoms (Schmiedmayer, 1995a).
In the following we describe the atom chip and its present experimental status.
Future goals will be addressed in Sect. VI.
A. FABRICATION
FIG. 28. Electroplating. Left: cross section of the Munich-group chip. The metallic layer on top of
the wires gives the chip enhanced surface quality in order to form a mirror MOT. Right: the layout
of the chip. The magnetic 'conveyor belt' explained in Sect. II is visible. The wires are connected
to the chip pads from the outside by means of wire bonding. Recently, this chip was used to achieve
Bose-Einstein condensation. Courtesy J. Reichel.
reflection layer (e.g. the Munich chip as shown in Fig. 28) (Reichel et al., 2001).
This, however, carries the price of not enabling atoms to be closer than some
20 gm from the wires themselves. A technical advantage of electroplating is that
it wastes less gold or copper because one avoids evaporation of large amounts
of metal, which mostly cover the evaporation chamber and not the chip.
Atom chips fabricated using using this technique have been used sucessfully
by the groups at Harvard (M. Prentiss), Munich (J. Reichel and T.W. HS.nsch),
JILA, Boulder (D. Anderson and E. Cornell) and Ttibingen (C. Zimmermann).
A.2. Nanofabrication
Atom chip structures can also be fabricated into an evaporated conductive layer
with state-of-the-art processes used for electronic chips. To the best of our
knowledge, this approach is only used by the Heidelberg (formerly Innsbruck)
group. In these atom chips a 1-5 gm gold layer is evaporated onto a 0.6-mm
thick semiconductor substrate (GaAs or Si). As GaAs or Si tend to leak currents,
especially in the presence of light, a thin isolating layer of SiO2 is put between
the substrate and the gold layer. The chip wires are defined by 2-10 gm wide
grooves from which the conductive gold has been removed. This leaves the chip
as a gold mirror that can be used to reflect MOT laser beams (the 10-gm grooves
impede the MOT operation only in a very slight way). The mirror surface quality
is very high, achieving an extremely low amount of scattered light. The chips
were produced at the microfabrication centers of the Technische UniversitS, t Wien
and of the Weizmann Institute of Science, Rehovot, see Fig. 29.
Atom chips fabricated with this method have the advantage that the structure
size is only limited by nanofabrication (<100nm). The drawback is that the
conductive layer cannot be too thick. This is due mainly to restrictions on the
available thickness of the photoresist used in the process. The thin wires support
only smaller currents, and therefore only smaller traps closer to the surface can
306 R. Folman et al. [IV
FIG. 29. Nanofabricated atom chips (Heidelberg). Left: a mounted chip, ready to be put into the
vacuum chamber. The mechanical clamp contacts to the pads are visible. The mounting also includes
cooling in order to remove heat produced by the currents. Center (from top to bottom): details of
fabrication and assembly: (i) a chip in the middle of the fabrication process, after some gold has
been evaporated and before the photoresist has been removed. The visible wires have a cross section
of 1• 1 ~tm2; (ii) an electron-microscope view of the surface: a 'T' junction of a 10-~tm wide wire
is visible as well as the 10 ~tm etchings which define it; (iii) typical design of the U- and Z-shaped
wires placed underneath the chip to help in the initial loading process; the wires can support >50 A
of current in DC operation without degrading a p < 10-11 mbar vacuum. Right: a typical design of
an atom chip. On both sides contact pads are visible. The center of the chip is used for loading
the atoms, which are then released into the physics areas: on top, a magnetic guide with arrays
of electric leads, on the bottom, a spiral formed by two parallel wires enables atom guiding in all
directions on the chip.
In general there are two different approaches to loading cold atoms into the chip
traps:
(i) Collect and cool the atoms at a different location and transport the cold
ensemble to the surface traps. This may be achieved using direct injection from
a cold atomic beam coming from a low-velocity intense source (LVIS) (Mfiller
et al., 1999, 2000, 2001) or a released MOT whereby the atoms are pulled by
gravity (Dekker et al., 2000). Transferring the atoms with magnetic traps has
been achieved by (Ott et al., 2001), and a Bose-Einstein condensate (BEC) has
been loaded using optical tweezers (Gustavson et al., 2002).
(ii) Cool and trap atoms close to the surface in a surface MOT, and transfer
the atoms from there to the microtraps on the chip (Reichel et al., 1999; Folman
et al., 2000). For this method the atom chip has to be either transparent or
reflecting.
In the following, we describe experiments performed at Heidelberg (resp.
Innsbruck), Sussex and Munich using the second approach. Further on, several
experiments using the first approach will also be discussed (see Figs. 37 and 38).
B. 1. Mirror M O T
FI6. 30. (A) a 'pyramid MOT' is obtained when one single laser beam is retro-reflected by
a four-sided pyramid in the center of a magnetic quadrupole. The reflections ensure the correct
helicities of the laser beams when the quadrupole field (field lines) has the same symmetry as the
pyramid. (B) The mirror MOT is generated from the pyramid by leaving out 3 of the 4 reflecting
walls. Two MOT beams (I and II) impinge from opposite directions on the reflecting surface of
the atom chip. The correct MOT configuration is ensured together with the magnetic quadrupole
field rotated 45 ~ to the atom chip surface as illustrated by the field lines. The magnetic field can
be obtained either by a set of external quadrupole coils, or by a U-shaped wire on the chip. Top:
the Sussex mirror MOT chip setup with the external quadrupole coils on the mounting, inside the
vacuum; two parallel wires embedded in a fiber are positioned on the surface of the mirror, forming
a two-wire guide and a time-dependent interferometer (see Sect. II). Two small 'pinch' coils visible
at the edges of the mirror provide longitudinal confinement. Courtesy E. Hinds.
10 In another version of this experiment, an evanescent field just above the extremely thin metal
surface, formed by light beams impinging on the back of the surface, was used as an atom mirror.
This allowed to produce a MOT with reasonable surface induced losses even at the extreme proximity
of 100nm from the surface.
IV] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 309
beams off the chip surface (see Fig. 30b) (Reichel et al., 1999; Folman et al.,
2000). The magnetic quadrupole field for the MOT can be obtained either by a
set of external quadrupole coils, or by superimposing a homogeneous bias field
with the field generated from a U-shaped wire on or below the chip ('U-MOT').
External quadrupole coils generate the correct magnetic field configuration if one
of the reflected light beam axes coincides with the coil axis. If the U-MOT is
used, the reflected light beams must lie in the symmetry plane of the U. Trapping
in the U-MOT has the advantage that the MOT is well aligned with respect to
the chip and its microtraps. If the mirror MOT is sufficiently far from the surface
(a few times the MOT radius), its loading rate and final atom number are very
similar to a regular free space MOT under the same conditions (laser power,
vacuum, supply of cold atoms, etc.). In agreement with earlier observations using
wires, the shadows (diffraction patterns) from the 10~tm etchings in the gold
surface of the nanofabricated atom chip do not disturb the MOT significantly
(Denschlag, 1998; Denschlag et al., 1999b).
Such atom chip mirror MOTs have been loaded from an atomic beam in Inns-
bruck/Heidelberg (Folman et al., 2000), from the background vapor in Munich
(Reichel et al., 1999), and in a double MOT system in Innsbruck/Heidelberg
(>108 atoms at lifetime <100 s), using either external coils or the U-wire for
the quadrupole field. In addition, at Sussex and Harvard surface MOTs were
realized using permanent and semi-permanent (magnetizable cores) magnetic
structures.
As an example we describe the Innsbruck/Heidelberg lithium setup. Figure 31
(overleaf) shows a top view of the mirror MOT just above the chip with
some of its electric connections. For the transfer into the U-MOT, the large
external quadrupole coils are switched off while the current in the U-shaped
wire underneath the chip is switched on (up to 25 A), together with an external
bias field (8 G). This forms a nearly identical, but spatially smaller quadrupole
field as compared to the fields of the large coils. By changing the bias field,
the U-MOT can be compressed and shifted close to the chip surface (typically
1-2 mm). The laser power and detuning are changed to further cool the atoms,
giving a sample with a temperature of about 200 ~tK.
After the U-MOT phase, atoms are cooled using optical molasses, optically
pumped and transferred into a matched magnetic trap, typically produced by
a thick Z-shaped wire plus bias field. From there atoms are transferred closer
and closer to the chip and loaded sequentially into smaller and smaller traps. In
general, it is favorable to lower the trap towards the surface by increasing the
magnetic bias field. This way the trap depth increases and less atoms are lost
due to adiabatic heating during compression. Unfortunately this is not feasible
310 R. Folman et al. [IV
FIG. 31. Loading of cold atoms close to the surface of an atom chip. Top left: Picture of the
mirror MOT, taken from above; the cloud is visible at the center while the electrical contacts can be
seen at the edges. Top right: schematic of the MOT beams and quadrupole coils. Center row: Atoms
trapped in the U-MOT created by a current in the large U-shaped wire underneath the chip and a
homogeneous bias field. Bottom row: Atoms in a magnetic trap generated by the U-wire field; from
left to right, the columns show the top, front and side (direction of bias field) views respectively, the
far right column shows the schematics of the wire configuration; current-carrying wires are marked
in black. The front and side views show two images: the upper is the actual atom cloud and the lower
is the reflection on the gold surface of the chip. The distance between both images is an indication
of the distance of the atoms from the chip surface. The pictures of the magnetically trapped atomic
cloud are obtained by fluorescence imaging using a short laser pulse (typically < 1 ms).
all the way: Finite size effects limit small traps to thin wires, at the price o f not
being able to p u s h high currents.
The basic transfer principle from a large wire to a small wire is to first
switch on the current for the s m a l l e r trap, and then to r a m p d o w n the c u r r e n t
in the b i g g e r trap m a i n t a i n e d by a thicker wire (Fig. 32). F u r t h e r c o m p r e s s i o n
is a c h i e v e d by using s m a l l e r and s m a l l e r currents. Care has to be taken that
the transfer is adiabatic, especially with r e s p e c t to the m o t i o n o f the p o t e n t i a l
m i n i m u m . B y an appropriate c h a n g e o f the bias field, the c o m p r e s s i o n o f the
a t o m s in the shrinking trap can be p e r f o r m e d v e r y smoothly. T r a n s f e r r i n g into
IV] M I C R O S C O P I C A T O M O P T I C S : F R O M W I R E S TO A T O M C H I P 311
Fl6. 32. Principle of compressing and loading wire guides. The position of the surface-mounted
wires and equipotential lines of the trapping potential are shown. Top row: the transfer from two
large 200 ~tm wires to one small 10 ~tm wire. In (a)-(c) the current in the small wire is constant
at 300 mA and the bias field is constant at 10 G. The current in the two large wires is decreased
from 2 A in each wire to zero. This transfers the atoms to the small wire. (d) By increasing the bias
field the trap can be compressed further. Bottom row: the transfer from one large 200 ~tm wire to
one small 10 ~tm wire. In (a)-(d) the current in the large wire drops from 2 A to zero. The thick
line shows how the trap center moves during transfer. A much weaker confinement during transfer
is obtained in this configuration.
FIG. 33. Compressing a cloud of cold atoms on an atom chip: Top row: view from the top;
center row: front view; bottom row: side view. The first three columns show atoms trapped on the
chip with the two U-shaped wires. The compression of the trap is accomplished by increasing the
bias field. The last row displays images from a Z-trap created by 300 mA current through the 10 gm
wire in the center of the chip. The pictures of the magnetically trapped atomic cloud are obtained
by fluorescence imaging using a short (<1 ms) molasses laser pulse.
serves as a magnetic trap for weak-field seekers (Fig. 3 l: U-trap). The magnetic
trap is lowered further towards the surface of the chip by increasing the bias
field. Atoms are now close enough to be trapped by the chip fields. Next, a
current of 2 A is sent through two 2 0 0 g m U-shaped wires on the chip, and
the current in the U-shaped wire located underneath the chip is ramped down
to zero. This procedure brings the atoms closer to the chip, compresses the
trap considerably, and transfers the atoms to a magnetic trap formed by the
currents on the chip surface. This trap is further compressed and lowered towards
the surface (typically <100~tm) by increasing the bias field (Fig. 33). From
there the atoms are transferred to a microtrap created by a 10 g m Z-shaped
wire.
In the lowest height and most compressed trap achieved to date, a 1 x 1 ~tm2
Z-shaped wire is used with a current of 100 mA (Heidelberg). With a bias field
of 30 G the atoms are trapped at a height of about 7 ~tm above the surface and
at an angular oscillation frequency co ~ 2Jr x 200 kHz (magnetic field gradients
of 50 kG/cm) for several tens of ms (see Eq. 6 for typical trap frequencies). At
such a small trap height several problems come into play: First, with the present
IV] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 313
A simple way to observe the trapped atoms is by fluorescence imaging. For this,
one illuminates the cloud with near-resonant molasses laser beams for a short
time (typically much less than l ms). The scattered light is imaged by CCD
cameras as shown in Fig. 31 and Fig. 33. One should use short enough exposure
times to avoid blurring of the image due to atomic motion. One also has to
select the camera positions wisely to avoid stray light caused by scattering off
the grooves in the atom chip surface. Furthermore, it is important that the metal
surface itself shows minimal light scattering. Here, the excellent surface quality
of evaporation on semiconductor surfaces is advantageous.
A different possibility is to use absorption imaging. If the probe beam is
directed parallel to the chip surface, the surface quality is not as critical, and
one does not have to take care of diffraction peaks from the grooves. Such
absorption imaging is used by the Munich, Tfibingen, Heidelberg, and MIT
groups. Profiting from an excellent surface mirror quality, the Heidelberg group
has also implemented absorption imaging with laser beams reflected from the
chip surface, which allows direct distance measurements. More sophisticated
methods such as phase contrast imaging will be important for more complicated
atom-optical devices on atom chips, where non-destructive observation very
close to the chip surface becomes essential. For an overview of these methods,
we refer the reader to the many BEC review papers (see, for example, Ketterle,
1999).
Finally, future light optical elements incorporated on the chip, such as
microspheres or cavities, will allow for much better detection sensitivity, possibly
at the single-atom level (see Sect. VI.A.3). Such work has been started in several
laboratories.
314 R. Folman et al. [IV
Since the first attempts two years ago, the atom chip has now become a 'tool
box in development' in numerous labs around the world. To the best of our
knowledge these include (in alphabetical order) the groups at Boulder/JILA
(D. Anderson and E. Cornell), CalTech (H. Mabuchi), Harvard (M. Prentiss),
Heidelberg (J. Schmiedmayer), MIT (W. Ketterle), Munich (J. Reichel and
T.W. H~insch), Orsay (C. Westbrook and A. Aspect), Sussex (E. Hinds), and
Tfibingen (C. Zimmermann). Unfortunately, we will not be able to present in
detail all the extensive work done, nor will we be able to touch upon other
surface-related projects, such as the atom mirror.
C.1. Traps
The simplest traps (i.e 3-dimensional confinement) are usually based on a straight
wire guide with some form of longitudinal confinement, which is produced either
by external coils or by wires on the chip (Sect. II.A.4). Additional wires for on-
board bias fields may also be added.
As an example, we start with the simple microtraps realized in Inns-
bruck/Heidelberg with lithium (Folman et al., 2000) and Munich with rubidium
atoms (Reichel et al., 1999; Reichel et al., 2001). Here, the traps are based on
wires of 1 to 30 ~tm width with which surface-trap distances below 10 ~tm were
achieved. The wires used are either U-, Z- or H-shaped.
In these experiments, the compression of traps and guides was also inves-
tigated (Folman et al., 2000; Reichel et al., 2001). This is done by ramping
up the bias magnetic field. In this process one typically achieves gradients of
>25 kG/cm. With lithium atoms, trap parameters with a transverse ground-state
size below 100nm and angular frequencies of 2:r x 200kHz were achieved
(Folman et al., 2000), thus reaching the parameter regime required by quantum
computation proposals (Calarco et al., 2000; Briegel et al., 2000).
In addition, an on-board bias field for the thin wire trap was also created
by sending currents through two U-shaped wires in the opposite direction
with respect to the thin wire current, substituting the external bias field
(see Sect. II.A.2). Hence, trapping of atoms on a self-contained chip was
demonstrated (Folman et al., 2000).
An example of a different configuration was realized in Munich with rubidium
atoms. Three-dimensional trapping was achieved by crossing two straight wires
and choosing an appropriate bias field direction, as discussed in Sect. II.A.4
(Reichel et al., 2001) (Fig. 34). Here the additional wire actually provides the
endcaps that were previously provided in the Z- and U-shaped traps by the same
wire. This type of trap will be useful for the realization of arrays of nearby
traps. In Tfibingen and Sussex longitudinal confinement has been achieved by
additional coils.
IV] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 315
FIG. 34. Ioffe-Pritchard trap created by two intersecting wires. The left-hand column corresponds
to I l > 12 and ]B0,y] > [B0,x[; in the right-hand column both relations are reversed. Top row:
conductor pattern; the thickness of the arrows corresponds to the magnitude of the current; dashed
arrows indicate the bias field direction. Middle row: calculated contours of the magnetic field
modulus ]B(x,y)] indicating how the long trap axis turns; the left potential continuously transforms
into the right one when the parameters are changed smoothly. Bottom row: absorption images
corresponding to the two situations. Courtesy J. Reichel.
FIG. 35. Top view of a thermal 200 ~tK cloud of lithium atoms in a double-well potential 40 ~tm
above the chip surface. The minima are separated by 350 ~tm. The imaging flash light pulse is 100 ~ts
long. The splitting may be done as slow as needed in order to achieve adiabaticity.
316 R. Folman et al. [IV
Fie. 36. (a) Cold atoms in a microtrap (left) and released all at once into a linear guide (right).
(b) Continuous loading of an atom guide by leaking atoms from a reservoir created by a U-trap into
the guide by ramping down the current in the U. Propagation is due to thermal velocity.
IV] MICROSCOPIC A T O M O P T I C S : F R O M W I R E S TO A T O M C H I P 317
FIG. 37. Vertical bias field: this Harvard experiment realized two-wire vertical guides, enabling
the guiding of atoms in a variety of directions. Left: setup. Right: absorption of probe beam versus
position along x at 3.5 mm below the output of the guide. The left and right peaks are attributed to
unaffected atoms and atoms deflected by the outside of the guide potential, respectively. The open
triangles are the data collected while the guide is turned off. Courtesy M. Prentiss.
FIG. 38. The JILA setup in which a 'low-velocity intense source' (LVIS) was used to directly load
the two-wire guide. The data show the need for strong potentials with which the magnetic guide
can overcome the kinetic energy in order to deflect the atoms, thereby bypassing the beam block.
Courtesy E. Cornell.
318 R. F o l m a n et al. [IV
Fic. 39. Moving atoms using a magnetic conveyor belt. (a) Potential for various phases of the
movement. The numbers indicate the position of the atoms as shown in the absorption images in
column (b). (c) Linear collider experiment: left, time evolution of the centers of mass of the two
clouds; right, absorption images of the colliding atoms. Courtesy J. Reichel.
a setup (Mfiller et al., 1999). Another similar use of this principle (in this case,
not surface-mounted), in which a storage ring has been realized is presented
in Sect. III.A.7. Although advantageous for the lack of bias fields, this concept
may be hard to implement on miniaturized atom chips as the atoms would be
extremely close to the surface for 1-2-~tm thick wires.
Guiding with semi-permanent magnets has also been achieved (Rooijakkers
et al., 2001; Vengalattore et al., 2001). These materials enhance the magnetic
fields coming from current-carrying wires (see Sect. II.A.10 for a description).
Completely permanent magnets are also being contemplated to avoid current
noise. However, to the best of our knowledge, only atom mirrors have thus far
been realized this way (Hinds and Hughes, 1999).
A further limitation of the guides described above is that they rely on thermal
velocity. Much more control can be achieved by transporting atoms using moving
potentials, as described in Sect. II.A.7. Such a transport device was implemented
in an experiment in Munich. Using the movable 3-dimensional potentials of their
'motor', atoms can be extracted from a reservoir and moved or stopped at will
(Hfinsel et al., 2001b) (Fig. 39). This considerably improves the possibilities of
the chip, as demonstrated by the 'linear collider' shown in Fig. 39c, in which
the motor was used to split a cloud in two and then to collide the two halves
(Reichel et al., 2001).
IV] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 319
FIG. 40. Beam splitter on a chip. (a) Chip outline; (b) fluorescence images of guided atoms. Two
large U-shaped 200 ~tm wires are used to load atoms into the input guide of a 10-~tm Y-beam splitter.
In the first two pictures in (b), a current of 0.8 A is driven only through one side of the Y, therefore
guiding atoms either to the left or to the right; in the next two pictures, taken at two different bias
fields (12 G and 8 G, respectively), the current is divided in equal parts and the guided atoms split
into both sides. (c) Switching atoms between left and right is achieved by changing the current ratio
in the two outputs and keeping the total current constant as before. The points are measured values
while the lines are obtained from Monte Carlo simulations with a 3-G field along the input guide.
The kinks in the lines are due to Monte Carlo statistics.
320 R. F o l m a n et al. [IV
means of symmetric scattering off the potential hill, which they encounter at the
splitting point. Such a beam splitter on an atom chip was realized by Cassettari
et al. (2000) in Innsbruck. Atoms were released from a chip microtrap and guided
into the beam splitter. Depending on how the current in the input wire is sent
through the Y, atoms can be switched from one output arm of the Y to the other,
or directed to the two outputs with any desired ratio (Fig. 40). Similar beam
splitters have been widely used for the splitting of guided electron waves in solid-
state quantum electronics devices. For example, two Y splitters were put back
to back to form an Aharonov-Bohm type interferometer (Buks et al., 1998).
A four-port beam splitter has been realized at JILA by the group of E. Cornell
and D. Anderson by making a near X-shape out of two wires which avoid a full
crossing (Mtiller et al., 2000). In this experiment, two input guides formed by
two current-carrying wires, merge at the point of closest approach of the wires
so that the two minima merge into one, and then again split into two independent
minima.
C. 4. B E C on a chip
FIG. 41. Left: the Ttibingen setup. The first pair of coils (right) produced the MOT and then the
atoms were conveyed to the trap formed by the second pair of coils. The chip mounting is visible
within the second pair of coils. Right: absorption images of the compression and final cooling stage;
(a) compression into the microtrap; (b) RF cooling in the microtrap; (c) release of the condensate
after 5, 10, and 15 ms time of flight. Courtesy C. Zimmermann.
adjacent pairs of coils (Fig. 41). In the chip trap, condensation was reached
after 10 to 30 s of forced RF evaporative cooling. Aside from being the first
surface BEC, the chip used in Tfibingen with its 25-mm long wires provides a
highly anisotropic BEC (aspect ratio 105), approaching a quasi one-dimensional
regime. In recent work, the BEC was taken to a height of only 20~tm without
observing substantial heating (Fortagh et al., 2002). The smallest structure
holding the BEC was a 3 x 2 . 5 / t m 2 cross section copper wire with a current
of 0.4 A. The BEC had a lifetime of 100 ms in the compressed trap (limited by
3-body collisions) and a 1 s lifetime once it was expanded into a larger trap.
The second experiment producing a BEC in a microtrap was performed in
Munich (H~insel et al., 2001a) (Fig. 42). Here an attractively simple setup
with a continuous dispenser discharge was used. Consequently, the vacuum
background pressure was high (10 -9 mbar) and evaporative cooling had to be
achieved quickly. RF cooling times were as short as 700 ms thanks to the strong
compression in the microtrap which results in a high rate of elastic collisions.
The final BEC included some 6000 atoms at a height o f 70 ~tm. The trapping
wire was 1 . 9 5 m m long and had a cross section of 50• the current
density approached 106 A / c m 2. Strong heating of the cloud was observed in this
experiment but the source remains elusive (possibly, current noise). A beautiful
feature of this experiment is the use of the magnetic 'conveyor belt' described
before (Sects. II.A.7 and IV.C.2, Fig. 39), in order to transport the BEC during
a time of lOOms over a distance o f 1.6 m m without destroying it (see Fig. 42).
Furthermore, the ability of the 'motor' to split clouds was used to show that a
322 R. Folman et al. [IV
FI6. 42. Munich atom chip BEC experiment. Left: schematics of the simple vapor cell apparatus.
Center: time-of-flight images showing the formation of a BEC. Right: (a) the BEC is transported
in a movable 3-dimensional potential minimum; (b) at the end it is released and is observed falling
and expanding. Courtesy J. Reichel.
BEC survives such a splitting. Two such halves were then released into free fall
exhibiting interference fringes as they overlapped.
In the third experiment, performed in Heidelberg, typically 3 • 105 87Rb atoms
were condensed in a Z-wire Ioffe-Pritchard trap, created by a structure under-
neath the chip, and subsequently transferred to a Z-trap on the chip (Fig. 43).
First, more than 3• 108 atoms are loaded into a mirror MOT ( < 1 0 -li torr)
created by external quadruople coils using a double MOT configuration with a
continuous push beam. The atoms are then transferred into a U-MOT, where they
are compressed and after molasses-cooling loaded into a Z-wire trap. The BEC
is formed by forced RF evaporation in typically 20 seconds. Creating the BEC
using a wire structure underneath the chip allows to place other surfaces close
to the BEC while maintaining the high precision of a microtrap for manipulating
the cold atoms. This will open up the possibility to study surfaces with the cold
atoms and to transfer the BEC to surface traps based on dipole forces in light
fields created by micro-optic elements and evanescent fields.
The MIT group transported a BEC of the order of 10 6 Na atoms into an
auxiliary chamber and loaded it into a magnetic trap formed by a Z-shaped
wire (Gustavson et al., 2002) (Fig. 44). This was accomplished by trapping
the condensate in the focus of an infrared laser and translating the location
of the laser focus with controlled acceleration. This transport technique avoids
the optical and mechanical access constraints of conventional condensate
experiments. The BEC was consequently loaded into a microstructure (Leanhardt
et al., 2002).
Finally, we would like to note that currently other groups are also working
IV] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 323
FIG. 43. Heidelberg atom chip BEC experiment. (a) Schematics of the double MOT setup. Atoms
from a lower vapor cell MOT are transferred to a UHV mirror MOT using a continuous push beam.
(b) Photograph of the upper (UHV) chamber. (c) The mounted chip and the U- and Z-shaped wire
structure underneath the chip (inset). (d) Thermal cloud, BEC with thermal background, and pure
BEC released and expanded for 15 ms.
FIG. 44. Transfer of a BEC to a microtrap. Left: schematics of the setup with the science chamber
housing the Z-trap on the far left and the BEC production chamber on the right. Right: condensates
in the science chamber (a) optical trap and (b) Z-trap. The condensate was (c) released from an
optical trap and imaged after 10 ms time of flight and (d) released from a wire trap and imaged after
23 ms time of flight. (e) Schematic of the Z-trap. Courtesy W. Ketterle.
towards BEC in s u r f a c e t r a p s , a n d w e e x p e c t to s e e m a n y d i f f e r e n t s u c c e s s f u l
experiments shortly.
324 R. Folman et al. [V
For atom chips to work, three main destructive elements have to be put under
control:
(i) Trap loss: It is crucial that we are able to keep the atoms inside the trap as
long as needed.
(ii) Heating: Transfer of energy to our quantum system may result in excitations
of motional degrees of freedom (e.g. trap vibrational levels), and conse-
quently in multimode propagation which would render the evolution of the
system ill-defined.
(iii) Decoherence or dephasing as it is sometimes referred to also originates from
coupling to the environment. While heating requires the transfer of energy,
decoherence is more delicate in nature (Stern et al., 1990). Nevertheless, the
effect is just as harmful because superpositions with a definite phase relation
between different quantum states are destroyed. This has to be avoided, e.g.
for interferometers or quantum information processing on the atom chip.
In discussing these three points, we focus on the particularities of atoms in
strongly confined traps close to the surface of an atom chip. The small separation
between the cold atom cloud and the 'hot' macroscopic environment raises the
intriguing question of how strong the energy exchange will be, and which limit
of atom confinement and height above the surface can ultimately be reached.
We review theoretical results showing that fluctuations in the magnetic trapping
potential give a fairly large contribution to both atom loss and heating. In
addition, thermally excited near fields are also responsible for loss and may
impose limits on coherent atom manipulation in very small (~tm-sized) traps
on the atom chip. Estimates for the relevant rates are given, and we outline
strategies to reduce them as much as possible. Experimental data are not yet
reliable enough to allow for a detailed test of the theory, but there are indications
that field fluctuations indeed influence the lifetime of chip traps (Hansel et al.,
2001a; Fortagh et al., 2002).
A. Loss MECHANISMS
Compression of a thermal atom cloud can lead to losses when the cloud
temperature rises above the trap depth. The smallest losses occur if the
compression is adiabatic. Atoms then stay in their respective energy levels as
the level energy increases. They can nevertheless be lost during trap compression
because of the finite trap depth. It should be noted that this loss occurs for the
highest energies in the trap and can also be used to evaporatively cool the cloud
(see Luiten et al., 1996 for a review).
V] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 325
where S~t(COL) is the noise spectrum of the magnetic fields, taken at the Larmor
frequency COL.We use the following convention for the noise spectrum:
Table II
Trace of the geometric tensor Y/j that determines the loss due to the thermally fluctuating magnetic
near field, according to the rate (22) a
a The metallic layer has a thickness d, assumed much smaller than the distance h to the trap center.
The wire has a radius a << h, and h << 6 is assumed where 6 is the skin depth of the metal. Taken
from Henkel and P6tting (2001). A more accurate calculation of Tr Y/j corrects the results of table 2
by a factor of 1/2 for the half-space and the layer (Henkel and Scheel, 2002).
Z
~dco O
(Bi(t)Bj(t))= ~-~SB(o)). (21)
For example, the rms magnetic field in a given bandwidth Af for a white noise
spectrum $8 is given by Brms = v/AfSB. The spectrum SB thus has units G2/Hz.
where 1/e is the substrate conductivity (for copper, ~)Cu = 1.7x 10-6f~cm) and
Ts is the substrate temperature. Note that the Larmor frequency COLactually does
not enter the loss rate. The 'geometric tensor' YO has dimension (1/length) and
is inversely proportional to the height h of the trap center above the surface
(Table II). The loss rate (22) is quite large for a trap microns above a bulk metal
surface. One can reduce the loss by two orders of magnitude when bulk metal in
the vicinity of the trap is replaced by microstructures. For a thin metallic layer
of thickness d, the loss rate (22) is proportional to d/h 2, and for a thin wire
(radius a), a faster decrease o( a2/h 3 takes over (Table II).
The estimates of Table II apply only in an intermediate distance regime,
d,a << h << 6((OL): on the one hand, when the trap distance h is smaller than
the size of the metallic structures, one recovers a 1/h behaviour characteristic for
V] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 327
FIG. 45. Loss rates in a magnetic trap above a copper surface. Results for two different Larmor
frequencies tOL/2Jr = 1 MHz (curve a) and 100 MHz (curve b) are shown. The arrows mark the
corresponding skin depths 6(~OL). Equation (22) applies to the region h << 6(~OL). See Henkel et al.
(1999) for details. Parameters: spin S = 89 magnetic bias field aligned parallel to the surface. The
loss rate due to the black-body field is about 10-13 s-I at 100MHz (not shown). Reproduced from
Henkel et al. (1999), Appl. Phys. B 69 (1999) 379, Fig. 3, with permission. 9 Springer-Verlag.
a metallic half-space; on the other hand, steeper power laws take over at large
distances, when h gets comparable to or larger than the skin depth
where the reference value Ssy = 3.2 x 10 - 1 9 A2/Hz corresponds to shot noise at a
wire current of 1 A (Ssy = 2elw). This estimate is pessimistic and assumes equal
328 R. Folman et al. [V
noise in both field components parallel and perpendicular to the static trapping
field. Nevertheless, it highlights the need to use 'quiet' current drivers for atom
chip traps. In future chip traps with strong confinement, it may turn out necessary
to reduce current noise below the shot-noise level. This can be achieved with
superconducting wires or permanent magnets, as discussed in Sect. II.A. 10 and
reviewed by Hinds and Hughes (1999). See also Varpula and Poutanen (1984).
A. 4. Collisional losses
A.4.1. Background collisions. Here, collisions between background gas atoms
and trapped atoms endow the latter with sufficient energy to escape the trap. In
order to estimate the loss rate per atom ~', let us assume that the background gas
is dominated by hydrogen molecules and at room temperature. We then get:
A.4.2. Collisions o f trapped atoms. For traps in UHV conditions, and especially
for highly compressed traps and high-density samples, the dominant collisional
loss mechanisms involve collisions between trapped atoms. The scattering of
two atoms leads to a loss rate per atom scaling with the density, while 3-body
collision rates scale with the density squared.
Spin exchange. This process corresponds to inelastic two-body collisions
where the hyperfine spin projections mF are conserved, but not the spins F
themselves. In the alkali atoms 7Li, 23Na, and 87Rb, for example, a collision
between two weak-field-seeking states IF = 1, mF = -1) can lead to the
emergence of two strong-field seekers ]2,-1 ) that are not trapped. This transition
requires an excess energy of the order of the hyperfine splitting to occur, which
is typically not available in cold atom collisions. Exothermic collisions between
the weak-field seekers 11,-1), 12, +1), and 12, +2) are not suppressed, however.
The corresponding rate constant is proportional to n ( a s - aT) 2 where as (at)
are the scattering lengths in the singlet (triplet) diatomic potential (C6t6 et al.,
1994). For 87Rb, these scattering lengths accidentally differ very little, leading
to a very small spin flip rate (Moerdijk and Verhaar, 1996; Burke et al., 1997).
As a consequence, 87Rb is practically immune to spin exchange and can form
stable condensates, even of two hyperfine species (Myatt et al., 1997; Julienne
et al., 1997; Kokkelmans et al., 1997). Spin-polarized samples consisting only
of 12, +2) cannot undergo spin exchange because of mF conservation, the other
available states having smaller F. For more details, we refer to the review by
Weiner et al. (1999) and references therein.
V] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 329
Spin relaxation. This process also results from inelastic two-body collisions,
but does not conserve mF. Spin relaxation is caused by a flip of the nuclear spin
and occurs at a lower rate because of the smaller nuclear magnetic moment. In
87Rb for example, the trapped weak-field seeker I1,-1) may be changed into the
untrapped strong-field seeker I1, + 1). More details can be found in the theoretical
work by Burke et al. (1997), Julienne et al. (1997), Timmermans and C6t6
(1998), the experimental work of Gerton et al. (1999) and S6ding et al. (1998),
and the review paper by Weiner et al. (1999).
Three-body recombination. In this process, two atoms combine to form a
molecule. Although the molecules may have a definite magnetic moment and
still be trapped, the reaction releases the molecular binding energy that is shared
as excess kinetic energy between the molecule and the third atom. The binding
energy being typically quite large (larger than 100 ~teV), both partners escape the
trap (Fedichev et al., 1996; Moerdijk and Verhaar, 1996; Moerdijk et al., 1996;
Esry et al., 1999). For references to experimental work, see Burt et al. (1997),
S6ding et al. (1999) and Weiner et al. (1999). We expect three-body processes to
be the dominant collisional decay channel in strongly compressed traps because
the collision rate per atom increases with the square of the atomic density.
A.5. Tunneling
Traps very close to the surface might also show loss due to tunneling of atoms out
of the local minimum of the trap towards the surface. The rate can be estimated
by
?'~ e)
1
exp\- (,/
2m[U(z)- E]/dz, (26)
rrier width ~
where U ( z ) - E is the height of the barrier above the energy of the trapped
particle. Tunneling will therefore only be important for states close to the
top of the potential barrier. Low-lying states in traps where the magnetic
field magnitude rises for long distances will have very little tunneling. Even
for atom waveguide potentials as close as 1 ~tm from the surface, tunneling
lifetimes of more than 1000s have been estimated (Pfau and Mlynek, 1996;
Schmiedmayer, 1998).
Table III
Loss mechanisms for the atom chip (overview)
a The columns 'Scaling' and 'Magnitude' refer to loss rates per atom at typical atom chip traps:
density n = 101~ -3, height h = 10~tm, trap frequency to/2Jr = 100kHz, Larmor frequency
tOL/2Jr = 5 MHz.
b Eq. (25).
c Flip rate (18) from trap ground state.
d Eq. (22). The exponent ct = 1,2, 3 for metal half-space, layer, and wire (see table 2). The estimate
10s -l is for a half-space.
e Eq. (24). SI(m)/SsN = 100.
f Experimental result for 87Rb (Myatt et al., 1997).
g Experimental result for Cs and 7Li, respectively (S6ding et al., 1998; Gerton et al., 1999).
h Experimental results for 87Rb and 7Li, respectively (Burt et al., 1997; S6ding et al., 1999; Gerton
et al., 1999).
To s u m m a r i z e , an o v e r v i e w o f the p r e v i o u s loss m e c h a n i s m s is g i v e n in
Table III. We e x p e c t that on the route t o w a r d s ~tm-sized traps with high c o m p r e s -
sion, inelastic collisions and m a g n e t i c field n o i s e will d o m i n a t e the trap loss.
B. HEATING
the influence of position and frequency noise using the harmonic oscillator
model, then turn to substrate and technical noise, and finally touch upon the
issue of heating due to light fields.
that is determined by the noise spectrum of the force at the oscillator frequency
SF(~O). The rate of energy transfer to the atom ('heating rate') is simply F0~lho)
or SF(O))/4M. Note that this estimate remains valid for an arbitrary initial state.
We may make contact with the work of Gehm et al. (1998) by noting that
fluctuations Ax of the trap center are equivalent to a force
F = Me)2Ax. (28)
In terms of the fluctuation spectrum of the trap center Sx(~O), the excitation
rate (27) is thus given by
Me) 3 09 2
F0___, 1 = Sx((D ) = -x-Sx/ao((_D), (29)
4h ~5
which is equivalent to the heating rate (12) of Gehm et al. (1998), given our
definition (20) of the noise spectrum.
Fluctuations of the trap frequency are described by the Hamiltonian MxZo)Aco
and heat the atom by exciting the 0 ~ 2 transition. The corresponding transition
rate is (Gehm et al., 1998)
and involves the frequency noise spectrum at twice the trap frequency. Using
the rates given by Gehm et al. (1998), one can show that the heating rate due
332 R. Folman et al. [V
FIG. 46. Heating rate for a trapped spin above copper and glass substrates. Parameters: trap
frequency to/2Jr = 100 kHz, M = 40 amu, magnetic moment/t =/t B = 1 Bohr magneton, spin S - 1.
The heating rate due to the magnetic black-body field (not shown) is about 10-39 s-1 . For the glass
substrate, a dielectric constant with Re e = 5 and a resistivity e = 1011 ~2cm are taken. Reproduced
from Henkel et al. (1999), Appl. Phys. B 69 (1999) 379, Fig. 5, with permission. 9 Springer-Verlag.
V] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 333
SF((,O)=(IA~176
2SrBb
2$I ((o), (33)
and we end up with an excitation rate
Another source of heating are the external light fields with which the atoms are
manipulated and detected. Here the Lamb-Dicke parameter r/ is a convenient
tool, where 27ra0
r/- ~ (37)
is the ratio between the ground-state size of the trap a0 and the wavelength of
the impinging wave. This becomes clear if we remember that the probability not
to be excited P0~0 is simply the well-known Debye-Waller factor
Table IV
Heating mechanisms for the atom chip (overview)
a The columns 'Scaling' and 'Magnitude' refer to transition rates from the ground state of a typical
atom chip trap: lithium atoms, height h = 10~tm, trap frequency co/2sr = 100kHz. Harmonic
confinement is assumed throughout.
b Eq. (32), for a metal half-space.
c Eq. (34). Note the scalings c o - B Z / I w and h ~ I w / B b for trap frequency and height.
d Eq. (36).
V] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 335
C. DECOHERENCE
C. 1. Internal states
The spin states of the trapped atom are promising candidates for the implemen-
tation of qubits. Their coherence is reduced by transitions between spin states,
induced by collisions or noise. The corresponding rates are the same as for the
loss processes discussed in Sect. V.A.
In addition, pure phase noise occurs in the form of fluctuations in the
longitudinal magnetic fields (along the direction of the trapping field). These shift
the Larmor frequency in a random fashion and hence the relative phase between
spin states. The corresponding off-diagonal density matrix element (or fringe
contrast) is proportional to (exp(iA~)) where Aq~ is the phase shift accumulated
336 R. Folman et al. [V
due to noise during the interaction time t. A 'decoherence rate' Ydec can be
defined by (A~ 2) S0)(o)--+ 0)
'/dec -- (39)
2t 4 '
where S~(o)) is the spectrum of the frequency fluctuations. Two spin states
[mF), Imp-), for example, 'see' a frequency shift (p(t)- g l l B ( m F - m~F)ABil(t)/h,
that involves the differential magnetic moment and the component ABII(t ) of
the magnetic field noise parallel to the trap field. The spectrum S~(co) is then
proportional to the spectrum of the magnetic field fluctuations.
Equation (39) is derived in a rotating frame where the phase shift has zero
mean and making the assumption that the spectral density Sr is essentially
constant in the frequency range o) ~< 1/t. The noise then has a correlation time
much shorter than the interaction time t. We consider, as usual in theory, that
A~ is a random variable with Gaussian statistics, and get a fringe contrast
(il~llli)
AwL(t) - ~ABil(r, t). (41)
Here, the average magnetic moment is taken in the spin state ]i) trapped in the
static trap field, thus picking the component ABI[ parallel to the trap field. The
noise spectrum of this field component, for thermal near field noise, is of the
same order of magnitude as for the perpendicular component (Henkel et al.,
1999) and depends only weakly on frequency. We thus get a decoherence rate
comparable to the loss rate (22), typically a few l s-1 . The same argument can be
put forward for fluctuations in the wire current and the bias field. Assuming a flat
current noise spectrum at low frequencies, we recover the estimate (24) for spin
flip loss (a few l s-1). Therefore, keeping the atoms in the trap, and maintaining
the coherence of the spin states requires the same effort.
We finally note that near field magnetic noise also perturbs the coherence
between different hyperfine states that have been suggested as qubit carriers.
Although these states may have the same magnetic moment (up to a tiny
correction due to the nuclear spin), excluding pure phase noise, their coherence
is destroyed by transitions between hyperfine states. The corresponding loss rate
(relevant, e.g., for optical traps) has been computed by Henkel et al. (1999) and
is usually smaller than the spin flip rate.
V] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 337
Here, the distance z - z t denotes how 'off-diagonal' the element is, and D is the
momentum diffusion coefficient. The coherence length thus decreases like
h
~:~ - v / ~ . (43)
At the same time, the momentum spread Ap "-" (2Dt) 1/2 increases, so that the
relation Ap~c -~ h is maintained at all times. At long times, ~c will be limited by
the thermal de Broglie wavelength at the equilibrium temperature. However, this
regime will not be reached on atom chips for typical experimental parameters.
For a particle trapped in a potential, the density matrix tends to a diagonal
matrix in the potential eigenstate basis if the timescale for decoherence is
large compared to the oscillation time 2zr/co. This regime typically applies
to the oscillatory motion in atom chip waveguides. The regime in which the
two timescales are comparable has been discussed by Zurek et al. (1993) and
Paz et al. (1993); it leads to the 'environment-induced selection' of minimum
uncertainty states (coherent states for a harmonic oscillator).
In the following we discuss different decoherence mechanisms for a typical
separated path atom interferometer on the atom chip.
where the decoherence rate Ydec(s) depends on the spatial separation s = z - z'
between the two parts of the atomic wave function being observed:
1 -C(s)
Ydec(S) = 2],l 2 Sv(h; co ~ 0). (46)
Here, C(s) is the normalized spatial correlation function of the potential (equal
to unity for s = 0), and the noise spectrum Sv(h; co ---+ 0) characterizes the
strength of the magnetic noise at the waveguide center.
For an atom chip waveguide perturbed by magnetic near field noise, the
decoherence rate is of the order of
0)
y = 2h 2 (47)
and hence comparable to the spin flip rate (19, 22). Decoherence should thus
typically occur on a timescale of seconds. The correlation function C(s) is
well approximated by a Lorentzian, as shown by Henkel et al. (2000), and the
decoherence rate (46) can be written as
ys 2
Ydec(S)- $2 + 12, (48)
where lc is the correlation length of the magnetic noise. This length can be
taken equal to the height h of the waveguide above the substrate (Henkel et al.,
2000). This is because each volume element in the metallic substrate generates a
magnetic noise field whose distance-dependence is that of a quasi-static field (a
1/r 2 power law). Points at the same height h above the surface therefore see the
same field if their distance s is comparable to h. At distances s >> h, the magnetic
noise originates from currents in uncorrelated substrate volume elements, and
therefore C(s) ~ O. The corresponding saturation of the decoherence rate (48),
Ydec(s >> lc) ---. y, has also been noted, for example, by Cheng and Raymer
(1999).
Decoherence due to magnetic noise from technical sources will also happen
at a rate comparable to the corresponding spin flip rate, as estimated in Eq. (24).
The noise correlation length may be comparable to the trap height because the
relevant distances are below the photon wavelength at typical electromagnetic
noise frequencies, so that the fields produced by wire current fluctuations are
quasi-static, and the same argument applies. The noise correlation length of
sources like the external magnetic coils will, of course, be much larger because
these are far away from the waveguide. These rough estimates for the spatial
noise properties of currents merit further investigation, in particular at the shot-
noise level (Henkel et al., 2002).
V] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 339
I F(s,t) I
1
0.8
=
0.6
0.4
0.2
s/l c
1 2 3 4 5 6
FIc. 47. Illustration of spatial decoherence in an atomic wave guide. The spatially averaged
coherence function F(s, t) = f d z p(z + s,z, t) is plotted vs. the separation s for a few times t. Space
is scaled to the field correlation length lc and time to the 'scattering time' 1/y _= 1/Ydec(~ ).
A Lorentzian correlation function for the perturbation is assumed. Reproduced from Henkel and
P6tting (2001), Appl. Phys. B 72 (2001) 73, Fig. 3, with permission. 9 Springer-Verlag.
s2
~dec(S) ~ ~ [2 (49)
for the decoherence rate (48). From the density matrix (45), we can then read
off the momentum diffusion constant D hZy/l 2. =
C.4.2. Phase noise. The coherence between the spatially separated interferom-
eter arms is suppressed in the same way as the longitudinal coherence discussed
in Sect. V.C.3. To show this, we use an argument based on phase noise, and
focus again on magnetic field fluctuations, either of thermal or technical origin.
Magnetic fluctuations affect both the bottom of the trap well and the transverse
trap frequency, but are only relevant when they differ in the spatially separated
arms. The well bottoms get differentially shifted from an inhomogeneous bias
field, e.g., while the trap frequency shifts due to changes in the field curvature.
We generalize formula (39) to a phase shift Aq) that is the accumulation of
energy-level differences AE(t) along the paths in the two arms. The decoherence
(or dephasing) rate is thus given by
SAE(O0 ~ O)
Ydec = 4h 2 , (50)
<AE(t) AE(t')) = (ER(t) ER(t')) + (EL(t) Ec(t')) - <ER(t) Ec(t')) - <EL(t) ER(t')) ,
(51)
where the last two terms contain the correlation between the noise in both arms.
They may therefore be expressed through the normalized correlation function
CRC =-- C(s) with s the separation between the left and right arms. The reasonable
assumption that both arms 'see' the same white noise spectrum, say SE(W),
yields
1 - C(s)
Ydec = ] I d e c ( S ) = 2h 2 SE(o) ~ 0), (53)
where we recover the decoherence rate (46) obtained for the quasi-free
longitudinal motion. We also recover the trivial result that the contrast stays
constant if both interferometer arms are subject to the same noise amplitude
(perfect correlation C ( s ) - 1).
V] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 341
The previous argument shows that transverse and longitudinal coherence are
affected in a similar way by magnetic noise. Again, near field noise is a serious
threat due to its short correlation length. Since the decoherence rate is so
small that Ydec(CX3)t << 1 for interaction times not longer than a few hundred
ms, the phase noise remains small even for widely separated arms subject to
decorrelated noise (separation larger than the guide height). This is a worst-
case estimate: a more careful approach would take into account the form of
the interferometer, where the arm separation is not constant. Current noise
should neither be underestimated. It is certainly possible to reduce dephasing
by feeding the same current through both left and right wire guides, as shown
by Eq. (53). But this does not seem to help at the shot-noise level because each
electron randomly follows one or the other wire. The wire current fluctuations
are thus uncorrelated, leading to a transverse decoherence rate comparable to
the longitudinal decoherence rate. Both rates are thus of the order of the flip
rate (24), typically a few s-1 .
Let us estimate as another example the dephasing due to technical noise in
a magnetic field gradient. This may be introduced by an imperfect Helmholtz
configuration or coil misalignment. For small gradients b, we have
where Ib and Bb are the Helmholtz current and the bias field. The experimentally
reasonable parameters Ib = 1 A, s = 100 ~tm, R = 10 cm, Bb = 10 G yield the
small value I/dec(S) "~ 10-10 S -1 X SI(O) --+ 0 ) / / S s N . We note that the residual
gradient of imperfect Helmholtz coils is usually less than 0.1 G/cm which is an
order of magnitude below the estimate Bb/R - 1 G/cm taken here.
Finally, let us estimate the phase noise due to fluctuations in the spring constant
of the guide potential. Even in the adiabatic limit where the transitions between
transverse quantum states are suppressed (no heating), these fluctuations shift
342 R. Folman et al. [VI
Table V
Decoherence mechanisms for atom chip interferometers (overview)
Substrate fields b
s << h Tss2/eh a+2 << 10s -1 little metal,
a 'Magnitude' refers to the decoherence rate Ydec(S) for a typical guided interferometer: lithium
atoms, height h = 10 gm, separation s - 10 ~tm, transverse guide frequency o9/2:r = 100 kHz. Along
the waveguide axis, the atomic motion is free.
b Exponent a = 1,2, 3 for metal half-space, layer, and wire (Eq. 22 and table 2).
c Eq. (34).
d Eq. (56). The bias field scales as B b ~ Ib/R where R is the size of the bias coils.
e Eq. (36).
the energy of the guided state. In the harmonic approximation, we have for the
ground state of the guide AE = l hA~o where Ao9 is the relative shift of the
vibration frequency. This gives a dephasing rate
BEC on an atom chip. Where to go from here? What can we expect from future
integrated matter wave devices? There are still many open questions before we
can assess the full promise of integrated microscopic atom optics.
In the following we try to pinpoint the relevant future developments and
directions. Some of them, like the study of the influence of the warm thermal
surface and the fundamental noise limits on lifetime, heating and coherence of
atoms, are already under way. Hopefully in a few years we will know how far
micromanipulation of atoms on chips can be pushed.
micro-optics will allow to load atoms into evanescent-wave guides and traps,
as proposed by Barnett et al. (2000). Such traps and guides would be a way
to circumvent the decoherence caused by Johnson noise in a warm conducting
surface (Sect. V).
With the standing wave created by reflecting light off the chip surface one
will be able to generate 2-dimensional traps with strong confinement in one
direction, resembling quantum wells, as demonstrated by Gauck et al. (1998).
Adding additional laser beams or additional electrodes on the surface restricts the
atomic motion further, yielding 2-dimensional devices as in quantum electronics
(Imry, 1987). Similarly one can build and load optical lattices close to the surface
where each site can be individually addressed by placing electrodes on the chip
next to each site.
In principle, many other quantum optical components can be integrated on the
atom chip. For example, high-Q cavities combined with microtraps will allow
atoms to be held inside the cavity to much better than the wavelength of light
providing a strong coupling between light and atoms. For recent experimental
work concerning the manipulation and detection of atoms in cavities, we refer
the reader to Berman (1994), Pinkse et al. (2000), Hood et al. (2000), Osnaghi
et al. (2001) and Guth6hrlein et al. (2001).
Regarding cavities one can think of examining a wide variety of technologies
ranging from standard high-Q cavities consisting of macroscopic mirrors to
optical fiber cavities (with Bragg reflectors or with mirrors on the ends); from
photonic band gap structures to microcavities like microspheres and microdiscs
fabricated from a suitable transparent material. One proposed implementation is
presented in Fig. 48 (Mabuchi et al., 2001).
FIG. 48. A proposed implementationof an integrated nanofabricated high-Q cavity from CalTech.
The cavity is made of a 2D photonic crystal utilizing holes with diameters of order 100nm. A
Weinstein-Libbrecht-type Ioffe magnetic trap will hold the atom in the cavity. CourtesyH. Mabuchi.
VI] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 345
A.3.1. Single-atom detection using near field radiation. To detect light scattered
from single atoms near a chip surface, the main challenge will be to minimize the
stray light scattered from the surface. One possible solution may be to collect a
large fraction of the light scattered by the atom using near field apertures and/or
confocal microscope techniques. An atom could also be used to couple light
between two wave guides, as used in some micro-optic detectors for molecules
and directional couplers in telecommunication.
B. MESOSCOPIC PHYSICS
The potentials created on an atom chip are very similar in scale and confinement
to the potentials confining electrons in mesoscopic quantum electronics (Imry,
1987). There electrons move inside semiconductor structures, in our case
atoms move above surfaces in atom-optical circuits. In both cases they can be
manipulated using potentials in which at least one dimension is comparable to
the de Broglie wavelength of the guided, trapped particle. To find similarities
and differences between mesoscopic quantum electronics and mesoscopic atom
optics will probably become a very rich and fascinating research field.
Electrons in semiconductors interact strongly with the surrounding lattice.
It is therefore hard to maintain their phase coherence over long times and
distances. An atomic system on the contrary is well isolated. Furthermore, atoms
(especially in a BEC) can be prepared in such a way that the temperature is
extremely low with respect to the energy level spacing. The consequence is that
phase coherence is maintained over much longer times and distances. This might
enable us to explore new domains in mesoscopic physics, which are hard to reach
with electrons.
B.2. Interferometers
In the near future it will be essential to develop and implement interferometers,
and to study through them the decoherence of internal states and external
motional states. Atom chip interferometers have been discussed in detail in
Sect. II.A.9. They can be built either in the spatial (Andersson et al., 2002)
or in the temporal domain (Hinds et al., 2001; H~insel et al., 2001 c). Integrated
VI] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 347
on an atom chip, they are very sensitive devices that may be used to measure
inertial forces or even to perform computation (Andersson and Barnett, 2000).
Coherence properties in more complicated networks can be studied by observing
interference and speckle patterns.
Interferometers can also serve as probes for the understanding of surface-
atom interactions, allowing for a quantitative test of the limits imposed on the
atom chip by the warm surface for both internal state and external (motional)
state coherence. Since many of the important parameters scale with the spin flip
life time in a trap (see Sect. V), a first important step would be to measure the
(BEC) lifetime in a microtrap as a function of distance to the surface. Aside from
heating and spin flips, the surface also induces 'phase noise'. Interferometers will
be able to measure this subtle effect as a function of surface material type and
temperature as well as atom-surface distance and spatial spread of the atomic
superposition, through a reduction in the fringe visibility. Finally, by coupling
microtraps (atomic quantum dots) to one of the interferometer arms, similar to
the mesoscopic electron experiments (Buks et al., 1998), subtle interaction terms
may be investigated, e.g., 1/r second-order dipole interactions as discussed by
O'Dell et al. (2000).
Internal state superpositions of atoms close to surfaces can be studied using
internal state interferometers. Using Raman transitions or microwave transitions
we can create superpositions, observe their lifetime and put theoretical estimates
to the test.
B. 4. Non-linear phenomena
Let us end this subsection concerning mesoscopics by noting that the ability
to change the number of atoms in a system, or alternatively to address specific
atoms in an interacting ensemble, will allow us to probe the boundary between
the macroscopic and microscopic description. Starting from a large system,
we will try to gain more and more control over the system parameters,
imprinting quantum behavior onto the system. On the other hand we can
try and build larger and larger systems from single quantum objects (called
qubits in modern lingo), and keep individual control over the parameters.
Success in such an undertaking would bring us much closer to implementing
quantum information transfer and quantum information processing as discussed
below.
C. QUANTUMINFORMATION
One method to realize a qubit is to write the qubits into single atoms, which
requires selective cooling and filling of atoms into the qubit sites. However,
recently it was proposed that single qubits can also be written into an ensemble
of atoms using 'dipole blockade' (Lukin et al., 2001). This may be simpler
as it avoids the need for single-atom loading of traps. As will be pointed out
below, the dipole blockade mechanism can also be used to manipulate the
qubit.
- E n t a n g l i n g qubits. The fundamental two-qubit quantum gate requires state-
selective interaction between two qubits, which is more delicate to implement.
A two-qubit quantum gate is a state-dependent operation such as a control
NOT gate:
FIG. 49. A possible implementation of a neutral atom qubit processor on an atom chip which
includes a reservoir of cold atoms in a well-defined state (for example a BEC or a degenerate Fermi
gas). From there the atoms can be transported using guides or moving potentials to the processing
sites. Either single atoms or small ensembles of atoms are then loaded into the qubit traps. Each
qubit can be addressed either by bringing light to each individual site separately, or by illuminating
the whole processor and addressing the single qubits by shifting them in and out of resonance
using local electric or magnetic fields created by the nanostructures on the atom chip. We think that
electric fields are preferable, since magnetic fields might produce qubit-state dependent phase shifts,
which have to be corrected. A different method would also be to address the single sites using field
gradients like in NMR.
mediate 'bus'. A light mode of a high-Q cavity can serve as such a 'bus'
acting on an array of atoms trapped inside the cavity (Pellizzari et al., 1995).
Atoms in high-Q cavities which in turn are connected with fibers, can also
act as a converting device between 'flying' qubits (photons) which transverse
distances, and storage qubits (atoms). The same principle can be used for
entangling atoms in different cavities for a 'distributed' computation process
(van Enk et al., 1998, 1999). In all of the above, the atom chip promises to
enhance the feasibility of accurate a t o m - c a v i t y systems.
- Input~Output. Even without high-Q cavities, an integrated atom chip, with
atoms trapped in well-controlled microtraps and with individual site light
elements, can probably provide input/output processes by making use o f
techniques such as light scattering from trapped atomic ensembles (Duan
et al., 2001), slow light (Hau et al., 1999; Vitali et al., 2000), stopped light
(Phillips et al., 2001; Liu et al., 2001; Fleischhauer and Lukin, 2002) or
macroscopic spin states (Duan et al., 2000; Julsgaard et al., 2001).
Let us summarize the road map for quantum computation with the atom chip:
one would need to implement
(a) versatile traps to accurately control atoms up to the stage of entanglement;
VIII] MICROSCOPIC ATOM OPTICS: FROM WIRES TO ATOM CHIP 351
(b) controlled loading of single qubits (atoms or excitations) into these traps in
well-defined internal and external states;
(c) manipulation and detection of individual qubits;
(d) control over decoherence; and
(e) scalability to be able to achieve controlled quantum manipulation of a large
number of qubits.
A schematic view of a possible realization is shown in Fig. 49.
VII. Conclusion
VIII. Acknowledgement
Foremost we would like to thank all the members of the Innsbruck, now
Heidelberg, atom chip group for their enthusiasm and the enormous effort they
put into the experiments. We would like to thank our long-time theoretical
collaborators Peter Zoller, Tommaso Calarco and Robin C6t6. The atom chips
for the Innsbruck-Heidelberg experiments were fabricated by Thomas Maier at
the Institut ft~r Festk6rperelektronik, Technische Universit~t Wien, Austria, and
by Israel Bar-Joseph at the Sub-micron center, Weizmann Institute of Science,
Israel. We would also like to extend a warm thanks to the entire atom chip
community for responding so positively to our requests for information and
figures. Our work was supported by many sources, most notably the Austrian
352 R. Folman et al. [IX
Science Foundation (FWF), projects S065-05 and SFB F15-07, the Deutsche
Forschungsgemeinschaft Schwerpunktprogramme: 'Quanten Informationsverar-
beitung' and 'Wechselwirkungen in ultrakalten Atom- und Molekfilgasen', and
the European Union, contract numbers IST-1999-11055 (ACQUIRE), HPRI-CT-
1999-00069 (LSF), TMRX-CT96-0002, and HPMF-CT- 1999-00235.
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A D V A N C E S IN A T O M I C , M O L E C U L A R , A N D O P T I C A L P H Y S I C S , V O L . 48
M.L. KEELER
Department of Physics, Wesleyan University, Middletown, Connecticut 06459
TODD A. Z I M M E R M A N and M. L A R S E N
Department of Physics, University of Wisconsin, Madison, Wisconsin 53706
PAUL FENG
Department of Physics, University of St. Thomas, St. Paul, Minnesota 55105
RENEE C. NESNIDAL
New Focus, Inc., Middleton, Wisconsin 53562
I. I n t r o d u c t i o n
target. In this chapter we describe a new type of atomic target: ultra-cold trapped
atoms (Schappe et al., 1995, 1996; Keeler et al., 2000).
An atom trap has three features that make it desirable for use as a target in
scattering experiments. First, the atoms in a trap can be confined to a very small
volume (diameter < 1 mm). Hence, an atom-trap target can be treated practically
as a point target of atoms. This property greatly simplifies the calculation of the
overlap of the target with the electron beam; absolute calibration can be done
without undertaking the difficult task of determining the profiles of both the
electron beam and atomic beam and then finding their convolution as must be
done in a crossed beam experiment (Mark and Dunn, 1985). Second, atoms in
a typical optical trap are cold, with temperatures on the order of hundreds of
gK or atomic speeds on the order of ten cm/s. Thus the atoms in a trap are for
all practical purposes at rest. Consequently, an atom that has undergone even
a weak electron-atom collision can pick up a sufficient atomic recoil velocity
to differentiate it from atoms that have not undergone a collision. Furthermore,
for the investigation of excited states, the linewidth of an atomic transition for
the trapped atoms is determined by the natural linewidth of the transition, and
not a Doppler profile. This vastly reduces the laser intensity needed to saturate
a transition. Third, atoms in the trap are constantly scattering photons from
the trapping laser beams and thus the trap fluorescence is directly proportional
to the number of atoms in the target. Because this signal is large ( - g W ) it
can be measured easily with excellent time resolution using even a simple
photodiode.
The high rate of photon scattering, Doppler-free transition width, and small
target size can be combined to yield a target with a large laser-excited state
fraction using only low-power lasers. For example, to study electron-impact
excitation out of the Na(3P) level with a conventional crossed beam target,
Stumpf and Gallagher (1985) needed -100 mW of laser power to create an
excited state fraction of~20%, while an atom-trap target can yield ~40% excited
state fraction with only ~10 mW of laser power (Keeler et al., 2000).
Collisions between cold atoms in a trap have been extensively studied since
the start of atom trapping (Walker and Feng, 1994; Weiner et al., 1999). To
our knowledge, however, the first application where all of the advantages of
using a trap as a separate target for measuring cross sections was the work of
Dinneen et al. (1992) on photoionization of Rb(5P). In their work, trapped atoms
were ionized (and thus lost from the trap) by a Kr-ion laser. Atom traps have
subsequently been used to study photoionization of the Rb(5D) level (Duncan
et al., 2001), and of the Li(2P) (Wippel et al., 2001), Na(3P) (Wippel et al.,
2001), and Cs(6P) (Marag6 et al., 1998) levels. Atom traps have also been used
in the study of heavy ion collisions (Flechard et al., 2001; Turkstra et al., 2001;
van der Poel et al., 2001).
In this chapter we describe the techniques for using trapped atoms for
II] ELECTRON-ATOM COLLISION CROSS SECTIONS 359
There are a number of issues involved in using a MOT as a target for collision
studies. Some of these issues are challenges; for example, a MOT relies on a
quadrupole magnetic field that interferes with the propagation of an electron
beam. On the other hand, the very complexity of atom trapping allows the
experimentalist many options for achieving a given task. For instance, the trap
(i.e., the confining and cooling forces) can be turned on/off in many ways:
(a) by turning on/off the magnetic field, (b) by modulation of the trapping laser,
or (c) by modulation of the hyperfine repump laser. Each method has its own
advantages and disadvantages in terms of complexity, cost, and time response. In
fact, there are a number of different natural time scales involved in the trapping
of atoms as listed in Table I. For example, if the trapping forces on a cloud of
trapped atoms are turned off for 5 ms and then restored, few if any atoms will
be lost from the trap. But, if the trapping forces are left off for 30 ms, all of the
atoms will be lost from the trap due to ballistic expansion. This sets a natural
upper bound on the time the trap can be left off. Alternatively, the decay time of
the magnetic field sets a lower bound on the time the trap must be turned off to
propagate an electron beam. Finally, we note that trap parameters and controls are
richly interconnected. For instance, to increase the fraction of trapped atoms in
the 5P excited level one might increase the photon scattering rate, which depends
on both the intensity and frequency detuning of the trapping laser. This will,
however, also affect the forces on the trapped atoms, which causes changes in
II] ELECTRON-ATOM COLLISION CROSS SECTIONS 361
Table I
Approximate times for processes in a typical Rb MOT
Process Time
the loading rate of atoms into the trap, the trap depth, and even the total number
of atoms in the trap.
emission. We conclude that the polarization of the cloud of trapped atoms (both
before and after the trap's anti-Helmholtz coils are turned off) is small (P < 0.1).
B. APPARATUS
In the following four sub-sections we describe the components of our atom trap
common to all our measurements: the laser system, the vacuum system, the
magnetic field coils, and the electron gun. Further details on the components
unique to each type of cross-section measurement are described in Sect. III.
B. 1. Laser system
The optics associated with the frequency stabilization of the trapping laser are
shown in Fig. 2, while Fig. 3 illustrates the optics associated with the trap. We
use a commercially available 30 or 70mW, 780nm diode laser in an external
cavity arrangement (MacAdam et al., 1992; Arnold et al., 1998) using a Littrow-
mounted 1200 groove/mm holographic grating for feedback. Tuning of the laser
frequency is achieved by varying the laser diode current and temperature, and
coarse adjustment of the grating angle. A piezo-electric stack is installed on the
horizontal grating adjustment to provide fine-control of the laser wavelength by
changing the effective cavity length.
The linearly-polarized, elliptical output beam from the diode laser is converted
into a circular profile with an anamorphic prism pair, and passed through a 40 dB
optical isolator to prevent disruptive optical feedback from retro-reflected laser
light. A Doppler-free saturated absorption spectrometer is used to determine the
laser wavelength relative to the Rb (52S1/2 F = 3 + 52p3/2 F t = 4) trapping
transition. Since we want to lock the laser to a frequency A less than this
trapping transition, we use an acoustic-optical modulator (AOM) to downshift
the frequency of the beam entering the saturated absorption spectrometer relative
to the trapping beam. Feedback from the saturated absorption spectrometer
(Wieman et al., 1995) is used to stabilize the laser frequency at the peak of
the crossover feature between the F = 3 ---+ F ' = 2 and F - 3 --+ F ' = 4
transitions, located 92 MHz below 52S1/2 F = 3 ---+ 52p3/2 F ' = 4 transition.
A single mode optical fiber is used to decouple the laser alignment from the
trap optics alignment and to provide spatial filtering.
A beam expanding telescope is used to convert the output of the optical fiber
into a collimated beam approximately 1 cm in diameter. The linearly polarized
laser beam is split into three beams using half-wave plates and polarizing
beamsplitter cubes. Since the magnetic field gradient is twice as large along
the axis of the anti-Helmholtz coils (the z-axis) as along the x and y axes,
the power in the beams are set in the ratio 2:2:1 so as to roughly equalize the
x , y , z restoring forces. The linearly polarized beams are converted into circularly
polarized beams with zero-order quarter-wave plates. Since the direction of the
II] E L E C T R O N - A T O M C O L L I S I O N CROSS SECTIONS 363
magnetic field gradient is opposite for the z-axis relative to the x&y axes, the
beam incident on the trap along the z-axis is left circularly polarized, while the
x&y beams are right circularly polarized.
The hyperfine repump beam is obtained by coupling a 2 . 9 1 5 G H z mi-
crowave modulation signal into the primary trapping diode laser drive current
(Feng and Walker, 1995). This modulation creates a sideband approximately
1% the intensity of the primary laser transition at the frequency of the
5281/2F = 2 ~ 5 2 p 3 / 2 F t -- 3 transition (see Fig. 1). Since only -1 in
200 photons result in a Raman scattering event that populates the dark state,
this weak sideband intensity is enough to keep the dark state essentially empty.
If, however, the hyperfine repump is turned off (by shifting the microwave
364 Schappe et al. [II
FIG. 3. Top view of the atom trap chamber (and optics) used in electron-impactexcitation studies
(Sect. III.B.4), but contains all the elements used in our earlier trap-loss measurements(Sect. Ill.A).
Photodiode and CCD camera are used to monitor the trap. For clarity, the z laser beam and associated
optics are not shown.
laser frequency is very stable (< 1 MHz), typically remaining locked >48 hours
at a time, with an observed variation in trap fluorescence over 24 hours (due to
changes in laser intensity and frequency) of ~< 5%.
uniform field gradient. Typically, we run 4.0 A through each coil to generate
a measured magnetic field gradient of 9Gauss/cm along the z-axis, although
trapping is possible over a wide range of currents (2 to 18 A).
Since the trapping magnetic field deflects the electron beam, the magnetic field
must be switched off during electron beam pulses. We have used two circuits to
perform this function, one using a power MOSFET as a switch, and one using a
commercial solid-state relay. We measure the effective decay rate of the magnetic
field by monitoring the temporal distortion in the shape of an electron beam
current pulse. The minimum measured delay between the time the magnetic field
is switched off and the start of the electron beam pulse that does not distort the
electron current is 500 ~ts, which is comparable in performance to slightly more
advanced switching circuits with eddy-current compensation (Dedman et al.,
2001).
The center of the trap is determined by the location of the minimum in the
magnetic field, while the optimum trap fluorescence and trap-loading rate are
located at the intersection of the six laser beams. We use the vacuum chamber
to align the two; the coils are attached to the top&bottom viewports, and the
laser beams are centered on each viewport. The most uniform trap, however, is
achieved by using magnetic field shim coils to steer the magnetic field 'zero'
to the intersection of the laser beams. The quality of the trap alignment can be
monitored by observing the dispersal of the atom cloud when the magnetic field
is turned off. For a well aligned trap the atoms disperse isotropically ("poof"),
but for a poorly aligned trap the atoms move off in a directional jet.
The electron gun used in this work consist of five grids and a cathode assembly.
The stainless steel grids are 1.78 cm square with alumina spacers between grids.
The cathode consists of an indirectly heated BaO cathode. One of the grids can
be biased negative relative to the cathode to chop the beam on and off. The
electron beam current is measured by a deep Faraday cup (L/D ,~ 5). The back
plate of the Faraday cup is conical so that specularly reflected secondary electrons
are not reflected back towards the collision region. The back plate is also biased
at +18 V to prevent the escape of low energy secondary electrons. The electron
gun and Faraday cup are separated by distance of 4.5 cm to allow the trapping
laser beams access to the collision region. Space charge expansion of the electron
beam over this distance limits the low energy performance of the electron gun.
To determine the electron beam current density, J, we translate a thin (0.19 mm
diameter) tungsten wire across the electron beam at the location of the atom trap.
The current measured on the wire produces a series of line integrals of the beam
current density. Assuming the beam is cylindrically symmetric, the measured
beam spatial profile is converted into the current density J ( x , y ) using an Abel
transform (Hansen and Law, 1985). Due to secondary electron emission from
III] E L E C T R O N - A T O M C O L L I S I O N CROSS SECTIONS 367
Fl~. 4. Profile of the electron beam (100 eV) at the location of the trap. Measured current values as
the wire is traversed along the x-axis are deconvoluted with an Abel transform assuming cylindrical
symmetry. The current density is essentially constant over the size of the atom cloud (~< 0.1 cm).
the wire, we only use the translating wire measurements to find the shape o f
the current density. We put J on an absolute scale using the total electron beam
current measured by the Faraday cup. At high energies (>100 eV) the beam is
approximately Gaussian, with a F W H M of 2 mm at high energies (see Fig. 4).
The value of the peak current density ranges from 0.1 mA/cm 2 at low energies
to 3 mA/cm 2 at high energies.
Due to the small size of the atom trap, the electron beam is carefully aimed
at the atom cloud by using a set o f gimbals (particularly for the trap-loss
measurements described in Sect. III.A). The decrease in trap intensity due to
electron-atom scattering collisions can be used to aim the electron beam at
the trap. Due to residual magnetic fields and the build-up of surface charge
on insulators, the center of the electron beam has some dependence on the
electron beam energy, requiring that this alignment must be repeated for different
energies.
the number of atoms in the trap; the low initial velocity of atoms in the trap
differentiates electron-scattered atoms, and the small size of the trap simplifies
the absolute calibration. On the other hand, the second class of experiments
(Keeler et al., 2000) uses the high excited state fraction in the trapped atom
target to measure ionization and excitation cross sections from the laser excited
5P level and is described in Sect. III.B.
dN
- A L - r0N - f G N , (1)
dt
where L is the loading rate of atoms into the trap from the background vapor, F0
is the loss rate of atoms out of the trap for all causes other than electron-atom
collisions, Fe is the loss rate of atoms out of the trap due to electron collisions,
J~ is the fraction of time the trap is on, and f is the fraction of time the electron
beam is on. For a vapor loaded trap, the loading rate, L, depends on the Rb partial
pressure in the chamber and the laser detuning and intensity. Atoms can only be
loaded into the trap during the fraction of time, J~, when both the trapping lasers
and magnetic field are 'on'.
The loss rate of atoms out of the trap when the electron beam is off,
F0, is due to a number of causes. At very high trap densities, atom-atom
collisions within the trap are the largest loss mechanism, while at lower densities
collisions with hot background gas atoms become important (Walker and Feng,
1994) 3. Additionally, when the trap is turned off, all of the formerly trapped
atoms ballistically expand away from the center of the trapping region with a
velocity dependent on the temperature of atoms in the trap. If the trap is turned
back on after only a very short delay, these atoms are retrapped with almost
100% efficiency. For longer delay times, this ballistic expansion allows atoms to
3 Since the asymptotic number of atoms in the trap is different with and without the electron beam,
to eliminate any possibility of density-dependent changes in F0, one should vary fL so that N~ is
the same in both cases.
III] ELECTRON-ATOM COLLISION CROSS SECTIONS 369
escape the physical limits of the trapping laser beams, thus depleting the number
of atoms in the trap. The average (rms) speed of Rb atoms in a 150 ~tK trap is
21 cm/s. For a laser beam of radius 0.5 cm, atoms leave the trapping volume in
about 24 ms. Since the atoms have a Maxwell-Boltzmann velocity distribution,
and the laser beam has a Gaussian profile, this is not a well-defined time limit.
Gravity will also eventually pull atoms out of the trapping region. The time
it takes to fall 0.5 cm is 32 ms, which is only slightly longer than the ballistic
expansion time for Rb.
Solving Eq. (1) with the initial condition that there are no atoms in the trap,
the number of atoms in the trap as a function of time (a loading curve) is simply
where N ~ is the steady state number of atoms in the trap, and is equal to
j~L/(F0 +fFe). If the electron beam is always off, the form of the solution is the
same, except Fe = 0. By fitting a rising exponential to two sets of experimental
d a t a - one with the electron beam on, and one with the electron beam o f f - F~
can be separated from the background loss rate.
The loss rate due to electron collisions, F~, is directly related to the
corresponding electron-atom collision cross section, o, by
oJ
r~ - , (3)
where J is the current density of the electron beam at the location of the trap,
and e is the magnitude of the electron charge. Note that since the size of the
trapped atom cloud is small compared to the size of the electron beam, we can
safely assume J is constant over the volume of the trap. Furthermore, in contrast
to the general difficulties of crossed beam experiments, for an atom-trap target
the only measurements needed to find absolute cross sections are the electron
beam current density (see Sect. II.B.4) and the change in the loss rate with the
electron beam on/off. There is no need to measure the absolute number of target
atoms.
By varying the delay time between the electron beam pulse and the time the
trap is turned back on, T, it is possible to measure different types of collision
cross sections. To measure total scattering cross sections (Sect. III.A.2), we use
a long delay. With a long delay, any atom that has gained any excess recoil-
momentum due to an electron-atom collision will have enough time to leave the
trapping region. On the other hand, if the trap is turned on immediately after
a short electron gun pulse, recoiling atoms will not have had enough time to
leave the trapping region, and will be retrapped. Ions formed via electron-impact
ionization, though, are not resonant with the trapping lasers, and are lost. Thus
only ionizing collisions result in trap loss, allowing us to measure ionization
cross sections as is described in Sect. III.A.3.
370 Schappe et al. [III
Hyperfine~ o f f - - I ton = 30 ms
Magnetic
Field
one, ~ i ~'"
off/ ~,.
i"~
-IT= 0- 18 ms
a
Electron
Beam
off n 0.8 - 4 ms
FIG. 5. Timing diagram for total scattering experiment. The electron beam pulse is delayed from
the the start of the trap-off phase to allow time for the magnetic field to decay (dashed lines).
Total scattering cross sections (Schappe et al., 1995) are obtained by monitoring
the time dependence of the trap fluorescence as the trap is periodically hit with
an electron beam pulse. A timing diagram of one electron beam pulse cycle is
shown in Fig. 5. Atoms are loaded'into the trap for 30 ms, at which time both the
magnetic field and hyperfine repump are turned off. With no repumping, Raman
scattering shifts atoms into the F = 2 dark state of Rb, which is non-resonant with
the primary trapping laser. Before pulsing the electron beam, however, a delay of
1 ms is needed for the decay of the magnetic field. After a short electron beam
pulse (0.8 to 4 ms long), the trap is left off for a variable time of 0 to 18 ms.
At the end of this delay, the trap is turned back on (i.e., hyperfine repumping
is resumed and the magnetic field is turned on) and the number of atoms in
the trap is recorded. After acquiring trap fluorescence data for approximately
12 s, the number of atoms in the trap reaches the asymptotic value, N ~ . To
obtain another loading curve, the magnetic field is turned off for 2 s to empty
the trap, and the above process is repeated. A loading curve is also obtained
with the exact same timing structure, but without the electron beam to obtain
the background trap-loss rate F0. Typically, the results from five pairs of loading
curves are averaged together to reduce the statistical noise in the data.
The relative number of atoms in the trap, for a fixed laser intensity and laser
detuning, is proportional to the trap fluorescence. This fluorescence is collected
by a lens and detected with a photodiode. The -50 nA signal is amplified by a
current to voltage amplifier with a gain of 6 x 107 V/A and recorded by either a
digital storage oscilloscope or a data acquisition computer. The computer is also
used to control the timing of the electron beam, magnetic field, and hyperfine
repumping.
In Fig. 6 we show a pair of sample loading curves with and without an electron
beam. The trap fluorescence demonstrates a slow exponential rise due to atoms
being loaded into the trap via Eq. (2), superimposed on a rapid modulation due
III] ELECTRON-ATOM COLLISION CROSS SECTIONS 371
no e l e c t r o n b e a m .= ..,--,,..:~.
9
" b ~ - _-~r"or'-=~.,L
lb--
l
- ~
l
9 --o
I
.Q
v 3
~
e"
2 e l e c t r o n beam
m
e~
0
0 2 4 6 8 10 12
Time (s)
FIa. 6. Sample loading curves for an electron beam energy of 50 eV with a 2 ms electron beam
pulse and 13 ms delay time. The data presented in the main plot has been averaged over one full
pulse cycle (46 ms). The raw data for the start of the electron beam off loading curve (shown in the
insert) demonstrates the rapid time dependence of trap fluorescence on the modulation of hyperfine
repumping.
4 Technically F0 is not fully time independent, since the background loss rates are different when
the trapping lasers are on or off. While some high-frequency residuals in the fit can be removed by
including a two parameter background loss rate, only the time averaged value is needed to extract
the electron-impact induced loss rate.
5 Only data averaged over integer multiples of a timing cycle will produce fits with no spurious
high-order frequency components and valid Z2 values.
372 S c h a p p e et al. [III
20 eV
g..
E 6
T--
v
e- 4
0
co
0
2 250 eV
o
. i . i , i . i , I l I , I , i
0
0 2 4 6 8 10 12 14 16
Delay Time toff (ms)
Fie. 7. Variation of loss rate, and thus cross section, with delay time.
using a laser-slowed atomic beam that could be switched off during loss rate
measurements. Alternatively for a vapor loaded trap, the decay can be measured
for a short time interval if the trapping lasers are turned off so that there is no
loading term. The presence of the loading term in Eq. (1) also complicates the
extraction of loss rates from monitoring only the asymptotic number of atoms
in the trap, N ~ . Relative measurements of loss rates (and thus cross sections)
can be obtained by monitoring the equilibrium number of atoms in the trap with
and without an electron beam. But since N ~ = f L L / ( F o + f F e ) , knowledge of
the loading rate is necessary to place these results on an absolute scale. Hence,
while being less intuitive, we have found the loading curve method to be easier
to implement and analyze experimentally.
The measured electron-induced loss rate varies with the delay time as is shown
in Fig. 7. For short delay times, only atoms with a very large recoil velocity have
sufficient time to leave the retrapping region before the trap is turned back on.
Kinematically, the relation between the recoil velocity of the atom, V, and the
scattering angle of the electron, 0, is (McDaniel, 1989)
2E0 - AE M(m+M) V 2
COS 0 = 2m , (4)
2 ~Eo(Eo - AE - 89M V 2)
6 At 10 eV all inelastically scattered atoms via 5S-5P excitation have recoil velocities in excess of
100 cm/s, and are thus included for delay times in excess of 5 ms. For elastic scattering (at 10 eV),
a delay time of 18 ms corresponds to 0mi n ~1.6~
III] ELECTRON-ATOM COLLISION CROSS SECTIONS 373
longer delay times allow more of these slow moving atoms to escape, which is
equivalent to probing electron-scattering angles closer to 0 ~ Thus the measured
trap loss corresponds to the integral of the relevant differential cross sections
where T is the delay time, d o / d ~ is the "total" differential cross section, and
Omin(T)is found from Eq. (4) assuming V = r/T with r being the effective radius
of the retrapping zone. Since the data in Fig. 7 converges to an asymptotic value
well before the maximum delay time, we can be assured that our total scattering
cross section measurements include the contribution down to all non-negligible
scattering angles.
In principle, since there is a functional relationship between delay time and
the electron scattering angle, the derivative of the trap loss vs. delay time curve
can be used to measure differential cross sections,
do d0min do
d---~(T) = -2:r dT (T)~-~(0mi,) sin 0min. (6)
For electron energies below the first excitation energy (-2eV), this would
correspond to the elastic scattering differential cross section. On the other
hand, at very high energies the elastic cross section is negligible, leaving
only contributions from excitation into all bound levels because the ionization
component does not contribute to the variation of trap loss with the delay time as
the ions are never retrapped regardless of the delay (see Sect. III.A.3). For alkali
atoms the nS ~ nP excitation cross section dominates all the other nS ~ n~L
excitation cross sections (Phelps et al., 1979). It may be possible to utilize a
detailed measurement of the trap loss as a function of the delay time to obtain
information about the 5S ~ 5P differential excitation cross section at very small
scattering angles, which is difficult with conventional methods. The effective
angular resolution of such a measurement is limited by the length of the electron
beam pulse, the number of data points, and the quality of the trap model used
to relate the atomic recoil velocity (V) to the delay time (T).
As indicated by the simplicity of Eq. (3), there are only two measured
quantities, and hence only two major sources of uncertainty, that enter into
the determination of the cross section. The measurement of the peak current
density which is obtained by taking the Abel transform of the translating thin-
wire electron beam profile has an estimated uncertainty of 7%. The uncertainty
in the extraction of the electron-induced trap-loss rate Fe from fitting the loading
curves, and finding the asymptotic delay time value is estimated to be 6%.
Results obtained over a wide variety of trap parameters (laser intensity, detuning,
laser beam diameters, trap size) and experimental parameters (electron beam
pulse length, electron beam spatial width, trap on time) give consistent results.
374 Schappe et al. [III
Trap
off
1 ton=-10-20 ms J I
Oil
Thus, in the apparent absence of any secondary effects, we believe the total
uncertainty in our measurements is about 9%.
One very important secondary effect that can complicate measurements made
with the trap-loss technique is electron stimulated desorption (ESD) of Rb atoms
from the Faraday cup. The background trap loss is dominated by collisions
of trapped atoms with background gas atoms in the trap. Any increase in the
background gas pressure synchronous with the electron beam will appear to
be due to electron-atom collisions and will be erroneously included in Fe.
Due to the low operating pressure of the trap chamber, the small number of
atoms/molecules liberated from the Faraday cup by ESD can significantly change
the background gas number density. For example, we have observed the pressure
in the chamber rise from 10 -9 to 10 -7 Torr when the electron beam first hits
the Faraday cup in a chamber that was pumped down after being opened. Two
actions minimize the ESD-induced gas load: the chamber is baked out at 250 ~
for 48 hours to remove as much contamination from the chamber as possible,
and before data is collected the electron beam is left on at a high current
(100 to 400 gA) for an extended period of time. Data is only acquired after the
pressure in the chamber is the same with the electron beam gated on or off.
As described in Sect. II1.A, if the trap is turned on immediately after the electron
gun pulse, most of the trap losses will be due to ionization since the ions are
non-resonant with the trapping laser which is tuned to an atomic transition. As
seen by the timing diagram in Fig. 8, the ionization experiment is very similar
to the previously described total scattering experiment. The trap is periodically
turned off by turning off the magnetic field and hyperfine repump. After the delay
needed to allow the magnetic field to decay, the electron beam is turned on for
a short pulse (0.167 to 2 ms). The trap is turned on immediately following the
electron beam pulse and the trap fluorescence is recorded. New atoms are loaded
into the trap for 20 ms and the process is repeated. Note that the cross section
measured with this technique is related to the number of ions created (or the
III] ELECTRON-ATOM COLLISION CROSS SECTIONS 375
1.75 . . . . . ! . . . . ! . . . . ! 9 , , ~ 1-
1.50
50 eV
1.25
,~ 1.00
IT" 0.75
2 5 0 eV
co
o~
0
--J 0.50
G)
._
0.25
n'-
0.00 | | | , l i i i | i , ,
FIG. 9. Variation in trap-loss rate versus the width of the electron beam pulse. At high electron
energies, collisions are mainly small-angle electron scattering (low atom recoil). At low energies
(50eV), however, large-angle (fast atom recoil) scattering is more evident. Measurements at widths
less than 0.2 ms are dominated by trap-depth effects.
number of atoms lost from the trap), and does not depend on the charge state of
the ion produced, i.e., we measure ~rion
"count defined as
ount = ~
O-ci o n
ok+, (7)
k
7 It may be possible to overcome this limitation on measuring 5P total scattering cross sections,
however, by shifting the red-detuned trapping laser beam directly onto resonance. On resonance, the
absorption and emission of photons does not provide any net force to the atoms - it will, however,
rapidly heat them, leading to increased background trap-loss rates which may pose a new problem.
III] ELECTRON-ATOM COLLISION CROSS SECTIONS 377
while excitation cross sections out of the 52p level are described in Sect. III.B.4.
Both of these measurements, however, depend upon an accurate measurement of
the excited state fraction.
Generally, it has been the practice to calculate the expected excited state fraction
based upon the known laser intensity (Walker and Feng, 1994). If we assume the
trapped atoms can be treated as a simple two level atom, stimulated emission
limits the maximum excited state fraction, fe, to be 0.5 or less in steady state.
As a function of the laser intensity, I, the fraction of excited atoms in the trap
is (Metcalf and van der Straten, 1999),
1 I/Is
fe - 2 1 + I/I, + 4A2/F 2' (8)
;rhc
/" 3/Pr (9)
through a small aperture approximately the size of the trap (d = 1 mm). If the
laser beams are well aligned, the total laser intensity is simply the sum of the
peak intensities of the six counter propagating laser beams. Any misalignment of
the beams, or unaccounted-for losses at windows, etc., would introduce an error
into this value. Additionally, for our laser not all of the measured laser power
is available for excitation into the 52p3/2F' = 4 level since some of the laser
power is in the hyperfine repumping sidebands.
Due to these complications, we instead determine the excited state fraction of
the trap by fitting a surrogate measure of the excited state fraction to Eq. (8)
using Is as a parameter. In steady-state, the 5P ~ 5S trap fluorescence is equal
to the number of 5P atoms in the trap times the transition probability for the
5P ---. 5S transition. The number of 5P atoms in the trap is simply feN where
N is the total number of atoms in the trap. Thus, for a fixed number of trapped
atoms, the trap fluorescence is directly proportional to the excited state fraction.
The number of atoms in the trap, however, generally depends upon the laser
intensity, detuning, and a vast variety of other parameters. To keep the number of
atoms in the trap constant, the trap is always loaded with the same laser intensity,
/Load. A fast variable attenuator is then used to rapidly switch to a new laser
intensity, Im, and the trap fluorescence is recorded. These relative measurements
of the excited state fraction as a function of the easily measured laser power are
then fitted to the shape of Eq. (8) with I~ as the only free parameter (i.e., the
asymptotic value is forced to 0.5).
A liquid crystal variable retarder (LCVR) followed by a linear polarizer is used
to rapidly attenuate the trapping laser intensity. The response time of the LCVR
we use is on the order of 10ms. Few atoms are lost out of the trap in 10 ms,
even with a full attenuation of the laser intensity. However, ballistic expansion
of the atom cloud in this time may affect the overlap of the laser beam and
atom cloud for very low attenuation powers. This effect should be minimal for
Im >~ 0.05ILoad. The trap fluorescence is monitored with a photodiode in the
same way as that used in our trap-loss measurements. Since the photodiode also
detects scattered laser light (and fluorescence from background atoms), we take
the difference of two measurements: one with the trap on, and one with the trap
off obtained by turning off the hyperfine repump.
A sample plot of excited state fraction versus laser intensity is shown in
Fig. 10 for a laser detuning of 9.9 MHz and maximum laser power of 6 mW (total
power before being split into separate beams). The fitted value of the saturation
intensity, 3.5 mW/cm 2 falls within the range of expected values. Interestingly,
the horizontal scaling of Fig. 10 is irrelevant, e.g., we plot fe versus laser power
instead of laser intensity as in Eq. (8). If we assume the calibration of the
horizontal scale is off by some scale factor (e.g., not properly accounting for
window losses), our fitted Is value will be off by the same factor. However, the
vertical scale, and thus the extracted f~ value, is unaffected.
III] ELECTRON-ATOM COLLISION CROSS SECTIONS 379
0.5 . , . , . , . , . , . , . , . , . , .
0.4
.o
0.3
LL
0.2
._
x
UJ
0.1
0.0 . . . . . . . . . .
L a s e r P o w e r (mW)
The one underlying (and possibly problematic) assumption made by using the
trap fluorescence as a surrogate forf~N is that the atoms in the trap are assumed
to be in either the 52SI/2 F = 3 or 52P3/2 F ~ = 4 levels. However, if the hyperfine
repump laser is at a low intensity, a substantial number of atoms in the trap will
be in the 5 2 3 1 / 2 F = 2 dark state. Assuming the microwave modulation induced
sidebands for hyperfine pumping are 3% of the intensity of the primary trapping
laser intensity, we calculate <~ 5% of the atoms are in the F = 2 dark state at any
one time. This has a negligible effect on our f~ measurements. If the intensity
of the sidebands is reduced to 0.5%, the fraction in the dark state soars to 22%.
To verify that there are essentially no atoms in the dark state we increase the
size of the microwave-modulation sideband intensity until the trap fluorescence
is essentially independent of the repump intensity.
I trapoZ.
Hypermfi;e~' 5"~on'~Ysigna 1
I
~ 5S&5P mixed signal
i_ .I
Electron Beam [0.6 ms-]
Ion Extractor
FIG. 11. Timing diagram for measuring ionization out of the Rb(5P) level. The target is controlled
by turning the hyperfine pumping laser on and off: no trapped atoms are present when it is always
off, a 5S target is achieved by turning it off only during the electron beam pulse, and a mixed
5S&5P target is obtained by leaving it on during the electron beam pulse.
sources, the Cmix signal includes a contribution from the fraction of atoms in
the excited state, fe Ssp, and a contribution from the fraction of atoms in the
ground state, (1 - f e ) Sss. Hence,
In general, the electron-impact signal rates (BG, S5s, S5p) depend upon a vast
collection of experimental parameters including: the electron beam current, the
number of target atoms (in the trap and in the background vapor), and the 52S
and 52p ionization cross sections. Assuming a constant number of atoms in the
trap for both the 52S and mixed 52S & 52p targets, and a constant overlap of
the electron beam with the trapped atoms, it is possible to find the ratio of the
52p to the 52S ionization cross sections from the expression
16 Rb++ Rb +
.mr 12
~ 8
r- 4
._~
o 0
m 2 3 4 5 6 7 8
Time (gs)
Fie. 12. Time of flight spectra for detection of Rb ions at 150 eV. The dotted line is background
only (no trap), the solid line is with an atom trap target (53 only).
CEM detector assembly) receives a high voltage pulse. After the ion signal
is recorded, the magnetic field is turned back on. To replace atoms lost in
electron-atom collisions, additional atoms are added to the trap for 100 ms. We
obtain reasonable signal rates by averaging counting rates for 300 pulses, which
corresponds to 30 s.
To obtain a signal from only trapped atoms in the 5231/2 F = 2 dark state,
the hyperfine repump is turned off for the duration of the electron-beam pulse.
A mixed 523 & 5 2 p target is obtained by leaving the hyperfine repump on during
the electron beam pulse. To maintain a constant number of atoms in the trap for
the two cycles the hyperfine pumping is turned off for 0.6 ms shortly before the
electron beam pulse to maintain a constant repump duty cycle. A background
run (no trap) is obtained by leaving the hyperfine pump (or magnetic field) off.
When switching from the trap off data run to one of the trap signal runs, we first
reload the trap for 10 seconds before acquiring data.
A time of flight spectra at an electron energy of 150 eV is shown in Fig. 12.
Singly ionized Rb atoms from the trap arrive at the detector at (4.5+0.5)~ts. As
seen in Fig. 12, ions formed by ionization of background gas atoms arrive at the
detector with a much broader range of arrival times, approximately (3.5+2)~ts.
To maximize the SNR ratio, the ion signal is recorded with a box-car integrator
with a signal gate centered 4.5 ~ts after the start of the ion-extractor pulse with
a total width of 1 ~ts. Based upon the arrival time of the Rb + ions, the Rb ++ ions
are expected to arrive at the detector at 3.2 pts, versus an observed peak arrival
time of 2.9 pts. This illustrates another advantage of the trapped atom target in
that the Rb + and Rb ++ yields can be determined separately by means of a simple
time-of-flight detection system.
The largest single source of ions in this experiment is from ionization of
background gas atoms. The number of ions produced by the electron beam is
proportional to f n(F)J(F)dY, where n is the number density of atoms, and J is
the electron beam current density. For ionization of trapped atoms, this is equal
to NJo, where N is the number of atoms in the trap, and J0 is the current density
382 Schappe et al. [Ill
at the trap location. For ionization of atoms in the Rb background vapor, ions are
created along the entire length of the electron beam from the electron gun to the
Faraday cup. The number of background ions created is proportional to nscleL,
where nBc is the number density of background atoms, Ie is the total electron
beam current, and L is the effective length of the electron beam from which ions
are extracted into the detector. Using typical values (N ~ 106, J0 ~ 2 mA/cm 2,
nsa ~ 109 cm -3, Ie ,~ 100gA, L ~ 1 cm), the ion yield from the background
vapor is a factor of fifty larger than the ion yield from the trap. Two factors help
minimize the contribution from background gas ionization: (1) the ion-extractor
is designed to minimize the effective range L from which ions are collected (since
ions from the trap are well localized at the trap center), and (2) TOF selection is
used to separate the 'cold' trap ions from the 'hot' ions created by ionization of
room temperature background gas atoms. Details about the design and operation
of the ion extractor are given in Keeler et al. (2000). Computer modeling of
ion trajectories indicate that the transmission of the ions to the detector is
essentially constant for ions within +0.25 cm of the extraction axis. In principle,
the extractor could be designed to have a smaller extraction volume (i.e., the size
of the ball of trapped atoms) to further eliminate the inclusion of background gas
ions, but this would require the placement and alignment of the extractor relative
to the cloud of trapped atoms to tolerances beyond our control. To maximize the
alignment of the trap to the fixed location of the ion-extractor, shim coils are used
to move the zero of the trapping magnetic field. The contribution from ionization
of background gas atoms can also be improved by switching from a vapor loaded
trap to one fed by a collimated, slowed atomic beam.
The estimated uncertainty in our o+(5P)/o+(5S) measurements is on the order
of 28%. The 52p ionization cross section is obtained by multiplying the measured
ratio in Eq. (11) by the ionization cross section out of the 52S ground state. Note
that the total ionization cross section measured in Sect. III.A.3 using the loss-
rate technique (Schappe et al., 1996) is the sum of the Rb +, Rb++, ... ionization
cross sections, i.e., Eq. (7). Thus the contribution from higher ionization levels
must be removed before these values can be used to place the 52p results on an
absolute scale. Combining the uncertainties in the ratio measurement, the ground
state total ionization cross section, and the correction of Ocount to o +, the total
uncertainty in our 52p cross sections (Keeler et al., 2000) is estimated to be
+33%.
It is interesting to compare the 52p ionization cross-section results obtained by
direct detection of the ions with those using the trap-loss technique as described
in Sect. III.A.4. The loss-rate measurements must be interpreted with some
trepidation since the method forces us to assume that loss rate from atoms in the
trap during a brief electron beam pulse is the same if the hyperfine repumping
is on or off. That is, the recapture rate of atoms is the same for 52S atoms with
no optical molasses and for a mixture of 52S and 52p with an optical molasses.
III] ELECTRON-ATOM COLLISION CROSS SECTIONS 383
Nonetheless, at 50 eV, the loss rate measurement (Keeler et al., 2000) yields a
total ionization cross section of 2.2x 10-15 cm 2 in remarkably good agreement
with the o+(5P) direct detection value of (2.5+0.7)x 10-15 cm 2.
Accounting for the solid angle of the optical system, and assuming a typical
cross section value of 10- 1 6 cm 2, and an effective electron beam current of 10 gA
passing through the trap volume, the electron-impact excitation signal is expected
to be approximately 3 x 10-14 W. If we are measuring the excitation cross section
out of the laser-excited level, the atoms in the trap will be fluorescing at the
same time we are looking for electron-impact excitation signal. The 780 nm trap
fluorescence radiated into the solid angle of the optical system is approximately
2 x 10-6 W. Note that as this light is co-located in space and time with the electron
excitation signal, the only way to remove it is by wavelength selection. For a 1 nm
FWHM filter centered at 795 nm, the transmission at 780 nm is ~ 10--4. With only
10 -4 attenuation, the trap fluorescence is four orders of magnitude larger than
the expected excitation signal, hence the need for the holographic notch filters
which have a high transmission (>80%) at all wavelengths except the 780nm
laser wavelength. Another source of scattered laser light arises from a beam
reflecting off of surfaces near the trap region. For example, to keep the space
charge spreading of the electron beam to a minimum, the electron gun is located
within 12 mm of the collision region. For a laser beam with a 1/e 2 diameter of
1 cm, we might expect ~1% of the beam to be reflected off of the electron gun.
For an average beam power of 3 mW, this corresponds to 3 x 10-s W of scattered
780nm light. Two additional measures beyond the wavelength-selection filters
are used to minimize this light source. First, surfaces close to the viewing region
are coated with colloidal graphite which has a measured reflection coefficient of
<1% at 780 nm. Second, since this light does not originate at the exact location
of the trap, most of the scattered light can be removed by limiting the viewing
region to the trap volume.
Data is taken in three phases similar to those used in the 5P ionization
experiment (see Sect. III.B.3). However, in comparison to the ionization
experiment where there were four major sources of ion counts (two signal sources
and two background sources), there are seven major sources of photon counts
(two signal sources and five background sources). A detailed description of these
sources and typical count rates from each source are listed in Table II.
The signal is extracted from these numerous background sources using the
timing cycles shown in Fig. 13. In the first phase two counting gates are used.
Within each of these gates the electron gun is on half the time and the hyperfine
repump is on half the time. In the A-gate the timing of electron beam and laser
pulses are synchronous, while in the B-gate the two pulses are asynchronous.
When the pulses are synchronous, the resulting signal is from a mixed 52p &
52S target, while the asynchronous gating produces excitation from only the
52S level. This leads to a very simple determination of the relative difference of
the 52p and 52S signal rates. Using the definitions provided in Table 2:
A1 = 2 S L + 2L + B G + B F + T F + (1 - f e ) E s + f e E p , (12a)
B 1 = 2 S L + 2L + B G + B F + T F + E s , (12b)
III] ELECTRON-ATOM COLLISION CROSS SECTIONS 385
Table II
Light sources in an atom-trap experiment measuring the optical emission cross section for the i ~ j
transition
Excitation from the laser excited 52p level into level i /l~j 100
Excitation from the 52S ground state into level i /lij 130
BG Excitation of background gas (52S) atoms into level i /1#- 6
TF Trap fluorescence ~rap 1
BF Fluorescence from background gas /1trap 1
L Scattered laser light /1trap 2
SL Other stray light sources (i.e., cathode blackbody emission) all/1 20
a Relative signal sizes are based upon measurements of the 52P1/2 ~ 52S1/2 optical emission
cross section, after taking all measures to reduce scattered laser light at/1trap = 780 nm.
L 1.35 ms .L 37.8 ms J
Magnetic Field [ i
i
i
T i
! i i
i
i
I
! r
Hyperfine Pump
~0.50 ms'],,
9 !
Magnetic Field I i il
[
.ypo ne um I iil
Electron Beam l !
0.25 ms
Hyperfine Pump !
Electron Beam [ i
|
FIG. 13. Timing diagram for 5P electron-impact excitation experiment. Phase-1 measures
excitation from the mixed target. Phase-2 measures excitation from the 5S target, and Phase-3
measures the background. We accumulate counts in each phase for 2000 cycles (~100 s).
386 Schappe et al. [IV
SO
A1 - B1 : fe(Ep - Es). (~3)
In phase two, we record the electron-impact excitation signal from the trap, but
with the hyperfine repumping off during the entire counting gate; hence signal
arises only from excitation of the 52S level. Phase three is the same as phase
two, except the hyperfine repump is always off, so we never have a trap. The
difference in these two counts gives the signal rate for excitation of trapped atom
in the 52S ground state,
The signal rates Es and Ep are proportional to the cross sections for the
respective 52S ~ n2L and 52P ---. nZL electron-impact excitation processes.
In addition, they are also proportional to the total number of atoms in the trap,
the electron beam current density at the location of the trap, the optical system
detection efficiency, and the branching ratio of the particular nL ~ n~L ' transition
observed. All of these other factors, however, are the same for excitation from
both the initial levels, so the ratio of cross sections can be found from the ratio
o(SeP--~neL)_ 1 (A1-B1)
o(52S~n2L) fe A 2 - A 3 +1. (15)
Thus the unknown o(52P -~ n2L) excited state excitation cross section can
be found from the four photon counter readings, the measured excited state
fraction (see Sect. III.B.2) and the known o(52S -~ n2L) ground state excitation
cross section.
Due to the large amount of background light, the signal to noise ratio of
these measurements is very low. Long counting times (-2 days per energy)
are needed to reduce the statistical uncertainty in our measurements to less
than 10%. We estimate the total uncertainty in our measurements including
that from the f~ measurement and from the uncertainty in the ground state
excitation cross section to be 35%. Preliminary measurements for excitation
into the 72S indicate that the 52p ~ 72S cross section is significantly
larger than the 52S -+ 72S cross section as predicted by earlier theoretical
calculations (Krishnan and Stumpf, 1992). A further discussion of the results
of this experiment is outside the scope of this chapter and will be published
separately.
IV. Conclusions
the need for beam profile and overlap calculations. The low temperature (low
velocity) of the trapped atoms makes them very sensitive to collisions so
that even small angle scattering (low-recoil) events can be detected. Accurate
measurements of the relative trap population are made by simple measurements
of the trap fluorescence and suitable experimental design can eliminate the need
to determine the absolute target density. These distinctive features allow trap-loss
rate measurements which produce very accurate total scattering cross sections
(uncertainty <10%) that include scattering events down to very shallow angles.
Trap-loss measurements also produce ionization cross sections out of the ground
state with uncertainties of < 14%. Also, it is possible to create a trap target with
a significant and well-known fraction of atoms in an excited state. By directly
detecting the collisionally excited atoms (or ions), it is also possible to measure
ionization and excitation cross sections out of the 5 2 p laser-excited level.
Our present discussion has mainly been limited to measuring Rb cross sections
with an atom trap. However, a wide variety atomic species can be trapped,
including all of the alkali atoms, alkaline-earth, and the noble gases (in
metastable levels) (Metcalf and van der Straten, 1999). Work is also ongoing
to cool and trap molecules (Bethlem et al., 2000). In comparison to the low
polarization of a typical trap (see Sect. II.A.3), it is also possible to create spin-
polarized (P ~ 0.7) atom traps (Walker et al., 1992), which could be used as
targets for a new class of electron collision experiments.
V. Acknowledgments
This work was supported by the National Science Foundation and the U.S. Air
Force Office of Scientific Research.
I
f
3 4 5 6
1 2
FIG. 14. (a) A 1D model atom trap is located at zero magnetic field. The spins of the photons
entering the trap are anti-parallel to the local direction of the magnetic field. (b) We denote the
2S1/2 m=- 89and+l states by the labels l&2, and the 2P3/2 m - ~,- 89 and +3 states by
the labels 3 through 6.
slight excess in scattering from the o - beam approaching from the right. Besides
pushing the atom back towards the center of the trap, this will also tend to
optically pump atoms into the mj -_ - ~ 1 sublevel The local force on the atoms in
the trap due to the trapping lasers depends on the local polarization. The force
is increased by optical pumping which pumps the atoms into states with a high
differential scattering rate between o + and o - light.
We denote the states in the 2S1/2 ground level with m -- - ~i a n d m = + l by the
3
labels 1 and 2, respectively, and the states in the 2p3/2 excited level with m - 2,
l ~,
~., I and ~3 by the labels 3 , 4, 5 , and 6, respectively (see Fig. 14). At a given
location in space the rate of change of the population NI of state 1 is given by
dN2
dN1 _ 2 Rz4N2 - 2RlsN1 - , (16)
dt 3 3 dt
where RI5 and R24 are the absorption rates for the levels 1 and 2 into states
5 and 4, respectively. The absorption of laser light between levels 2 and 6 and
between levels 1 and 3 do not affect the ground level populations since the
2
excited levels all decay back to the same initial state. The factors 5 are the
branching ratios out of the excited states 3 and 4 to return to the opposite
spin ground state. The population of state 2 is given by N2 = 1 - N1. The
population of state 2 in the steady state is given by N2 = R15/(R15 + R24).
The local polarization of the atoms at a particular location in space is given
by P = N2 - N 1 = (R15 - R z 4 ) / ( R 1 5 + R24).
The rate of absorption of light between state i and state j is given by
16~ij 2
(17)
Rij = [09- o90 + (gumu -gtml)ff2] 2 + F2/4 '
where f2 = ~ B is the Larmor precession frequency of the atoms in the magnetic
field, gu = 4 and gt = 2 are the Land6 g-values of the 2p3/2 and 2S1/2 levels,
VII] E L E C T R O N - A T O M C O L L I S I O N CROSS SECTIONS 389
F is the natural linewidth of the atomic transition, o00 is the natural frequency o f
the transition, and o) is the frequency o f the laser light with a Rabi frequency e~.
If we define the detuning of the laser as A = o) - o)0, in the approximation where
A >> ~ , the denominator can be expanded, resulting in
Rij ~ A2 + F2/4
I ]
1 - A2 + F2/4 (gumu - g t m t ) 9 (18)
2A~ )
Rij = R o f u 1 - A2 + F2/4 (gumu - gzml) 9 (19)
From this we can obtain the individual absorption rates of the m sublevels,
Typical values for an atom trap used in our work are a detuning A/2Jr - 12 MHz,
a magnetic field gradient of 9G/cm, and an atom-trap size of approximately
0.5 mm diameter. Thus the magnetic field at the edge of the atom cloud is approx-
imately 0.2 G, which yields a precession frequency o f f2 =/z0B - 6.3 x 105 Hz.
Inserting the F/2sr = 5.9 MHz natural linewidth of the Rb resonance transition
along with these values into Eq. (21) yields a polarization value at the edge o f
the atom cloud of 0.16. We have extended this model to the F = 3 case of interest
here; numerical solution gives P = - 1 . 2 9 b , implying a polarization at the edge
of the cloud of 0.21.
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Wippel, V., Binder, C., Huber, W., Windholz, L., Allegrini, M., Fuso, E, and Arimondo, E. (2001).
Eur. Phys. J. D 17, 285.
Index
391
392 INDEX
G
g-factor, 192 It
electron bound in neutral atom, 192 H- photodetachment in constant electric
electron bound to ion, 193 field, 50
398 INDEX
405
406 C O N T E N T S OF V O L U M E S IN THIS SERIAL
The Auger Effect, E.H.S. Burhop and Role of Energy in Reactive Molecular
W.N. Asaad Scattering: An Information-Theoretic
Approach, R.B. Bernstein and
R.D. Levine
Volume 9
Inner Shell Ionization by incident Nuclei,
Correlation in Excited States of Atoms, Johannes M. Hansteen
A. W. Weiss
Stark Broadening, Hans R. Griem
The Calculation of Electron-Atom Exci-
tation Cross Sections, M.R.H. Rudge Chemiluminescence in Gases, M.E Golde
and B.A. Thrush
Collision-Induced Transitions between
Rotational Levels, Takeshi Oka Volume 12
The Differential Cross Section of Nonadiabatic Transitions between Ionic
Low-Energy Electron-Atom Collisions, and Covalent States, R.K. Janev
D. Andrick
Recent Progress in the Theory of
Molecular Beam Electric Resonance
Atomic Isotope Shift, J. Bauche and
Spectroscopy, Jens C. Zorn and
R.-J. Champeau
Thomas C. English
Topics on Multiphoton Processes in
Atomic and Molecular Processes
Atoms, P Lambropoulos
in the Martian Atmosphere,
Michael B. McElroy Optical Pumping of Molecules, M. Broyer,
G. Goudedard, J.C. Lehmann and
J Vigu~
Volume 10
Highly Ionized Ions, Ivan A. Sellin
Relativistic Effects in the Many-Electron
Time-of-Flight Scattering Spectroscopy,
Atom, Lloyd Armstrong Jr. and Serge
Wilhelm Raith
Feneuille
Ion Chemistry in the D Region,
The First Born Approximation, K.L. Bell
George C. Reid
and A.E. Kingston
Photoelectron Spectroscopy, W.C. Price Volume 13
Dye Lasers in Atomic Spectroscopy, Atomic and Molecular Polarizabilities-
W. Lange, J. Luther and A. Steudel Review of Recent Advances,
Recent Progress in the Classification of Thomas M. Miller and Benjamin
the Spectra of Highly Ionized Atoms, Bederson
B. C Fawcett Study of Collisions by Laser Spectroscopy,
A Review of Jovian Ionospheric Paul R. Berman
Chemistry, Wesley T. Huntress Jr. Collision Experiments with Laser-Excited
Atoms in Crossed Beams, I. V. Hertel
and W. Stoll
Volume 11 Scattering Studies of Rotational and
The Theory of Collisions between Vibrational Excitation of Molecules,
Charged Particles and Highly Excited Manfred Faubel and J. Peter Toennies
Atoms, I.C. Percival and D. Richards Low-Energy Electron Scattering
Electron Impact Excitation of Positive by Complex Atoms: Theory and
Ions, M.J Seaton Calculations, R.K Nesbet
The R-Matrix Theory of Atomic Process, Microwave Transitions of Interstellar
P G. Burke and W.D. Robb Atoms and Molecules, WB. Somerville
408 CONTENTS OF VOLUMES IN THIS SERIAL
Volume 36
Rydberg Ionization: From Field to Photon,
G.M. Lankhuijzen and L.D. Noordam
Complete Experiments in Electron-Atom
Collisions, Nils Overgaard Andersen Studies of Negative Ions in Storage
and Klaus Bartschat Rings, L.H. Andersen, T. Andersen
and P. Hvelplund
Stimulated Rayleigh Resonances and
Recoil-induced Effects, J.-Y Courtois Single-Molecule Spectroscopy and
and G. Grynberg Quantum Optics in Solids, WE. Moerner,
R.M. Dickson and D.J. Norris
Precision Laser Spectroscopy Using
Acousto-Optic Modulators, W.A. van
Volume 39
Wo'ngaarden
Author and Subject Cumulative Index
Highly Parallel Computational Techniques
Volumes 1-38
for Electron-Molecule Collisions, Carl
Winstead and Vincent McKoy Author Index
Quantum Field Theory of Atoms and Subject Index
Photons, Maciej Lewenstein and Li You Appendix: Tables of Contents of Volumes
1-38 and Supplements
Volume 37
Evanescent Light-Wave Atom Mirrors, Volume 40
Resonators, Waveguides, and Traps, Electric Dipole Moments of Leptons,
Jonathan P. Dowling and Julio Eugene D. Commins
Gea-Banacloche
High-Precision Calculations for the
Optical Lattices, P.S. Jessen and Ground and Excited States of the
I.H. Deutsch Lithium Atom, Frederick W. King
Channeling Heavy Ions through
Storage Ring Laser Spectroscopy,
Crystalline Lattices, Herbert E Krause
Thomas U. Kiihl
and Sheldon Datz
Laser Cooling of Solids, Carl E. Mungan
Evaporative Cooling of Trapped Atoms,
and Timothy R. Gosnell
Wolfgang Ketterle and N.J. van Druten
Optical Pattern Formation, L.A. Lugiato,
Nonclassical States of Motion in Ion
M. Brambilla and A. Gatti
Traps, J.L Cirac, A.S. Parkins, R. Blatt
and P. Zoller
Volume 41
The Physics of Highly-Charged Heavy
Ions Revealed by Storage/Cooler Rings, Two-Photon Entanglement and Quantum
P.H. Mokler and Th. St6hlker Reality, Yanhua Shih
Quantum Chaos with Cold Atoms,
Volume 38 Mark G. Raizen
Electronic Wavepackets, Robert R. Jones Study of the Spatial and Temporal
and L.D. Noordam Coherence of High-Order Harmonics,
Pascal Sali~res, Ann L'Huillier, Philippe
Chiral Effects in Electron Scattering
by Molecules, K. Blum and Antoine and Maciej Lewenstein
D. G. Thompson Atom Optics in Quantized Light
Optical and Magneto-Optical Fields, Matthias Freyburger,
Alois M. Herkommer, Daniel S. Kriihmer,
Spectroscopy of Point Defects in
Erwin Mayr and Wolfgang P. Schleich
Condensed Helium, Serguei I. Kanorsky
and Antoine Weis Atom Waveguides, Victor I. Balykin
CONTENTS OF VOLUMES IN THIS SERIAL 415