Formation of cold molecules from atoms

•Magnetoassociation (Feshbach  Resonance) 2002­2003
(R. Grimm, C. Salomon, W. Ketterle, D. Jin, G. Rempe, …)
.
Bmag

•Collision with another partner, 3­body recombination (E.  
Cornell, C. Gabannini, R. Grimm, 1998­2003,…)

•Photoassociation, (Pillet 1997, …)
 Why cold molecules?
– Fondamental tests (e­ dipole, chirality, variation of 
fundamental constants)  
– Photochemistry  (photoassociation) 
– Quantum properties (dipole), molecular collective quantum 
systems BEC,BCS

– Quantum Reactions and control 
– frequency standards and ultracold chemistry
– Quantum information, … [3]

Need ultra-cold molecules in v=J=0

Broadband Vibrational Cooling of Cs2 Molecules
M. Pichler*, D Sofikitis, A. Fioretti, S. Weber♯, R. Horchani, X. Li, M. Allegrini♯♯,
B. Chatel♯, D. Comparat and P. Pillet

Laboratoire Aimé Cotton, CNRS, Université Paris-Sud, 91405 Orsay Cedex, France
*Physics Department, Goucher College, Baltimore MD 21204, USA
♯Université Paul Sabatier Toulouse 3, IRSAMC, Toulouse, France
♯♯also CINSM, Dipartimento di Fisica, Universita di Pisa, Pisa, Italy

(1) 1g PA step
(2) and (3) mixing with v=0
of 1g (4), and two-step
decay to low v” of X1g+

ref: M. Viteau et al. PRA 79, 021402 (2009), Science 321, 232 (2008)
 Motivation for further cooling

–Ultra­cold [1] 
•Laser cooling of atoms :  reduction of velocity through 
accumulation of light momentum.

                                        
•Ultra­fast [2] 
•Femtosecond optical sources and pulse­shaping techniques 
allows control of chemical reactions and of molecular 
internal dynamics
•Control of all degrees of freedom.
•Toward the ro­vibrational cooling of 
ultracold molecules
Photoassociation and cold molecules
Photoassociatio
n
(
1
6s+5 )
1 d 2 atoms absorbs resonantly a
g 6s+6 photon
0u p

Deexcitatio

A.
P.
Spon.

n
Em.

(2 Atoms are
') lost
a
3Σ + 6s+6 (
Xu s 2'' Cold
1Σ + ) molecules
g

ref: M. Viteau, et al. Science 321, 232 (2008)

 Experiment
Cs MOT:
•T~100µK Detection by resonant 2-
•300µm photon ionization
•density~5.1010cm-3
Grid 2 Grid 1
MCP
Ti
:S
a

Ionization laser
La
se

Pu
r

lse
Las
ers

Time
(ns)
er
La s
nd
eco
tos
Fem
 Detection (X 1Σg+,a3Σu+)

(2)3g

(2)3g
–2 photons detection (REMPI)
–Pulsed dye laser, 1 mJ (LDS722 13500-
14500 cm-1 for triplet and LDS751 + 532
nm (B) or DCM (C) state for singlet)
Spectrum when PA is on 0g- (v=79)
Formation and vibrational cooling into a selected v
level of X 1Σg+ state[7]

Experimental setup for vibrational cooling

to a selected vX with a femtosecond laser
using 4-f line with spatial light modulator
(SLM).
Franck-Condon
factors in gray with
the red indicating the
excitation transitions
(a); Fs laser
spectrum (b);

Simulation of
population
accumulation into
vX=0 (c) and REMPI
spectrum without
(black), and with
shaped fs optical
cooling (d)
 Franck-Condon
factors in gray with
the red indicating the
pulsed excitation
transitions (a); Fs
laser spectrum (b);

Simulation of
population
accumulation into
vX=1 (c) and REMPI
spectrum with
shaped fs optical
cooling (d)

D. Sofikitiset al. to appear in NJP

 a) Experimental setup for
vibrational cooling into v=0, with a Even better: diode laser
broad-band diode and using 3
interference filters. vibrational cooling

c) MOT layout

b) Experimental setup for vibrational

pumping with a broad-band diode to
vx=1, using a 4-f line with a grating,
and a mechanical mask.
a)

BBD source spectrum

before (a), and after passing
though the interference filters
line (b).
b)
vX vB
0 0

vX vC
0 0 0 1

REMPI spectrum of the

X1g+ state with (upper
trace with a offset of 10
points) and without (lower
trace) optical pumping.
 a)

BBD source spectrum before

(a), and after passing though
the 4-f line (b).
b)
vX vB
1 01 1

vX vC
1 0 1 1 1 2

REMPI spectrum of
the X1Sg+ state with
(upper trace + offset
of 10 points) and
without (lower trace)
optical pumping.

D. Sofikitis et al. to be submitted

 b)
0.4

0.2

Franck-Condon factors in gray scale. Red hatched squares indicate

transitions excited by optical pumping (blue spectrum). Arrows indicate
a possible evolution of population from the vX=6 level.
Rotations and prospects for cooling

Depletion spectroscopy of vX=0 level. Diode

laser is scanned on vX=1 to vB=4 transition.
Calculated lined for P, Q and R branches are
shown (with JX).

A. Fieoretti et al. submitted to J. Mod. Optics

Close-up of depletion spectroscopy
of vX=0 level. Diode laser is scanned
on vX=0 to vB=3 transition.
Calculated lined for P, Q and R
branches are shown (with JX).

REMPI spectrum of the X1g+

state. Upper trace (with a 50 points
offset) with the depletion laser and
lower trace is without . vB-vX
vibrational transitions are indicated
Vibrational cooling of the a3 u+ molecules

Main motivation:
•high production rates (PA through RG1:
(v=103,Bv =138MHz Re =14.0a0)
•vibrational cooling on the a3u+ - 23g
•better prospects for optical trapping and
evaporation
Triplet Cooling mechanism on a3u+ - 23g
 Conclusions and Outlook
•Production of UCMswith resonant coupling
•Cs2 -real candidate for complete cooling
•KCs – new polar dominated physics

• optical trapping of molecules

• studies of rotations and rotational cooling
• ro-vibrational cooling with a super-continuum source
Funding: 

LAC: IFRAF, Triangle de la physique