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Quantum Dots
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Lucjan Jacak
Pawel Hawrylak
Arkadiusz W6js
Quantum Dots
With 93 Figures
Springer
Professor Lucjan Jacak
Dr. Arkadiusz W6js
Wroclaw University of Technology
Wybrzeze Wyspianskiego 27
PL-50-370 Wroclaw, Poland
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Preface
1. Introduction.............................................. 1
Scientific research into electronic systems was limited for a long period of time
to naturally occurring isolated atoms or particles, metallic or semiconductor
crystals, or beams of beta radiation. Most of these are three-dimensional
systems, while an effective reduction of geometry to two or fewer dimensions
- by a strong spatial localization to a plane, line, or point (i.e., confinement
of an electron in at least one direction at the de Broglie wavelength) - occurs
only in the case of atoms and electrons localized on crystal imperfections
(e.g., on impurities).
The beginning of the 1970s marked the new era of research on electronic
structures of dimension limited to two, so-called quantum wells [29, 35]. The
quantum well is a very thin, fiat layer of semiconductor sandwiched between
two layers of another semiconductor with a higher conduction-band energy
[64]. The difference between the conduction-band energies of the two materi-
als binds the electrons in the thin layer. Since the effective mass of an electron
in a semiconductor is small, the de Broglie wavelength is relatively large. The
motion of electrons bound in a layer as thin as several crystalline mono lay-
ers is two-dimensional, and the excitations in the perpendicular direction are
strongly quantized. The material used most commonly for creating quantum
wells is gallium arsenide, GaAs, which in combination with a ternary solution
aluminum-gallium arsenide, AlxGal-xAs, serving as a barrier allows for the
creation of very thin epitaxial layers as a result of the almost equal lattice
constants.
The new, unusual properties of quasi-two-dimensional systems, which
promise applications mostly in electronics and opto-electronics, have at-
tracted the attention of many research laboratories. This in turn has resulted
in a rapid development of production technology and extensive research. The
discovery of the integer quantum Hall effect (IQHE) by Klaus von Klitz-
ing's research team [86] was awarded the Nobel Prize in 1985. The fractional
quantum Hall effect (FQHE) brought the Buckley Prizes to its discoverers
D. C. Tsui, H. C. Stormer, and A. C. Gossard [129]' and to Robert'Laughlin
for his theoretical work [92, 93, 94]. At present, the properties of the quasi-
two-dimensional systems are well investigated and understood, and quantum
wells have been produced and implemented for years in numerous devices,
2 1. Introduction
2.1 Etching
Fig. 2.3. Etched quantum dots: (a) diameter of 200 nm, GaAs/ AlGaAs well, elec-
tron scanning microscope picture [125]; (b) diameter of 30 nm, InGaAs/lnP well,
transmission electron microscope picture [128]
Fig. 2.4. Quantum dot on the intersection of electrodes; four internal electrodes
localize the electrons, and four external ones serve as contacts for the electrons
tunneling to and from the dot [117]
result, the distance between the electrode (overlying the surface with the
islets) and the plane of the quantum well is modulated, and the electrons are
bound in small areas under the prepared islets: The photograph of a matrix
of such dots, together with the profile of the confining potential, is shown
in Fig. 2.5. Instead of modulating the distance between the electrode and
the well, it is also possible to build a pair of parallel, thin electrodes above
the well. The lower electrode can have regularly placed holes, which is where
quantum dots are to be created [1, 52]. This idea is shown in Fig. 2.6. If
a voltage is applied to the pair of electrodes, the result is a change both
in the dot size (Vgb) and the depth of the confining potential (Vgt). The
potential depth influences the number of confined electrons. However, when
the additional electrode is introduced between the quantum-well layer and
the doped layer, the number of electrons and the potential depth can be
changed independently.
A very advantageous feature of quantum dots whose electrons are confined
by the electric field produced by a set of electrodes is their smooth lateral
confinement, showing no edge effects. The possibility of controlling certain
parameters is also very important. In experimental reports one, can find in-
formation about these types of dots, which can be created on, for example,
gallium arsenide GaAs [3, 4, 51, 52, 97, 105], indium antimonide InSb [122],
and silicon Si [1].
2.2 Modulated Electric Field 9
chlorides can be used instead of glass [66]. The heating of such a matrix with
the addition of copper leads to the formation of CuCl microcrystals.
AI~S:?2
(111)8 GoAl
Fig. 2.7. Quantum dots created on the surface of GaAs in selective MOCVD growth
(scanning electron microscope pictures); width of the electron localization area at
the top of the pyramid is about 100 nm [45]
12 2. Creation and Structure of Quantum Dots
Fig. 2.8. Quantum dots (a), and quantum wires (b) created on the surface of GaAs
in MOVPE selective growth (scanning electron microscope pictures) [95]
Petroff and DenBaars [110] describe another method for the self-crystallization
of quantum dots that does not require the creation of a mask. When the
lattice constants of the substrate and the crystallized material differ consid-
erably (7% in the case of GaAs and InAs, the most commonly used pair of
compounds), only the first deposited monolayers crystallize in the form of
epitaxial, strained layers with the lattice constant equal to that of the sub-
strate. When the critical thickness is exceeded, a significant strain occurring
in the layer leads to the break-down of such an ordered structure and to
the spontaneous creation of randomly distributed islets of regular shape and
similar sizes. The shape and average size of islets depend mainly on factors
such as the strain intensity in the layer as related to the misfit of lattice
constants, the temperature at which the growth occurs, and the growth rate.
The phase transition from the epitaxial structure to the random arrangement
of islets is called the Stranski-Krastanow transition [127]. Figure 2.9 presents
the dependence of the critical number of InGaAs monolayers deposited on
the GaAs substrate, at which the phase transition occurs, on the indium con-
centration in the solution (lower axis), or alternatively the misfit of lattice
constants (upper axis), i.e., the strain.
2.6 Self-Organized Growth 13
On the other hand, Fig. 2.10 presents subsequent phases of the creation of
islets for a pair of compounds with the maximum misfit of lattice constants:
InAs and GaAs, where according to Fig. 2.9 the transition occurs at the
1.8 monolayer deposition. When the process of crystallization is terminated
shortly after reaching the phase transition, the islets evolve to the state of
quasi-equilibrium, in which they assume the shape of pyramids [47,84, 103]
or flat, circular lenses [40,41, 114, 115] formed on a thin layer of InGaAs (the
wetting layer). When the inhomogeneous InGaAs layer is eventually covered
with another GaAs layer, a structure of a quantum well with significantly
increased thickness in very small areas is obtained.
Raymond et al. [114] report the growth of self-assembled dots in the shape
of lenses with ~ 36 nm diameter and ~ 4.4 nm height (with fluctuations of
5-10%). Marzin et al. [103] obtained dots in the shape of regular pyramids
with a square base of side ~ 24 nm and height ~ 2.8 nm (with fluctuations
of ~ 15%), and distance between neighboring dots ~ 55 nm.
14 2. Creation and Structure of Quantum Dots
energy
Fig. 3.1. Density of states as a function of energy in systems with different numbers
of spatial dimensions: 3D, bulk material; 2D, quantum well; ID, quantum wire; OD,
quantum dot
16 3. Single-Particle States of Quantum Dots
and for a zero-dimensional system (quantum dot) has the shape of 8-peaks,
(3.4)
Above, Ci are discrete energy levels, eis the Heaviside step function, and 8
is the Dirac function.
At low enough temperatures (several K) the energy of phonons is too low
to excite the electrons and the strong quantization of energy determines the
striking electronic properties of quantum dots.
H -1- ( p - -A . + -me)2
1 * wor
2 2
2m* c 2
-
2m*
1 *
p2- + -m
2
(2Wo + -w
1 2) r 2-
4 e
1 l
-w
2 e z, (3.8)
where
(3.12)
is the effective length scale, equal to the magnetic length in the absence of
the confining potential
lB = [ffi. (3.13)
(3.16)
The eigenstates of the Hamiltonian (3.8) are constructed by acting with the
creation operators on the ground state (a 100) = b 100) = 0):
(3.18)
(3.23)
where
1
[22 = w5 + -w~.
4
(3.27)
(3.28)
The thick line represents the tenth energy level. For the special values of the
magnetic field, corresponding to the integer ratio w+ : w_, the characteristic
of a zero magnetic field degeneracy of levels is restored. The crossings of
energy levels at these fields lead to the occurrence of rapid changes of slope
20 3. Single-Particle States of Quantum Dots
>.
f2> 12
(]) 11
c:
(])
10
/
40,31,22, ...
./
/
/
/
/ ""
30,21,12,03 ~-_*"~ " "
""
(i)+
r---t-----; 05 j;
20,11,02 ---,..'"---01-----104 :::I
03 g.
02
01 ~
=-
10,01 00 m..
1 "
1 "
1 //
1-__,.;/:"'-7/:"'---
00 /"
/ ,,/
1/ / "
~~-
magnetic field
Fig. 3.2. Evolution of the Fock-Darwin energy levels in a magnetic field; dashed
lines - the Landau energy levels; vertical arrows - allowed optical transitions
(small peaks) in the energy of higher single-particle levels (as was shown in
the example of the tenth energy level: at the point w+ : w_ = 2 the transition
between orbitals 11 and 03 occurs).
transition (n+ n_) +-+ (n~ n'J is proportional to the squared perturbation
Hamiltonian,
A(n~n~,n+n_) ex (n~n~IHe-mln+n-) ex (n~n~1 r In+n-), (3.30)
while the respective oscillator strength [91] is
"
f (n+n_,n+n_ ) = TW n+n_,n+n_ ) 1A ("
2m * .(" ) 12
n+n_,n+n_, (3.31 )
Beside the conduction-band electrons, the valence-band holes are the second
type of carriers that can be bound in a quantum dot. The binding of holes,
initially confined to a two-dimensional quantum well, in the quantum dot is
possible by, for example, applying a spatially modulated electric field. The
dots that bind electrons in this way have been described in Sect. 2.2. Due to
the opposite electric charges of the two types of carriers, the lateral potential
defining dots of this kind cannot attract both electrons and holes at the same
time (either bind electrons and repel holes, or vice versa).
In the case of a quantum well it is possible to achieve the effect of bind-
ing both electrons and holes as a result of the appearance of steps in the
conduction and valence-band energies at the interface between the well and
surrounding barriers. As shown in Fig. 3.3, the energies of conduction and
valence bands can be arranged in two ways on the interface [64]. In a con-
travariant heterostructure (e.g., on the GaAs/ AIGaAs interface) both elec-
trons and holes are confined in the same material (here GaAs). However, in a
covariant heterostructure (e.g., on the InAs/GaSb interface) electrons accu-
mulate in one layer (here InAs), while holes flow into the other (here GaSb);
i.e., the barrier for electrons is the well for holes and vice versa.
An interesting problem is whether a quantum dot can bind both types of
carriers at the same time. In the case of a quantum well it was possible to
obtain the configuration of band energies on the well-barrier interface shown
in Fig. 3.3a, i.e., a contravariant heterostructure. In such a structure both
types of carriers are bound simultaneously. It should, however, be remem-
bered that the quantum well is a crystalline structure theoretically infinite in
22 3. Single-Particle States of Quantum Dots
~ (a) ~ (b)
Q)
c vacuum level ~ vacuum level
Q)
~ -~~r~:-------------------'
Ea
two directions, which justifies its description in the band model. The quan-
tum dot, on the contrary, is a very small object, and using a band model to
describe its electronic properties seems to be a rather rough approximation.
When a pair of semiconductors is chosen as in Fig. 3.3a and the quantum
dot is created in the form of a small microcrystal of the material of the well
immersed in the material of the barrier (e.g., the self-assembled dots), then
the band description of such a structure should be approached with great
caution, as it is only an approximation. In this case it seems more appro-
priate to describe the quantum dot as a perturbation of the crystal field of
a surrounding semiconductor, and to search for the electron-hole structure
of the dot in the effective-mass approximation [16]. The applicability of the
effective-mass approximation requires the condition of a small variation of
the perturbing potential on the interatomic distance. This seems to be true
particularly for the dots created by interdiffusion (see Sect. 2.3), but is rather
questionable for the self-assembled dots (see Sect. 2.6). Conversly, the idea of
a simultaneous binding of electrons and holes in the self-assembled dots has
been supported by recent pseudopotential calculations [44]. However, if the
effective-mass approximation is accepted, then the bare potential (electric by
nature) that attracts a hole has to repel an electron, and vice versa.
The charge-neutral electron-hole pair can, however, be bound in such a
potential as a result of the mutual Coulomb attraction between the particles.
It should be stressed that the two approaches, using (i) the approximation
of the band structure of the material forming the quantum dot and (ii) the
3.5 Valence-Band Holes 23
can be neglected, and the only difference between such a simplified descrip-
tion of holes and that of electrons consists in the occurrence of a number of
subbands (a number of distinguishable types of particles, characterized by
various masses).
A more accurate description of holes requires taking into account the
interaction between the sub bands (intersubband mixing). The model Lut-
tinger Hamiltonian HL [98] describes the interaction between the heavy-
hole and light-hole sub bands (u and m oriented in the same direction:
Iii = lu + ml = ~). In the basis of jz = {+~, -~, +~, -D,
the Hamiltonian
HL is expressed as follows (in the so-called circularly symmetric approxima-
tion):
(3.34)
The operators that appear in the above expression are defined as follows (we
use here the atomic units where the effective Bohr radius aB and the effective
Rydberg Ry are equal to unity):
(3.35)
"2 1""
where k± = -i(ox ± iOy ), kz = -ioz, and k = 'i(k+k- + Lk+).
A A "A
The effective masses for heavy holes (h) and light holes (1) along the
axis of symmetry (z) and in the perpendicular plane (r) are defined by the
Luttinger parameters of a given material (e.g., for GaAs 1'1 = 6.8,1'2 = 1.9,
and 1'3 = 2.9):
-1
m hz = 1'1 - 21'2, -1
mhr = 1'1 + 1'2,
m -1
1z = 1'1 + 21'2, mlr-1 = 1'1 -1'2· (3 .36)
Figure 3.4 presents the dispersion curves for the 8.5 nm thick GaAs quan-
tum well, and the discrete energy levels of the quantum dot created in the
form of a disk 40 nm in diameter etched out of such a well. The results were
obtained by diagonalization of the Luttinger Hamiltonian (3.34), i.e., in the
band-structure approximation, taking band parameters appropriate for the
bulk material of the quantum dot (GaAs).
In the case of a quantum well, the continuous energy spectrum splits into
discrete subspaces (quantum-well subbands), which correspond to different
discrete states of motion in the direction perpendicular to the plane of the
well (uncoupled from the in-plane motion). In Fig. 3.4 we have plotted energy
E as a function of the in-plane wave vector k for a couple of the lowest
3.5 Valence-Band Holes 25
..
20~------~--~--~~~~------~
18
16
14
~ 12
>-
0)
~ 10
s:::
G> Fig. 3.4. Energy as a
8 function of wave vec-
tor for a valence-band
hole confined in a quan-
6
tum well (lines) and
lines - OW in a quantum dot (cir-
4 cles); thin lines - the
dots - 00 effective-mass approxi-
2,.~~~~~~~~~~~~~~~ mation; thick lines -
o 2 3 4 5 6 7 8 9 10 results including inter-
wave vector (a-~) subband mixing
t if j < i + 1,
Uij ={ -1 if j = i + 1, (4.5)
o ifj>i+1.
+ L Vint (T i - Tj ), (4.10)
i<j
where aD, ... ,005 are constants, and Vint is the interaction potential.
Using (4.5) and (4.7), subsequent components of the Hamiltonian (4.10)
can be expressed in terms of the Jacobi variables (unless indicated, the sum-
mations over i, j, k, and l run from 1 to N):
1. The term linear in coordinates:
LTi = 'L:Wij(!j == N(!N (4.11)
ij
4.1 Generalized Kohn Theorem 29
H {
1 2 + Ct5RxP }
Cto+CtlNR+Ct2P+Ct3NR2 +Ct4NP
+ {~
8 [Ct3i+1ei
i i+1
+ Ct4-i-'Tri 2
+ Ct5ei x 'Tri 2 ] }
+ Hint ,(4.18)
where Hint is the total interaction Hamiltonian, dependent only on the rela-
tive coordinates {el,"" eN-l}. As indicated in (4.18) by the large braces,
the Hamiltonian H can be split into a sum of two Hamiltonians: ,Hem' ex-
pressed in terms of the center-of-mass variables, and H re [, expressed in terms
of the relative variables:
(4.19)
Due to the separation of variables, these two Hamiltonians commutate:
30 4. Properties of an Interacting System
(4.20)
Thus, if the system of electrons is described by the Hamiltonian as in (4.10),
i.e., if the single-particle Hamiltonian contains only the terms linear and
quadratic in coordinates and momenta and linear in angular momenta (the
elements of types const, r, r2, p, p2, and r x p) and if the interaction potential
depends only on the differences of individual coordinates, then the motion of
the center of mass of the system decouples from the relative motion.
Hem
p2
= 2M + 2M
1 (2 + 41 w2) R 2-
Wo e
1
2 WeLz , (4.21 )
Thus the eigenstates of the total Hamiltonian are equal to the eigen-
states of the interaction potential alone, and the inclusion or variation of the
noninteracting terms of the Hamiltonian (i.e., the magnetic field or confine-
ment) leads only to (i) rescaling of the characteristic length lo, which scales
the wave functions and the Coulomb energy, and (ii) adding the appropriate
single-particle energy, which depends on the total angular momentum and,
through the kinetic-energy scale w_ (see (3.16)), on the magnetic field and
confinement.
More importantly, since in the units where the characteristic length lo
and the characteristic interaction energy e21lo are equal to unity, the wave
functions and their Coulomb energies do not depend on the noninteracting
Hamiltonian. Furthermore, since the single-particle energy is constant within
each eigensubspace labeled by the total angular momentum, the variation of
the noninteracting Hamiltonian does not rearrange the energy levels within
each subspace. It only rigidly shifts the entire energy spectra corresponding
to these eigensubspaces with respect to one another. The relative shift of the
energy spectra corresponding to the different angular momenta comes from
the fact that the variation of the magnetic field or confinement changes the
characteristic single-particle energy w_ on the scale of the Coulomb energy
e2 l l o.
The ground state within each angular-momentum subspace does not de-
pend on the magnetic field or confinement. It is simply the ground state of
the interaction Hamiltonian in this subspace (calculated, e.g., by Girvin and
Jach [46]). However, the absolute ground state of the system changes when-
ever it is pushed up above the lowest-energy state from another subspace.
ne=3 8=10T
no Landau level
mixing ,."
,.-'
, ....
-w
Cl)
"
E \... ,.".(
1,\ ,.-" single
10 "',
I ,'," electron
.,.,."
,../
/a"·
•
··i· . ·, ......
I
interaction
,
. . .......
Fig. 4.1. Contributions to the
ground-state energy of three elec-
trons as a function of the total angu-
lar momentum J; the confining po-
10 20 tential is parabolic (nwo = 4 meV)
J [101]
4.4 Magic States of a Few-Electron System 35
As shown in Fig. 4.1 for three electrons, the Coulomb energy decreases and
the single-particle energy increases (linearly) with the angular momentum
L tot . Adding the two energies together, One ohtains the total energy as a
function of angular momentum - a dependence with a minimum at a certain
value of L tot . One can choose the energy units of e2 /lo, such that the depen-
dence of the Coulomb energy On L tot is independent of the magnetic field
and confinement. The single-particle energy is linear in L tot , and the slope
is governed by the magnetic field and confinement. Therefore, these two pa-
rameters (magnetic field and confinement) control the minimum-energy value
of L tot . Alternatively, by varying the magnetic field and/or confinement, the
ground state can be driven through a sequence of subspaces, or values of
angular momentum.
5.8"'--'---"1;:::====::::;--:;;:::===::;;::::;'
-
>
II)
.§. 5.6
w
25 25 - _
- --~-
__-
w \ 12
\
>- \
EJ
II) \ I
c
II)
(a)
5.4~---.---.---.---.----.---.---.---,
2 4 6 8 10 12 14 16 18
magnetic field B (T)
~ 15,--------------------------------,
E (b)
.a 12
cII)
9
I
E
I
..
o 6
E
3
.!!!
:::s
OJ
1=-::-£', - - - , I -
04=~~--_r--~--_,--_,~--r_--~--~
- - - - - - - - - - - •
c 2 4 6 8 10 12 18
CIS 14 16
magnetic field B (T)
Fig. 4.2. (a) Magnetic-field evolution of the ground-state energy of three spin-
polarized (continuous line) and spin-unpolarized electrons (dotted line); without the
Zeeman energy. (b) Total angular momentum (continuous line) and spin projection
(dotted line) of three electrons as a function of the magnetic field; with the Zeeman
energy [54J
[93]. A finite energy is required in order to change the state of the system.
For example, a variation of the confining potential at a fixed magnetic field
does not change the area occupied by the electrons unless the ground-state
transition occurs. As noticed by Laughlin [93, 94], the series of magic fill-
ing factors 1I* can be attributed to the series of incompressible magic states.
The sequence of magic ground states, or the magic values of angular mo-
mentum or the filling factor, depends on the number of electrons N but not
on any material parameters or external parameters like the magnetic field
or confinement. The occurrence of the magic series is rather a manifestation
of very special properties of an interacting electron (fermion) system in two
dimensions, which appear also in the fractional quantum Hall effect (FQHE).
38 4. Properties of an Interacting System
electrons were there identified with the so-called compact states of weakly
interacting composite fermions (see the monograph by Jacak et al. [69]).
In the circular representation the presence of.a parabolic confining poten-
tial leads only to the rescaling of a magnetic field,
(4.24)
(i.e., to the rescaling of the length unit, according to (3.12)), but does not
change the form of single-electron wave functions. Hence, a spatially con-
strained system in the magnetic field B is equivalent to a free two-dimensional
system in the effective magnetic field B.
The transformation of an electron system (ES) into a composite-fermion
system (CFS) is performed by attaching to each electron an equal and even
number of elementary fluxes of a magnetic field. This can be achieved formally
by multiplying the ES wave function by the so-called Jastrow factor
V(TI - T2) = -E
e2 J J
dZ I dZ 2 1
ZI -
B*(ZI)e(Z2)
12 1
Z2 + TI - T2
12 < 00. (4.27)
Moreover, Johnson and Payne wrote that the potential of the actual interac-
tion differs from the bare Coulomb potential (ex: ITi -Tjl-I) due to screening.
The parameters Vo and .n should be chosen depending on the dimensions of
the quantum dot. A discussion of this model is also presented in [74]. In such
an approximation the Hamiltonian of the relative motion of N electrons con-
fined in a parabolic dot can be diagonalized analytically, and the obtained
ground state is a generalization of Laughlin's function. The excitation spec-
trum of the system was determined in [76] as a function of the value of the
parameter .n.
A substantial difference, which was introduced by replacing the Coulomb
l/r-type interaction by the harmonic interaction, is evident in the appear-
ance of additional degeneracies: degenerate now are the subspaces of states
with given values of the total angular momentum L tot and the center-of-mass
angular momentum Lcm. Denoting the total angular momentum of the rela-
tive motion of electrons by Lrel = L tot - L cm , in a strong magnetic field (in
the lowest Landau level) the operator of the total harmonic interaction that
acts on the N-electron state can be written as V = 2NVo - ~m*.n2 D2, where
where Cl, C2, and C3 are constants. The Hamiltonian is therefore diagonal in
the basis of any eigenfunctions of L tot and Lrel:
(4.30)
Thus in the case of three electrons, for example, instead of Laughlin's magic
state with angular momentum L tot = 9 (v = !)[93], in the harmonic-
interaction approximation a pair of degenerate states is obtained spanning a
two-dimensional space: L tot = Lrel = 9.
(4.32)
where Eo = .j2;=Ry* aB/lo is the energy scale, (Ry* = e2 /2Ea Bis the effective
Rydberg, a B = di 2 /m*e 2 is the effective Bohr radius, the length scale to is
defined by (3.12), and P = ml + m2 - PI - P2 (compare (8.24)).
Due to the circular symmetry of the quantum dot, the total angular mo-
mentum L = Li mi of the system is a good quantum number, which labels
the eigenstates. In a compact droplet composed of N + 1 electrons, N + 1
single-particle states with the lowest available angular momenta are occupied
where Ivac) stands for vacuum, and the total angular momentum of this
compact state is Lo = ~N(N + 1). Since (in the lowest Landau level, with
the total polarization of spins) it is not possible to construct another state of
N + 1 electrons with this angular momentum L o, the compact state (4.33) is
an exact eigenstate of the interacting system. Further in this section we shall
assume that the magnetic field, confinement, and the number of electrons
assume such values that the ground state of the system is the compact state.
Following the bosonization procedure described in [27, 28, 60, 61, 126]
we can construct the excited many-electron states with angular momen-
tum L = Lo + M by moving the electrons from the inside of the com-
pact droplet (m :::; N) to the outside (m > N) or, alternatively, creating
4.7 Reconstruction of the Edge of a Compact Droplet 43
In the above equation the electrons are excited to states li > N outside the
droplet and leave the holes in states k i ::; N inside the droplet. The values of
coefficients A and B, i.e., the full excitation spectrum of the system of N + 1
electrons, are obtained through the numerical diagonalization of the Hamil-
tonian performed in the basis of IP and 2P excitations. The diagonalization
in the basis consisting of IP and 2P excitations is accurate for M < 9, since
at M = 9 the first three electron-hole pair (3P) excitation occurs. For M 2: 9
this procedure is an approximation, since the diagonalization is performed in
a truncated basis.
The approximation that consists in a numerical diagonalization of the
Hamiltonian in a truncated (finite) basis (e.g., the so-called configuration
interaction method) is equivalent to the variational method - with the trial
function in the form of a linear combination of basis functions. However, the
diagonalization enables an easy improvement of accuracy by increasing the
basis size. This can be done by adding consecutive functions and testing the
accuracy through studying the convergence of results with the growth of the
basis size.
Besides this, and in contradiction to the variational method, as a result
of the diagonalization of the Hamiltonian, the complete energy spectrum, to-
gether with the complete orthogonal set of eigenfunctions, is obtained. With
the appropriate selection of the basis, a number of functions obtained in
this procedure can be good approximations of the exact eigenfunctions. For
instance, when the basis is constructed by choosing the lowest-energy eigen-
states (states below the cut-off energy) of a simplified Hamiltonian (e.g.,
the noninteracting Hamiltonian), the accuracy of the full-Hamiltonian eigen-
functions calculated in the diagonalization procedure can be controlled by
sweeping the critical cut-off energy. The best approximation in such a case is
obtained for the ground state and the low-energy excited states.
Matrix elements of the Coulomb interaction in the basis of IP and 2P exci-
tations are expressed through the two-body matrix elements in the following
way:
- IP-IP matrix element, which describes a single magneto-roton:
(k~ l~ IVeelhk 1) 81~ 11 8k~ kl {E~F - E~F}
+{(l~klIVeelhkD - (l~klIVeelk~h)}, ( 4.35)
where the Hartree-Fock energy is defined as
44 4. Properties of an Interacting System
0.4 (a)
N=15
0.3 - ~ -
o
W
UJ 0 .2
0.1
0.0 B = 2.0 T
0.4 (b)
0 .3
o
W
....... 0.2 Fig. 4.3. Evolution
W
--
0.1
of the excitation spec-
trum of a parabolic
0.0 B = 2.5 T quantum dot contain-
ing 15 electrons in
(c) a magnetic field: (a)
0 .2 B = 2.0 T, the ground
state is a compact
o 0.1 droplet with M = 0;
W
....... (b) B = 2.5 T, a mini-
W 0.0
mum develops at M =
-0.1 7 (magneto-roton); (c)
B = 3.0 T B = 3.0 T, the ground
-0.2 ..J.,-.,...,....,...,....,...,....,...,....,...,....,...,....,...,....,....,...,....,....,...,....,...,....,...,....,....,............... state has M = 24
o 5 10 15 20 25 30 (two bound magneto-
M rotons) [61]
outside and a hole inside the droplet. With an increase of the magnetic field
(Fig. 4.3b) we observe the appearance of a characteristic minimum in the
dependence of the excitation energy on the angular momentum (M = 7 for
B = 2.5 T). Figure 4.4a presents the occupation coefficients of the single-
particle orbitals ((c;;:"Cm) ~ radial charge density), which correspond to the
first excited state. Such excitation, which is located near the system edge,
is referred to as the edge magneto-rotan. A further increase of the magnetic
field results in a decrease of magneto-roton energy (due to the increasing
energy of repulsion between the electrons, compared to the difference between
kinetic energies of neighboring single-particle orbitals). For a certain field
value (B ~ 3 T) this energy becomes negative, and a change of the dot ground
state occurs (binding of a magneto-roton inside a droplet). This transition,
occurring in larger dots, is equivalent to a transition between subsequent
magic states in the few-electron dot. Further transitions in the ground state of
the quantum dot, induced by increasing the magnetic field, correspond to the
binding of subsequent magneto-rotons, i.e., the decrease of the filling factor v.
Figure 4.3c presents a situation where the droplet binds two magneto-rotons
46 4. Properties of an Interacting System
B = 2.5 T
M=7
(a)
(b)
Fig. 4.4. Occupation coeffi-
cients of the single-particle or-
bitals with angular momentum
m, for the magneto-roton min-
ima from Fig. 4.3, (a) M = 7
and (b) M = 24; empty bars -
o 6 10 16 20 the compact droplet with M =
m 0[61]
As shown in Sect. 4.1, the measurement of the FIR light absorption does not
allow for the investigation of interactions between electrons. The quantities
that can be measured (at least in principle) and in which the occurrence of
magic values of angular momentum is reflected, are, for instance, the ther-
modynamic quantities such as the heat capacity and (see the next section)
magnetization. The electronic heat capacity at a constant volume C v , which
is defined as the derivative of the average energy with respect to temper-
ature d (H) /dT, was calculated by Maksym and Chakraborty [101]. Their
results for the system of three and four electrons are shown in Fig. 4.5. In
the calculations only the lowest Landau level was taken into account, and the
Zeeman energy splitting was neglected. However, as the authors claim, this
had no qualitative influence on the results obtained. The confining potential
was assumed to be a parabolic well with characteristic energy 1lv.;o = 4 meV.
The dotted line in Fig. 4.5 represents the result for the noninteracting sys-
tem. The oscillating curve drawn with a solid line shows the results with the
inclusion of interactions. The difference between the two is considerable. The
4.9 Magnetization 47
0.3r------------,O.2r-----------,
n=4 T=3K J=22 ~ n=3 T=3K
i' 0.2
:> ,r---
GI 0.1
E
-;0.1
o
0.2:=::=~======:::, 0.2~=======~
n=4 T=1K J=22 •
n=3 T=1K
ro----.l
J=12
r---- ..
.r-------""
0.1 J=9 •
Fig. 4.5. Heat capacity of three and four electrons in a parabolic quantum dot
[101]
dashed step-like curve shows the values of angular momentum in the ground
state of the interacting system.
At a lower temperature Cv is close to zero, far from the critical magnetic-
field values B* for which a transition to the state with another magic angular
momentum L;ot takes place. It then increases in the vicinity of B* and falls
back to zero at the field equal exactly to B*. The reason for this behavior
is that at a very low temperature the contribution to the thermodynamic
average comes mainly from the two eigenstates with neighboring values L;ot.
At the magnetic field far from B*, a wide energy gap forbids thermal ex-
citation, and the system remains practically in the ground state. On the
other hand, when the field equals any of the values B*, the energies of both
strongly contributing states cross each other, and their thermal mixing does
not change the average energy. The only situation where considerable values
of heat capacity are observed occurs when the difference between the two
lowest energies is on the order of kBT.
At a higher temperature, where the thermal broadening is wide enough
for the thermal mixing of states with higher energies (at any value of B),
the shape of the heat-capacity curve changes slightly. However, the minima
remain at the transition values B*, for which the separation between the
ground-state energy and the next differing energy is the greatest.
4.9 Magnetization
In [102]' Maksym and Chakraborty present the dependence of the magnetiza-
tion M on the magnetic field B. It was calculated for quantum dots containing
three and four electrons. The magnetization can be calculated in two ways:
It is possible to determine the matrix elements of the magnetization operator
48 4. Properties of an Interacting System
2 r------------------------,
j::'O
0
3;
-
CI)
-1
E
-2
~ -2
-3 -4
10 10
..,
B
12
8
B
4
4
2
0 0
2
en I
I
0 0
0 II 10 16 0 5 10
B (T) B (T)
The frequencies w± have been defined in Sect. 3.3, and Vint is the interaction
energy in the ground state. In the case of GaAs, for which the calculations
were done, the spin contribution is very small (LlE = 0.03 meV /T, which
gives a 1 % contribution to M) and can be neglected. The first two components
describe a noninteracting system and after differentiation give a continuous
magnetization curve, marked in Fig. 4.6 with a dot-dashed line. The third
component, which describes the interactions, gives only a small correction to
M. However, due to the sharp changes of L tot (and hence also of Vind, this
correction is discontinuous and clearly visible at low temperatures.
Very similar dependencies to those presented in Fig. 4.6 for N = 3 and 4
were also demonstrated for N = 2 by Wagner et al. [131]. The magnetization
of a many-electron quantum dot and its connection with the spin-orbit inter-
action was also studied by Jacak et al. [70] (see Chap. 9). In the framework
of the Hartree-Fock approximation the analytical expression for total energy
as a function of a magnetic field was found. The respective dependencies are
shown in Figs. 9.2-4. For a magnetic field B at which the magnetization van-
ishes, Be/BB = 0, the transition between the paramagnetic and diamagnetic
states occurs. For a GaAs dot (tu.vo = 5.4 meV) a critical field is ;:::: 2 T, which
is in good agreement with the experimental results of Ashoori et al. [4].
5. Intraband Optical Transitions
0.99
::>
t:: 0.98 Fig. 5.1. Transmission of the
>C!J FIR light of wavelength 118 J-tm
i=" (Le., energy 10.5 meV) for dif-
0.97 ferent gate potentials VG. On
-0.720············
average, three electrons per dot
0.96 -0.715 •...........•. are bound at VG = -0.715 and
-0.720 V, and two electrons per
5.95 6.00 6.05 6.10 dot are bound at VG = -0.730
Magnetic field (8) and -0.735 V [63]
0.2
0.1
(a)
0.0 ! - - - - - ' - - - - ' - -......- -.......- -......- - i
0.3
-
-
~
0.1
p-lnSb (111)
T=4K
(b)
firo=3.2meV
number of electrons in each dot (0-20) was controlled by changing the gate
voltage. Below the threshold (turn-on) voltage VT = -98 V the dots were
empty. The measurements were carried out at helium temperature :::::0 4 K),
and at magnetic fields of 0-4 T. The measured quantity was a relative drop
in the transmission of light through a sample containing the quantum dots
populated with electrons (gate voltage VG > VT), compared to the drop of
transmission through the sample with empty dots (gate voltage VT ):
T(VG) - T(VT )
t= (5.1)
T(VT)
The energy of the laser beam f1w was fixed, while the magnetic field intensity
was increased continuously. The sample graphs published in [122] are shown
in Fig. 5.2. The maxima at the field B = 1 T on the curves for. the fixed
energy of f1w = 10.4 meV correspond to the resonance excitation energy of
10.4 meV in the field of 1 T. The average numbers of electrons per dot for
three different values of the gate voltage VG = 3, 8, and 18 V are N = 3, 9,
and 20, respectively. The identical positions of maxima for different values
of VG indicate that the actual confining potential is parabolic. The absence
54 5. Intraband Optical Transitions
30>15D13
16 n
.. .
20
10
Q)
~
S 5
•
..r::.
~ 20 00 5 15
.§.. J)"V (V) Fig. 5.3. Dependence of the FIR
p-lnSb(111) resonance energies of a quantum
8 T=4K
..s::: dot on the magnetic field; points
!Ng=8V
-EMA
- the experiment; lines - the
Fock-Darwin energies w+ and
w_. Inset: dependence of the FIR
resonance energy on the number
00~--~10~-===::::::::~3~0::==~40'
B (T)
of electrons (without a magnetic
field) [122]
of maxima on the curves for the energy /U.;J = 7.6 meV comes from the fact
that the magnetic field B for which 7.6 meV is the excitation energy is close
to zero (as can be seen in Fig. 5.3). On the curves drawn for /U.;J = 3.2 meV
the maxima appear again, at B = 1.5 T, as a mode with lower energy.
Demel et al. [34] present the results of measurements carried out on the
array of larger dots, each containing 25-210 electrons. The sample investi-
gated was etched from a modulation-doped GaAs/ AlGaAs heterostructure;
the quantum dots were created inside the columns in the shape of 600 nm
wide squares with rounded corners. Due to the deflection of the band edge
at the boundaries, the actual diameter of the area in which electrons were
confined was considerably smaller than that of the column, and depending
on the number of electrons varied between 100 and 160 nm. The Fermi level
in the obtained structure was below the first discrete energy level in the dots.
By controlling the intensity of illumination falling on the sample, the average
number of electrons per dot N (excited to the conduction band by the falling
photons) was varied between 0 and 210. The value of N was determined from
the intensity of absorption. The area from which the signal was collected was
3 x 2 mm 2 and contained about 107 dots. The measurements were carried out
using the Fourier spectrometer, at a magnetic field fixed in the range 0-15 T,
and a temperature of 2.2 K. The measured quantity was the transmission of
light through the sample. The reported absorption spectra for N = 210 are
shown in Fig. 5.4, and Fig. 5.5 gives the corresponding dependence of the
excitation energy on the magnetic field.
An interesting result, visible in Fig. 5.5, is the splitting of the resonance
spectrum and the anticrossing of respective energy curves. According to the
authors of the original work [34], the plasma excitations in the system may be
the reason for this effect. Chakraborty et al. [25] suggested that similar behav-
ior may result from the Coulomb interaction between neighboring dots, which
breaks the rotational symmetry of a single dot (the numerical calculations
presented were made for a pair of coupled dots, each containing three or four
5.2 Measurements of Far Infrared Absorption 55
100~ ~r /
100 ~Ylil- l2+
12.4T
ir-r
100 'I'1f1.5T 5.4T B=
...... 8.4T 11.4T
~
e....100
;if> ~T
~
W
100
m
i="
\1
T
100
k~
Fig. 5.4. FIR absorption spectra of
99
the array of quantum dots, for different
magnetic fields. ES in the schematic of
o 50 100 150 200 the sample shows the electron localiza-
Wave number (cm- 1) tion areas [34J
200 (a)
150
---'~
....
---
8
100
50
N=210
R=160nm
200 (b)
150
......-
---
'8
~100
N=25
8 R=100nm
50
Fig. 5.5. Evolution of
the FIR resonance ener-
°0 2 4 8 8 10 12 14 16
gies in a magnetic field:
(a) 210 electrons, (b)
Magnetic Field B (T) 25 electrons [34J
56 5. Intraband Optical Transitions
electrons). However, in the cited experiment of Demel et al. the large distance
between the neighboring dots (R:: 1J.Lm) seems to exclude this explanation. A
different interpretation of the observed form of FIR spectrum was given by
Gudmundson et al. [49], in which the higher-energy modes were interpreted as
the following transitions between the Fock-Darwin levels: (n, m) - 7 (n, m+2)
and (n, m) - 7 (n + 1, m + 1) (see Fig. 3.2). For a perfectly parabolic confining
potential V(x, y) these transitions are forbidden (see Sect. 3.4). However, as
shown in [49]' the observation of these forbidden transitions may be a result
of deviations from the ideal parabolic confinement (the anharmonic terms).
A similar interpretation was also given by Shikin et al. [120].
It seems, however, that both the splitting of modes and their anticrossing
are the manifestation of the spin-orbit interaction (see Chap. 9). As men-
tioned previously, such an interpretation is also supported by the fact that
for the same value of the spin-orbit coupling constant, the proposed model
provides a very good description of the dependence of energy (and the chemi-
cal potential) ofthe system on the number of electrons and the magnetic field.
These dependencies were measured independently by Ashoori et al. [4] (see
also the description on page 88). As shown by Darnhofer and Rossler [31] on
the example of two electrons confined in an InSb quantum dot, the inclusion
of the spin-orbit interaction within the band model leads to a qualitatively
similar excitation spectrum.
Alsmeier et al. [1] describe measurements carried out on the array of dots
created on the surface of silicon. The confinement of electrons was provided
by a pair of electrodes placed over the silicon surface, as shown in Fig. 2.6.
The lower electrode had regularly spaced, round holes that had a diameter
of 150 nm. The application of the appropriate voltages VCT (top-gate volt-
age) and VCB (bottom-gate voltage) resulted in the creation of a spatially
modulated electric field. The advantage of the system described is the possi-
bility of continuous, independent control of the dot diameters (in the range
40-150 nm) and the number of electrons per dot (in the range 20-350). The
measurements were carried out at a temperature of 2 K and at a constant
magnetic field of intensity 0-12.5 T. Similarly, as in the work described in
previous paragraphs, the directly measured quantity was the relative drop of
the transmission of light through the sample. The curves obtained for 350
and 140 confined electrons are presented in Fig. 5.6. The maxima correspond
to the resonance excitation energies. Also, the evolution of these energies in
a magnetic field is visible. This evolution roughly follows that of the lowest
Fock-Darwin levels shown in Fig. 3.2.
Meurer et al. [105] describe the application of the FIR absorption mea-
surement in the determination of the charging energy of the quantum dot (the
energy required to add a single electron to the dot). The sample investigated
consisted of an array of quantum dots, obtained from a single GaAs/ AIGaAs
quantum well by the application of a voltage Vc to the electrode covering
the square, about 100 nm high cubes of GaAs created on the surface of the
5.2 Measurements of Far Infrared Absorption 57
o
~
~o
!::: o
!<i
I 0
o
o o
o
o
o
o
Fig. 5.6. FIR absorption spectra of an array of quantum dots containing (a) 350
and (b) 140 electrons at various magnetic fields [1]
quantum-well structure. The varying distance between the electrode and the
quantum well led to the creation of a modulated electric potential, laterally
confining electrons in regularly spaced dots. The number of electrons in a
single dot N = 1, 2, 3, 4 was controlled by a change of voltage Vc. The
transmission of light through the sample was measured at a temperature of
1.2 K using a Fourier spectrometer. Figure 5.7 presents a characteristic de-
pendence of the excitation energies on the magnetic field obtained for four
electrons confined in each dot. It should be noted that contrary to the result
of Demel et al. [34], a splitting of the spectrum was not observed here. This
is in accordance with the interpretation of such splitting as a consequence of
spin-orbit coupling [70] (see Chap. 9), the effect of which increases with the
number of particles and is much weaker for several electrons.
On the other hand, the graph in Fig. 5.8 shows the dependence of the
average number of electrons per dot on the applied voltage Vc. The number
of electrons was determined from the integrated relative difference in trans-
mission: N ex: Ji1TIT. Sharp steps in the curve correspond to the binding of
consecutive electrons in the dot, which occurs whenever the potential of the
electrode reaches the ground-state energy of a subsequent number of elec-
trons: N = 1, 2, 3, 4 (i.e., the Fermi level passes through the consecutive
discrete energy levels). According to the authors of the experiment, it is very
surprising that such a great number of dots (~ 108 ) can be simultaneously
58 5. Intraband Optical Transitions
.
125r---------------------------
.....~.
"./"
e"
100 • ...."''''...,..
...
4 e/dot
~
Ul
c
0
4
1:5 I , ! I
Q)
3
Q)
...
<0-
0
! 1 ! q3
1
Q) 2
..c
E
::l
Z Fig. 5.S. Dependence of the av-
erage number of electrons per dot,
-0.76 -0.74 -0.72 -0.70 obtained from the FIR spectra, on
Gate voltage (V) the gate voltage [105]
populated with equal numbers of electrons. The reason for this is the signif-
icant charging energy that is required to add a next electron to the system
(~ 15 meV, which exceeds the energy of thermal excitation kBT). The charg-
ing energy measures the Coulomb repulsion between the added electron and
the electrons that are initially confined in the dot.
6. Interband Optical Transitions
The photoluminescence measurements are the basic tool that allow for the
investigation of discrete energy levels of quantum dots. For this reason this
is usually the first step in the studies of quantum dots obtained by vari-
ous methods (described previously in Chap. 2). The idea of the photolumi-
nescence experiment is presented in Fig. 6.l. A laser beam of appropriate
wavelength excites the electrons from the valence band (VB) to the conduc-
tion band (CB) and creates electron-hole pairs (rin ----+ e + h). These pairs
can be excited directly into the discrete levels in the quantum dot, or above
the discrete levels; to the two-dimensional quantum-well continuum or (even
higher excitation energy) to the bulk semiconductor continuum. A fraction of
the generated particles relax nonradiatively and fall to the ground state or to
weakly excited states in quantum dots. The electron-hole pairs confined in the
dots recombine, emitting photons, which are then registered (e + h ----+ ')'out).
-.0 I
increa sing excitation power.
CDI
;:1
.!!!I
<D
~I m
n.
•
§I
liiil a
::::J
00
(laser)
...
"0
•
[II Ol beam rout as a function of the
"0
--0-0-- wavelength rout at the con-
:::r stant wavelength of the incom-
o
1 m
00
ing beam rin (PL spectrum), or
I on the wavelength rin at the
1 constant wavelength rout (PLE
~O spectrum)
60 6. Interband Optical Transitions
the intensity of emitted radiation {'out on the energies of the incoming photons
E in , is related to the number of electron-hole pairs excited at a given energy
Ein. This is because the number of electron-hole pairs that relax to the state
from which the recombination is registered depends on the total number
of created pairs. On the other hand, the probability of creation of a pair
(absorption of a photon) is proportional to a joint (optical) density of states
of the electron-hole pair. Hence, a peak in the PLE spectrum corresponds to
a peak in the optical density of states, which in the case of a quantum dot
translates to a discrete energy level.
The condition of obtaining clear peaks in the photoluminescence spec-
trum, which are characteristic of systems with a strong spatial confinement
(with a discrete spectrum of energy levels), is the lack of thermal broadening.
Therefore, the temperature at which the measurements are usually taken is
on the order of a few K, so that it satisfies the condition kBT « E: (E: is the
separation of neighboring energy levels). However, in the case of very small
self-assembled dots (SAD) the energy quantization is so strong (E: ~ 45 meV)
that Raymond et al. managed to register the PL signal even at room tem-
perature [114].
Due to the small intensity of radiation that is emitted by a single dot,
the measurements are usually taken from a large system (array) of dots. The
inhomogeneity of the individual dot sizes leads to an additional broadening
of peaks.
(6.2)
62 6. Interband Optical Transitions
where Ii) and If) stand for the initial and final states of the exciton, respec-
tively, q is the wave vector of the emitted phonon; mu q = /iqc s is the phonon
energy, Cs is the velocity of sound (3700 mjs for GaAs) , and nB represents
the Bose-Einstein distribution of phonons in the crystal lattice at tempera-
ture T (at zero temperature we have nB = 0). The electron-phonon coupling
operator W has the form
(6.3)
The relaxation of an exciton, which is confined in a quantum dot, through
the emission of an optical phonon LO is rather inefficient. The phonon energy
ELO is almost constant (weakly dependent on the wave vector), and there-
fore the first-order process (with the emission of a single phonon) requires a
precise fitting of the distance between the two discrete energy levels of the
confined exciton, and the photon energy ELO. The interaction of the exciton
with LO phonons is obviously also possible through higher-order processes
(e.g., through a simultaneous emission ofLO and LA phonons). However the
efficiency of such combined processes is very limited. Moreover, energy ELo
is fairly high (~ 30 meV for GaAs) and excludes the relaxation between a
pair of closer excitonic energy levels.
Considering an acoustic phonon LA, in the simplest case of the electron-
phonon interaction, the parameter a in (6.3) is expressed by the deformation
potential D (8.6 meV for GaAs):
2 D2/iq
a (q) = -2-'
{lC
(6.4)
s
where {l is the density ofthe crystal (5.3 gjcm 3 for GaAs). A similar equation
describes the parameter a which governs the hole-phonon interaction (the
only difference is that due to the anisotropy of the hole effective mass, a
strongly depends on the direction of the phonon wave vector q). Figure 6.2
presents a comparison of the rates of the radiative recombination and of the
relaxation from the first excited state from which the recombination is allowed
by the selection rules (zero total orbital angular momentum of the pair), as a
function of the characteristic frequency Wo of the parabolic confining potential
of the dot ~m*w5r2.
For small phonon wave vectors lengths q the probability of relaxation
increases with q, and hence with the phonon energy, equal to the distance
between the ground and excited states of the exciton (~ muo). The reason
for such behavior is the relation W IX yfq (see also (6.3) and (6.4)).
However, if the phonon wavelength drops below the smallest characteristic
dot dimension (Le., below the thickness of a quantum well, from which the
dot was created), the matrix element I (fleiqrli) I, which appears in (6.3),
decays rapidly (integral of a quickly oscillating function) independently of
the direction of the emitted phonon (direction q). In effect, the relaxation
rate itself rapidly decreases with q. This means that the exciton confined in
6.2 Carrier Relaxation 63
80~-----------------------,
FIRST EXCITED
j=O EXCITON
60
--
20 rate (dashed line) of an exciton in
a quantum dot, from the first op-
RADIATIVE DECAY tically active excited state (with
zero angular momentum), as a
O~--~----~---r~--r---,
o 2 4 6 8 10 function of the characteristic fre-
quency of the confining potential
[11]
Inlerdiffused Region
[J 25nm 10.6s
Dol Size
w=
1000 A Si3N4
100A GaAs Onm
200 A AIGaAs (Inlerdiffused
30A GaAs Region)
200 A
~
(x=0.35) Q tu 0 t
---------=
uan m CB
L ~
0
E
I I
~
C
x.y
Dot Sizew
.
::I
.ri
.!!.
~
enz x50 400nm
w
I-
Z
W
U 450nm
Z
W
u
en
w 500nm
z
:2
::::>
...J
e
l-
1000nm
shown by Jacak et al. [68, 71] (see also Chap. 10), the investigation of the
stability of these states allows for an interpretation of the above-described
experiment of Bockelmann et al. (and also other results of luminescence mea-
surements for dots of different types). According to this interpretation, the
additional peak in the photoluminescence spectrum corresponds to a recom-
bination from a weakly excited metastable state of an exciton. It is shown
that the distance between the pair of peaks and also the height and broaden-
ing of the higher-energy peak, depend strongly on the dot size. The results of
the calculation, presented briefly in Chap. 10, show that the evolution of the
photoluminescence spectrum corresponds very well to the experimental de-
pendence in Fig. 6.3. For a large dot the spectrum is dominated by a strong
peak, which corresponds to the recombination from the ground state. The
decrease of the dot size is initially accompanied by the lowering of the excita-
tion energy of a metastable state, and in turn by a visible strengthening and
6.3 Observation of Magic States of Quantum Dots in the Absorption Spectrum 65
narrowing of the additional peak. At a certain critical dot size this additional
peak becomes comparable with the main peak. Above the critical size the
repeated increase of the main peak is observed, as well as a decrease of the
additional peak. At the same time the displacement of peaks toward higher
energies, which accompanies the decrease of the dot size, is observed, similar
to that observed in the experiment (see Fig. 6.3).
>-
~ Fermi level
- cb
(j)
c
ill
o~~~~~~~~~W+~~~~~
- - -______ vb
o 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15
Fermi level -
-
>- Fig. 6.4. Schematic dia-
....
Ol
holes
gram of the single-particle
(j)
c energy levels of a quan-
ill tum dot in a strong mag-
netic field; vertical arrows
- allowed interband opti-
cal transitions. Upper di-
agram: compact droplet;
o 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 lower diagram: recon-
M structed droplet [60, 61]
66 6. Interband Optical Transitions
band is completely filled, and the occupied electronic states in the conduction
band (states occupied by the confined electrons) are marked with rectangles.
Some of allowed optical transitions of an electron from the valence band to
the conduction band are marked with vertical arrows: the orbital angular
momentum of the excited electron does not change, and the orbital to which
the electron is promoted is empty (the Pauli exclusion principle).
The upper and lower diagrams show two possible situations. When the
electrons form a compact droplet (upper diagram), the excitation of an elec-
tron is possible only above the Fermi level, i.e., outside the area occupied
by the dot in the real space (outside the droplet). The kinetic energy of this
excitation is high, and the attraction between the hole and the electron sys-
tem is small. Hence, the energy of creation of such an exciton is high. When
the electrons are in the state with a lower filling factor (a magic state with
a higher total angular momentum for several electrons, or a many-electron
system with a reconstructed edge), it is possible to excite an electron below
the Fermi level, inside the physical area of the electron droplet. The energy
of the photon required to promote a valence-band electron inside the droplet
is lower than that required for the excitation outside the droplet. Thus, it
should be expected that the transition in the ground state of the quantum
dot, induced by a magnetic field, will result in the occurrence of a new strong
low-energy peak in the absorption spectrum (PLE). This new peak would
emerge below the main peak, which corresponds to the excitation near the
edge of the droplet. Obviously, the actual electronic droplet is an interact-
ing system, while what is shown in Fig. 6.4 disregards electron correlations.
However, as shown in the realistic calculations for the interacting system,
the conclusion, which suggested the appearance of a new peak indicating a
change of the ground state of a dot, remains true. It is assumed here that all
electrons are spin polarized (the calculations show that three electrons form
a polarized system, also a polarized compact droplet, over a wide range of a
magic field [54]), while the spin of the excited fourth electron depends on the
polarization of light.
The exact absorption spectra, determined for a parabolic dot contain-
ing three electrons, are presented in Fig. 6.5. The upper diagram shows the
spectrum in a magnetic field of 2 T, when the ground state corresponds to
v = 1 and angular momentum L = 3. The strong peak with the lowest en-
ergy indicates the creation of an exciton at the droplet edge. For a larger
number of electrons this corresponds to the Fermi edge singularity [53]. The
lower diagram presents a spectrum in a magnetic field B = 4 T, for which
the electrons form a ring with a higher magic angular momentum L = 6. A
new peak corresponding to the creation of an exciton inside the bulk of the
droplet is visible. The evolution of the absorption spectra of three electrons
in an increasing magnetic field is presented in Fig. 6.6. The circles represent
absorption peaks, and their areas are proportional to the individual transition
intensities. Since the circularly polarized light excites only electrons with a
6.3 Observation of Magic States of Quantum Dots in the Absorption Spectrum 67
4 compact dot
B=2Tesla, R=3
c 3
o
e-O
'.0:;
In 2
..0
«
04-------~--~~~~~~~~~
4 reconstructed dot
B=4Tesla, R=6
3 Fig. 6.5. Absorption
c
o spectra of a quantum
e-
'.0:;
dot containing three el-
O ectrons. Upper diagram:
2
In
..0
compact state with L =
« 3 (droplet), lower dia-
gram: reconstructed
state with L = 6 (ring) .
Insets: approximate elec-
tron density dis-
04-~~~~~~~~~~~~--~ tributions Insets: appro-
-2.0 -1.5 -0.5 0.0 ximate electron density
distributions [61]
-too --..-------T"""O.....-::.:-----.-""T"-,.-,'.i"'"-rr.
• • ! ; : :.
-rT."'!,,~"T'
• !
',' -,:r,.-,
•
••• ii,
!
i ~
, O
, , 'f· t
: t.
-1.25 : :: :
e a • • ~ •.•.•• !~,~~~~
ee@.
......
0
-1.50
. : :. .'
WO
:;;::~:
:::::::
::i.
•••••••
I
~ -t75
• •
• • •
-2.00
R=3 R=6
-1.25
WO -1.50
:::::::
r R~:
::i.
I
~ -1.75
-2.00 b) 1
R=3 R=6
23456
magnetic field, Tesla
Fig. 6.6a,b. Magnetic-field evolution of the absorption spectra of three electrons
confined in a quantum dot. Areas of circles correspond to intensities of individual
transitions. The two diagrams correspond to the two circular polarizations of light
(spin projection of four electrons in the final state): (a) 0"+ (Sz = 2) and (b) 0"_
(Sz = 1) [61]
by its opposite spin projection. As a result, the changes of the ground state do
not cause such dramatic changes in the absorption spectrum as was observed
for Sz = 2. The striking difference between the spectra for the two polar-
izations of light at low magnetic fields, when the three initial-state electrons
form a compact droplet, should be experimentally observable.
6.4 Interaction of the Exciton with an Additional Electron 69
10
8=10T X
-
::::I
~ 10
>- X Ct
-
:t::
en
c:
Q)
c: 5
c:
0
;:;
...0
Co
10 -
en X a+
.Q Fig. 6.7. Absorption spectra of an
CIS
empty dot (X is created) and of a
5 dot containing one electron (X- is
created) in a magnetic field of 10 T.
The two spectra for X - correspond to
two circular polarizations of light 0"+
Or-----~~~4-~~-L~~ and 0"_ (two spin-polarized and spin-
-15 -10 -5 o unpolarized electrons in the final state)
energy (meV) [132]
70 6. Interband Optical Transitions
of quantum-well thickness [82, 83]. The difference between the 0'+ and 0'_
spectra allowed for the identification of the low-energy peak as that corre-
sponding to the creation of X- . It should be added that in the magnetic field
of 10 T a weak confining potential (in [132] assumed as Wo = 2.5 meV) has
only a small effect on the obtained X- binding energy. Hence, the spectra
calculated in [132] describe both quantum dots and quantum wells.
The above-mentioned lack of interaction between an exciton and an elec-
tron in a strong magnetic field results from a more general property. This
involves a two-dimensional system of electrons and holes in a strong mag-
netic field, when all particles are spin polarized and the wave functions of
electrons and holes are identical (in spite of different effective masses). Such
a system has the eigenstate P, in which the excitons interact neither among
themselves nor with the fluid of excess carriers (e.g., electrons). Hence, the
excitons form the phase that is, in a sense, analogous to the Bose-Einstein
condensate [24, 96, 99, 108]. The state P is the state with the lowest en-
ergy in a subspace with total orbital angular momentum equal to that of the
ground state of excess electrons. This subspace is reached when the excitons
are created in an electron system that was initially in its ground state.
The vanishing of the interaction energy for two electrons and one hole
means that the electron-electron exchange energy, which attracts the photo-
created exciton to the initial-state electron, compensates exactly for the weak-
ening of the attraction within this created electron-hole pair, which has to be
created outside the orbital initially occupied by the first electron. As a result
the energy of the final-state X- complex is equal to the sum of electron and
exciton ground-state energies.
X5
~
(/)
c:
2c:
Fig. 6.9. Photoluminescence spectra of: (a) quantum dots with diameters (ii) d =
140 nm, (iii) d = no nm, (iv) d = 80 nm; (b) quantum wires with widths (ii)
d = 160 nm, (iii) d = 140 nm, (iv) d = 100 nm. In both diagrams, (i) is the
spectrum of the quantum well from which the dots and wires were made [95]
from other cases. A direct reason for the appearance of a large number of small
peaks, rather than a few strong and clearly separated ones at the energies that
correspond to the discrete energy levels, may be the inhomogeneity of sizes
of individual quantum dots. Figure 6.9 shows the graphs of Lebens et al. [95],
which present the changes in the photoluminescence spectra of quantum dots
and wires, which appear in decreasing sizes. The displacement of the main
maximum toward higher energies is visible. Also, the gradual emergence of
small peaks becomes more and more visible with an increase in the separation
between energy levels (compared to the widths of the peaks).
72 6. Interband Optical Transitions
>-
~
~ 1700
W • PL-Experiment
....:. - Calculation
Il. 1660L-_........:G::::aAs/.'-:::::.iI\I.::./>s~28::.::.8:.o:AJ:::.:50::..:.JA
-1.5 -1.0 -0.5 0.0 0.5 1.0 1.5
o
::I
o "L =632.8 nm tum well, collected from
the areas of diameters: (a)
....I E~- HHo dL = lOOp,m and (b) dL =
Il.
j (a) 2p,m. Sharp peaks in (b)
correspond to the recom-
bination of excitons local-
ized on the fluctuations
of the quantum-well thick-
ness. Insets: configuration
of band edges, and the de-
(b) pendence of the conduc-
tion-band energy in points
1700 1710 1750 1760 r and X on voltage VB
[139]
marked with arrows are clearly visible. These peaks are characteristic of the
recombination of an exciton from discrete energy levels, i.e., the localization
of an exciton in a small area.
Zrenner et al. [140] present a more recent experiment carried out by the
same group. They report a successful observation of photoluminescence peaks
that correspond to the optical transitions from the system of one and two
excitons confined in a single quantum dot in a perpendicular magnetic field.
The sample used in the experiment (coupled quantum well GaAs/AIAs) and
the relaxation of carriers to the quantum dot have been described above
(Fig. 6.10 and the description in the text). In order to obtain a signal from
a single dot, several conditions had to be fulfilled. The signal was collected
from an area limited to about 1 p,m 2 by the application of a high-resolution
detecting system (space-resolved photoluminescence). Such an area contains
about 100-1000 quantum dots, and in order to select only a single dot (the
one in which the exciton energy is the lowest), the voltage drop VB, which
was applied across the well, was varied. The excitons from the state with the
hole at point X (AlAs) can relax only to the dots in GaAs with energies below
the critical value, which depends on VB. By lowering VB to the appropriate
value, it was possible to obtain a situation in which the ground state of only
one dot is occupied in the sampled area. The enlargement of the exciton
lifetime obtained in the coupled-well structure is necessary in this situation
74 6. Interband Optical Transitions
GaAs/AIAs 30Al40A
AL=632.8nm
PL=20J.1W
T=8K
i~------~~~~~
r:::
::J I-----..I..--.=..~~Ir"""'"
£I---------~~~~V~
ro
~I-------~~~~
~ 1-----.-::::"-xtI-IrMd
::J
O~--~~~~~~~~--=---------~
()
~r---~~~~Hft-r--~--------;
~~---"~--~H*--=--------~
to allow the exciton to relax from the AlAs layer to the selected quantum dot
before recombination. Figure 6.11 presents the measured dependence of the
photoluminescence spectrum on voltage VB. Lowering of the X-point energy
in GaAs below the r-point energy takes place at VB = 0.35 meV. Starting
from that value, a shift of the main peak toward lower energies (the Stark
shift) is observed. For the values of VB close to zero, the filling of many
dots with various sizes becomes possible, and the spectrum is composed of
many separate peaks. Below VB = -0.35 a single peak is observed, which
corresponds to the emission of a photon from the single lowest-energy dot
containing one exciton.
Analyzing the spectrum a little below VB = -0.35, the authors observed a
peak emerging for VB > -0.35 at energy about 1720 meV and identified it as
the emission from the system of two excitons. Probably there are in fact two
very close peaks, corresponding to two spin configurations: a singlet (vanish
6.5 Measurements of Photoluminescence 75
both the total spin of the pair of electrons, ISel = IShl = 0, and the total
spin of the pair of holes, Se,z = Sh,z = 0) and a triplet (ISel = IShl = 1 and
Se,z = -Sh,z = 0, ±1), split by the electron-electron and hole-hole exchange
interactions.
Zrenner et al. [140] studied also the magnetic-field evolution of energies
of the photoluminescence peaks for the emission from a system of one or
two excitons in the dot (peaks are marked with arrows in Fig. 6.11). The
measurements were carried out in the magnetic fields 0-12 T. Each of the
three peaks (a single exciton and a pair of excitons in a singlet and triplet
spin configuration) in a nonzero magnetic field splits into two peaks, which
correspond to the opposite spin projections of all particles onto the field
direction. The magnitude of the splitting is the Zeeman energy, equal to
81.7 /LeV IT.
Brunner et al. [21] also describe the measurement of a photoluminescence
signal from a system of two excitons confined in a quantum dot. Similarly,
as in the work described above, the investigated dots were formed in the
fluctuations of the quantum-well thickness. The quantum well consisted of
a 3.4 nm thick GaAs layer placed between the Alo.35Gao.65As barriers. The
measurement was carried out using two values of power of the laser beam,
which created excitons: 0.1 /LW and 5 /LW. The area from which the photolu-
minescence signal was collected had diameter about 1 /Lm. One of the original
graphs is shown in Fig. 6.12. In the photoluminescence spectra measured at
a small laser power, a strong wide peak with energy 1671 meV can be iden-
tified, which corresponds to the recombination of two-dimensional excitons,
which move freely in a quantum well. Also, at energies of 1659-1671 meV, a
number of weaker sharp peaks appear. Similarly as in [139, 140], the sharp
peaks with energies below the free-exciton recombination energy (1671 meV)
were identified as the signals of the recombination of excitons localized in
areas of locally increased thickness of the quantum well (for the localization
of the exciton in the dot; see the discussion in Sect. 3.5.1). On the other
hand, in the graphs corresponding to a higher laser power, additional very
weak peaks appear at energies 1653-1655 meV. These energies lie below the
lowest energies of single localized excitons (1659 meV). When a higher ex-
citation (laser) power is applied, the number of created excitons in a given
area increases. Hence, the probability of capturing a subsequent exciton in
the quantum dot before the recombination of the first one occurs also in-
creases. Thus, new peaks were connected with recombination processes from
the systems of two excitons, which were confined in the quantum dot. (A
comment might be added here that the band-structure model of the quan-
tum dot does not allow one to analyze the metastable states of excitons, the
occurrence of which explains the additional luminescence peaks in a natural
way; see Chap. 10.) The difference between the ground-state energies of a
single exciton and of a pair of excitons was read from the photoluminescence
76 6. Interband Optical Transitions
; [ r----G-aA-sl-A-lo.-3s-G-a-o.o-sA-S-O-W---------t
spectrum as the distance between the appropriate peaks. This value allowed
to determine the dot diameter, on the order of a few tens of nanometers.
Figure 6.13 presents the photoluminescence spectra measured by Fafard
et al. [40] for the AlInAs self-assembled quantum dots (SAD) formed on the
AlGaAs substrate. The upper frame (a) shows the spectrum measured in a
sample containing about 106 dots. A single wide Gaussian peak is observed,
which corresponds to the recombination from a great number of dots of differ-
ent sizes. The broadening of the peak position reflects, to a certain degree, the
inhomogeneous broadening of the dot dimensions in the sample (the broad-
ening is also related to the exciton recombination time). The lower frame (b)
presents the spectra that were registered for smaller and smaller numbers of
dots: about 2500, 1400, and 600, which correspond to the sampled areas of
13, 7, and 3 J-Lm 2 , respectively. It is clearly visible that as the number of dots
in the sample decreases, the large Gaussian peak is gradually replaced by
a group of single small peaks, which correspond to the emission of photons
from particular dots. The width of an elementary peaks is ~ 0.4 meV.
Bayer et al. [7] present the results of photoluminescence measurements
in strong magnetic fields. The change of dot diameters (34-41 nm) and the
change of magnetic field in the range 0-12 T enabled the observation of the
influence of both factors on the structure of luminescence peaks. As can be
6.5 Measurements of Photoluminescence 77
3500r--.,........-r---.---.--------.---.---,---,
-2500 dots
3000 (b) T=2K
W
='=2500
§ 1 I Fig. 6.13. Photolumines-
..c:i 2000 Probing -1 31lm2
I cence spectra of self-as-
~1500
(1.1000
I \ sembled quantum dots with
average diameter :::::: 17 nm:
(a) large number of dots
500 (:::::: 10 6 ), (b) small numbers
of dots (600-2500). Zero on
-40 -20 0 20 40 60 the energy axis represents
Energy from the peak (meV) wavelength>. = 660 nm [40]
noted, in addition to the main peak, which dominates in strong fields and for
small dots (see Fig. 6.14), additional peaks appear at weaker fields and for
greater dot sizes. The number of peaks varies between one and three, which
agrees with our theory presented in Chap. 10, which predicts the radiative
recombination from the metastable excited states. Different values of the
excitation (laser) power were used in the experiment (15-15000 W/cm 2 ),
and at the higher values the creation of many-exciton complexes should be
expected.
The matrices of quantum dots were made of a 5 nm thick InGaAs/GaAs
quantum well. Outside the selected areas, the covering layer of GaAs was
etched away, and the following structure was obtained: a thin layer of InGaAs
(quantum well) created on a GaAs layer (barrier) and covered with GaAs
only in the small selected areas. The potential barrier at the GaAs/lnGaAs
interface is much lower than that at the GaAs/vacuum interface (the electron
affinity for GaAs IJ :::::: 4 meV, while the step in the conduction-band edge at
the GaAs/lno.13Gao.87As interface is LlEcB :::::: 0.1 eV). Thus, the carriers are
confined in the areas covered with the GaAs layer. Three different samples
contained dots with diameters 34, 35, and 41 nm.
The strain present in the narrow InGaAs layer created on GaAs (lattice
constants differing by :::::: 1%) causes the splitting of heavy-hole and light-
hole subbands in the valence band by about 60 meV. Hence, the interaction
between the subbands is negligible, and for the description of holes a single-
band approximation can be used. Due to the small sizes of quantum dots, the
78 6. Interband Optical Transitions
(a) (c)
>-
:!::::
en
C
SC
"C
.~
ca~
E
g 34nm 4T
OT
1.43 1.45 1.43 1.45 1.43 1.45
energy (eV)
Fig. 6.14. Photoluminescence spectra of quantum dots in a magnetic field, mea-
sured for different dot sizes: (a) 34 nm, (b) 35 nm, (c) 41 nm [7]
separation between the single-particle energy levels in the quantum dot (up
to 15 meV) is on the same order of magnitude as the energy of the Coulomb
interaction, and the eigenstates of the interacting system are close to those
of the noninteracting system. From the numerical calculations (in the band-
structure model of a quantum dot; see the discussion in Sect. 3.5.1) it was
obtained that in the quantum well of which the dots were made, there is only
one confined subband for electrons and one subband for holes (neglecting
the spin). In a zero magnetic field the quantum dots have three confined
single-particle states (both for electrons and for holes): the s-type state with
angular momentum L = 0 and a pair of degenerate p-type states with angular
momenta L = ±l. In higher magnetic fields the d-type state becomes bound,
having angular momentum L = 2 for an electron and L = - 2 for a hole.
Figure 6.14 presents the photoluminescence spectra measured for three
different dot sizes at different values of the magnetic field. Higher-energy
peaks are observed (overlapping neighboring peaks can be resolved as a
change of the asymmetry of the envelope), as well as the rearrangement of
the spectrum in the increasing field. Figure 6.15 presents the energies of the
photoluminescence peaks, which are taken from the spectra similar to that
in Fig. 6.14, as a function of a magnetic field. Comparing the experimental
data (points) presented in Fig. 6.15 with the curves determined numerically
(diagonalization of the Hamiltonian of an electron-hole pair for the realistic
three-dimensional confining potential in the band-structure model of a quan-
tum dot), Bayer et al. identified the peaks marked in the figures with squares
as recombination from the states with zero angular momenta of both parti-
cles Le = Lh = 0 (s-type states); with diamonds, from the states Le = -1
and Lh = +1; with triangles, from the states Le = +1 and Lh = -1; and
with circles, from the states Le = -2 and Lh = +2.
6.5 Measurements of Photoluminescence 79
(a)
1.43 ~O-~2-~4-~6-~a'-!O""---5---1-0---LO
--'2:---4--6---la
Obviously, the Coulomb interaction between the electron and the hole that
form an exciton, as well as (neglected in the calculations) the Coulomb inter-
action with other confined electron-hole pairs, makes the above description
even more complicated. The states with defined values of electron and hole
angular momenta are not the eigenstates of the total Hamiltonian, which
conserves only the total angular momentum of the pair. The approximate
agreement of the results of measurements and calculations, and hence the
possibility of a simple interpretation of observed photoluminescence peaks in
terms of transitions between the appropriate single-particle states according
to the appropriate selection rules (zero total spin and angular momentum of
the pair), can be explained as the effect of the small dot dimensions. As men-
tioned above, the quantization of motion in such a small system results, first of
all, from spatial confinement (and a magnetic field, when the magnetic length
is comparable to the dot diameter), whereas the Coulomb interaction does
not substantially change the wave functions. Thus, the spectra in Fig. 6.15
slightly resemble the spectrum of Fock-Darwin single-particle energy levels
in Fig. 3.2 (only the energy of electron excitation fiwo is now replaced by the
sum of energies of electron and hole excitations, and the entire spectrum is
vertically shifted by the energy of electron-hole attraction). The influence of
the Coulomb interaction on the photoluminescence spectrum in such small
dots was discussed in detail in [134], and a summary of those results is given
in Sect. 8.3. The interaction between a number of excitons confined together
in a quantum dot is described in [135, 136] and in Sect. 8.4.
80 6. Interband Optical Transitions
n=3
~8
::i
.!i
Q)
g 6
8III
Q)
c
'E:::I 4
'0
'0
..c
D..
2
~
'iii
c:
.e
c:
CI)
u
c:
CI)
u
en
CI)
c:
E
::l
'0
'0
..c:
c..
7.2 ~easurenaents
by ~eans of Capacitance Spectroscopy
200nm DOTS
400nm
DOTS
As expected, the total energy of the system read from the spectrum in-
creases when the dot size decreases, and so does the distance between subse-
quent peaks (i.e., the chemical potential). It is, however, interesting that the
resolution of peaks becomes worse for smaller dots. The clearest spectra were
obtained for a diameter of 300 nm. As the authors write, this may be caused
by a competition between two opposite effects: (i) decreasing the system size
enlarges the distances between the energy levels and leads to a clearer sep-
aration of individual peaks, and (ii) brings about the important increase in
the effects related to edge defects, which broaden the peaks. It was therefore
impossible to register the peaks for dots with diameter 100 nm. Hansen et al.
[51] for the first time observed the rearrangement of the energy levels of a dot
under the influence of a magnetic field. The dots investigated were prepared
by growing on the AIGaAs surface, slightly above the interface between the
modulation-doped GaAs layer and the AIGaAs layer, the regular lattice of
about 10 5 squares of GaAs, 30 nm thick and with 200-400 nm side length.
Covering this structure with a metal electrode and applying a voltage re-
sulted in the creation of an attractive potential under the GaAs squares, due
to the locally larger distance between the quantum well and the electrode,
and hence in the confinement of two-dimensional electrons from the hetero-
junction. The measurements were taken at temperatures 0.7-4.2 K, while the
magnetic field was varied in the range 0-2 T.
Figures 7.2-4 present three diagrams from the paper cited, measured for
an array of dots with side length 300 nm. Figure 7.2 presents the dependence
86 7. Capacitance Spectroscopy
...0. 0·0
00 •• 0.
°
",000 _ ••• 0 •
150 .':: 0ni 0 0 o. 0
o
D 00. e • 0 0 ·0
100 ~.- ?~. 0 0 •• 0 0 0
. ; 0 • 0 0
50 _ • ••• cp .....i • 0 0 •.
:>
_E 0
"0 -
00
j~~- [ •
~,,~. _, '!lP[ 0 0
0
o. •
••
0
(!)
•
._.
DON i~
--'YO
f •
•
0
00
......... 0.···
• ~ooo~.
...
-100 • .........------, • • • 0
-150
_. ___ •••
o
Fig. 7.3. Magnetic-field evolution
...--,_ ............. .
~_. 0 0 " 0 0 0 0 •••
of potentials VG corresponding to
-2oo~-"•• •
•• • 0 0
••• the maxima in Fig. 7.2 (chemi-
cal potentials of the dot with dif-
-250L----:.---L....--.L...._ _ _ _...J ferent numbers of electrons). Full
0.0 0.4 0.8 1.2 1.6 2.0 (empty) circles - strong (weak)
B (T) peaks in Fig. 7.2 [51]
7.2 Measurements by Means of Capacitance Spectroscopy 87
300nm dots
f=10kHz
8=30T
ic:
:l -
-
.ci
-
...
CU
> - 0.5K
~"C - 1K
2K
3K
Fig. 7.5. Capacitance spectra of the
quantum dots in a magnetic field of
30 T; minima occurring at low tem-
-O.l -0.1 0.1 D.l 0.5 0.7 peratures correspond to fractional fill-
VG (V) ing factors v = ~ and % [52]
This seems to be closely related to the fractional quantum Hall effect, which
occurs in two-dimensional systems. According to the authors, this is also
confirmed by the observed values of the magnetic field and temperature at
which this effect occurs. It may be also mentioned that in the magnetic field
30 T the magnetic length is as small as 4.5 nm, and the respective diameter of
the 30th orbit in the lowest Landau level is 25 nm. Hence, the dots used for the
measurements (diameter 300 nm) could not produce a spatial confinement
comparable with that due to the magnetic field, and the quantization of
energy in this regime had a purely magnetic (Landau) character, as in a
two-dimensional system.
Ashoori et al. [3, 4, 5] describe the spectroscopic measurements of single
quantum dots by means of a new method, called by the authors single electron
capacitance spectroscopy (SEeS). In [3] the dot diameter was on the order of
1 /-Lm, and the number of electrons was varied over a very wide range, from
zero to several thousand electrons. The measured separation between the low-
energy levels was several meV. This was much more than was expected as a
result of the spatial confinement in a dot with diameter 1 /-Lm. Therefore, the
authors concluded that the electrons were localized in smaller areas inside
the dot, in the local potential fluctuations.
In [4] Ashoori et al. report the investigations that were carried out on a
smaller dot, with diameter about 350 nm, containing 0-50 electrons. The con-
finement of electrons was obtained in the same way as reported by Hansen
et al. [51], i.e., by growing a circular GaAs disk over the GaAs/ AIGaAs
quantum well, and covering it with a slightly wider chrome electrode. The
7.2 Measurements by Means of Capacitance Spectroscopy 89
transitions in the ground state induced by a magnetic field. In Fig. 7.7 they
are marked with circles and triangles. As shown in Fig. 3.2, the ground-
state energy of two noninteracting electrons (both particles on the 100) Fock-
Darwin orbital with opposite spins) increases monotonously with the increase
in the magnetic field. Thus, the occurrence of peaks must be related to the
effects not taken into account within the simple approach that led to Fig. 3.2,
for example with the spin-orbit interaction and/or interaction between the
neighboring dots. It seems that the spin-orbit interaction [70] (see Chap. 9)
gives a proper explanation of these small inflections on the curves expressing
the dependence of the chemical potential on the magnetic field, which are
measured by means of capacitance spectroscopy.
In numerous works attempts have been made to explain the occurrence
of the characteristic irregularities in the dependence of the energy (or the
chemical potential) on the magnetic field without taking into account the
spin-orbit interaction, but based rather on an analysis of the crossings of
the single-particle Fock-Darwin levels. In such an approach the transitions
in the electron system under an increasing magnetic field can be classified by
a division into three stages, with respect to the value of the filling factor, (i)
v > 2, (ii) 1 < v < 2, and (iii) v < 1, and the mechanism of the transition
that dominates in each stage.
(i) Let us define the average numbers of single-particle excitations with
frequencies w± (see (3.16)) in N-electron quantum state cp:
N N
(n+)¢ = (cpl Laiai Icp), (n_)¢ = (cpl L bib i Icp), (7.5)
i=l i=l
where the pairs of operators (a,a+) and (b,b+) are defined by (3.11). Ac-
cording to (3.19), the asymmetry between the numbers of excitations of both
types is determined by the projection of the angular momentum of the sys-
tem:
(7.6)
The total energy of state cp contains single-particle terms: nw+ (n+) and
nw_ (n_). The first of these quickly increases, while the second decreases
to zero with an increase in the magnetic field. In stronger fields the higher-
energy excitations (nw+ ~ nwc ) correspond to the excitations between Lan-
dau levels, whereas the lower-energy excitations (nw_ « nw c ) correspond to
the excitations within a Landau level.
Due to the exact degeneracy of frequencies w+ and w_ in a zero magnetic
field in the ground state of the system cp in weak fields the projection of the
total angular momentum vanishes: (l z) ¢ = o. The energy of state cp increases
quickly with an increase of the magnetic field and at the critical value crosses
the energy of another state 'Ij; that has a nonzero projection of the angular
momentum (lz),p > 0 (due to the asymmetry of excitation energies, nw_ <
nw+). The state 'Ij; becomes a new ground state of the system. Since Ll (n+) =
92 7. Capacitance Spectroscopy
(n+) 'Ij; - (n+) q, > 0, the change of the ground state can be interpreted as
a transfer of a fraction of electrons (charge) from higher to lower Landau
levels (possibly with a simultaneous change of the spin configuration of the
system). Thus, the resulting peak in the magnetic-field dependence of energy
is a consequence of the crossing of the single-particle Fock-Darwin levels. A
further increase of the field is accompanied by subsequent transitions, until
all the electrons drop to the lowest Landau level: (n+) = 0 in the state
with filling factor v ~ 2. Transformations of the system of 1-6 electrons that
correspond to this stage are described in [133J (see Sect. 8.2).
(ii) A further increase of the magnetic field leads to a compression of the
system of electrons in a constantly diminishing area, since in strong mag-
netic fields the characteristic dimensions of electron orbits are scaled with
the magnetic length lB ex 1/~ (see Sect. 4.3). Thus, with an increase of
the field, the Coulomb energy of the system E ex 111B quickly increases. On
the other hand, the increase of the field reduces the energy of single-particle
excitations to states with greater orbital diameter (in the limit B ----* 00 the
Fock-Darwin spectrum rearranges into the system of degenerate Landau lev-
els; see Sect. 3.3). Moreover, in the state with v ~ 2 the total spin of the
system is close to zero, and the (attractive) exchange interactions are weak.
At the critical value of B, a fraction of charge is transferred from the inside of
the dot to the outside (at the same time reversing the spin) in order to mini-
mize the total energy of the system. The spin direction 1 (along the field B) is
preferred by the Zeeman interaction. However, the energy of this interaction
is considerably smaller than the energy of the exchange interaction.
Hence, the reason for transferring a fraction of charge from the inside of
the dot to the outside is the repulsive direct interaction, whereas the rea-
son for the change of spin configuration (increase of the total spin of the
system) is the attractive exchange interaction between electrons. As a result
of subsequent transformations, the system goes through a sequence of states
with an increasing number of tightly packed spin-l electrons and a decreasing
r
number of spin- electrons, until complete spin polarization is reached. The
completely polarized state closing the sequence has filling factor v = 1 and
is called the compact droplet (see Sect. 4.7).
(iii) A further increase of the magnetic field leads to the reconstruction
of the compact droplet, which occurs by introducing the holes to its inte-
rior. This corresponds to a further reduction of the filling factor v. These
transitions are described in Sects. 4.4 and 4.7.
The numerical calculations including the Coulomb interaction between
electrons were carried out, for example, by Hawrylak [55J and Young et al.
[138J (exact diagonalization of the Hamiltonian for a small n~mber of elec-
trons) , and also by Palacios et al. [107J (exact diagonalization and the
Hartree-Fock approximation). It should, however, be stressed t.hat. in this
approach realistic values of the measured parameters can be obt.ained only
for 2-3 elect.rons. The chemical potent.ial of the N-elect.ron dot, equal t.o
7.2 Measurements by Means of Capacitance Spectroscopy 93
B c
;;-
Ql
J D
E
1
~
..-
~
LY -0.1
N
W I
M
i[
>-
OJ
~ -0.2'
Ql
OJ
C
.~
Fig. 7.8. Chemical potential of
(ll three electrons in a quantum dot
.s:::. as a function of the magnetic
()
field; full circles ~ experiment [4J;
empty circles ~ average measure-
-O.3~~~....,.---.,...--...;..,.--"","",
0.0 2.0 4.0 6.0 8.0 ment error>::: 0.03 meV; solid line
Magnetic Field (Tesla) ~ numerical calculation [55J
15.6 -
~
E 15.4 -
........
,g B [TJ
;C 3 4 5 6 7
..-IN ............ N=6 15
I - -_______
::l 15.2 .. -....... N=5
-----------
N=4
---_ _____ 10
.......... ~- N=3
15.0
N=2
.-------------___ 5
2 3 4 5 6 7
B [T]
Fig. 7.9. Dependence of the chemical potential of six electrons in a quantum dot
on the magnetic field; pairs of numbers L,28 denote the states (L - angular mo-
mentum, 8 - spin projection). Inset: chemical potential for two to six electrons
[138]
of Palacios in Fig. 7.10 with the experimental data in Fig. 7.7. Clearly the
distances between the consecutive curves f..LN(B) do not agree (e.g., the cal-
culations give: f..L2(0) - f..Ll(O) = 7.6 meV instead of 4.2 meV measured by
Ashoori), nor do the values of the magnetic field at which the inflections on
the curves appear (e.g., for N = 15 the theoretical value of the field at which
the irregularity of a chemical potential occurs is 8 T, while the experimental
value is on the order of 2 T). Although the first discrepancy could be elimi-
nated by the effective reduction (~ 2 x) of the interaction between electrons
(e.g., by assuming a larger broadening of the electron wave functions across
the dot), the elimination of the second discrepancy requires (on the contrary)
the interaction to be enhanced. This proves that another effect plays a cru-
cial role in the Ashoori's experiment, which has been neglected so far in the
calculations.
Hallam et al. [50] analyzed the influence of the screening of the inter-
actions between the electrons confined in the quantum dot by the electric
charge present in the electrodes. They showed that for the parameters that
correspond to the Ashoori's experiment (the distance between the dot and
each of the two electrodes equal to 80 nm) the screening leads to a consider-
able lowering of the curves f..LN(B) and to a decrease in their separation. For
instance, the separation f..L3(0) - f..L2(0) is reduced due to screening from 2.1 to
1.4 meV (~30%), and f..L4(0) - f..L3(0) decreases from 2.7 to 1.5 meV (~45%).
7.2 Measurements by Means of Capacitance Spectroscopy 95
60
•
~
• 0
.N - 10
•
- •
•
D
• --
..
0
..-
0----, •
..
.. O~
•
•
N-S_
-
D
--
----
~
~
------
20
•
to
1.0 r - - - - - - - - - - - - -
1.0
6----
<:I 1.0
Fig. 7.11. Oscillator
strength ("'tunneling
intensity) of the transi-
1.0
tions between the elec-
trode and the quantum
dot, determined for two
to five electrons, as a
function of the magnetic
B (T) field [107]
InGaAs/GaAs SAD
s=180A
where Ve = 0 inside the wetting layer and the dot, and Ve = Vo within the
barrier (Vo = ..:1VCB is the difference between the conduction-band energies
in the two materials, including the effect of strain).
In order to solve this equation two methods were used: (a) The full diag-
onalization of the Hamiltonian in the space of three-dimensional wave func-
tions. In order to construct a convenient set of discrete basis states, the
system was embedded in a large cylinder with an infinite potential barrier
at the edges; (b) The adiabatic approximation. Since the full diagonalization
showed that the adiabatic approximation gives very accurate results, we shall
discuss here only the second method, which is more physically intuitive.
In the adiabatic approximation we can take advantage of the fact that the
electron wave functions are strongly confined to the lowest subband in the
narrow wetting-layer quantum well. Thus, we can write the wave function as
a product
(8.3)
(8.4)
First, the energy Eo(r), which corresponds to the electron motion in direction
z, is found for a given layer thickness, i.e., at a given distance r from the center
of the dot (Eo (r) is the effective lateral confining potential V, shown in the
corner of Fig. 8.1). Next, the equation for the radial motion of an electron
in the effective potential Eo (r) is solved numerically, separately within each
subspace with a fixed value of angular momentum. In order to solve this
equation, the potential Eo(r) is approximated by the n-step function
(8.5)
where 0 ::; i ::; n, So = 0, Sn+1 = 00, Si < SHI, and Vi < VHI. The wave
function that corresponds to energy E and angular momentum m can be
written in a compact form
(8.6)
where k; = IE - Vii and (F, G) is the appropriate pair of cylindrical Bessel
functions: (Jm, Y m ) for E > Vi and (Km, 1m) for E < Vi. The wave functions
must be continuous and smooth at each interface:
Ai-IFF + Bi-1Gf AiFiR + BiGf (8.7)
Ai - I V' FF + B i - I V'Gf AiV'FiR + BiV'Gf· (8.8)
In the above equations we use the following notation:
FF == F(ki-ISi ), V'FF == ki-lF'(ki-ISi),
Ff' == F(kisi ), V'FiR == kiF'(kis i ), F = F, G. (8.9)
The coefficients (A, B) are related to the transfer matrix Tj by
[BAj] = Tj [AB j-
J J- I
I ]. (8.10)
Based on (8.7-8.8):
(8.11)
(8.12)
From the condition that the wave functions are finite in the center of the dot
we obtain
100 8. Properties of Self-Assembled Quantum Dots
Bo = o. (8.13)
The energies of bound states Eb are obtained from the condition that the wave
functions vanish in the limit of the infinite radius. This additional boundary
condition,
Bn=O, (8.14)
is equivalent to the vanishing of the corresponding element of the total trans-
fer matrix,
(8.15)
for the discrete set of energies E b .
Electrons with the energies E from the interval that corresponds to the
two-dimensional continuum of states in the wetting-layer quantum well move
in a scattering potential of the quantum dot. This scattering modifies the
electron density of states. The phase shift 'f]m (E), which corresponds to energy
E and angular momentum m, can be expressed in terms of the transfer matrix
as
'f]m = arg(Tu - iT21 ), (8.16)
whereas the change in density of states due to the presence of the scattering
potential reads
300
250
~
g rr
>- 200 a
.... I -- 1 c:
--
C>
Q)
c
II -- 3
::J
0.
Q)
150 II ~ ---- 6 en
6D m ,I ------ 7 Q)
I ,I
II CD
I ,I en
100 I " "
o Tc.: "
t!_~\_~_#
-100
~
.s
'"
<{
'"
Cl -200
>I
W
A.V cb =350meV
-300 h/s=O.24
a 100 200 300
s (A)
a
~ -100
.s
'"
<{
'"
Cl
>I -200
W
-3001-~~~'-~~~~~~~~~~~
o 100 200 300 400
AV cb (meV)
Fig. 8.3. Dependence of the energy spectrum of an electron confined in a self-
assembled dot on the dot radius (upper frame) and on the height of the potential
barrier at the InGaAs/GaAs interface (lower frame). The arrows indicate the spec-
trum in Fig. 8.2 [134]
number of bound states. For the dot size chosen for this frame (based on
[41, 114, 115]) clearly separated shells occur in the whole range of Vo.
Connecting both dependencies in Fig. 8.3 it is possible (at least in princi-
ple) to design structures containing the self-assembled dots with an arbitrary
number of bound shells, which are separated by an arbitrary energy We'
Another piece of useful information that can be derived from Fig. 8.3 is a
possibility of connecting a measured distribution of dot sizes in a macroscopic
sample with an inhomogeneous broadening of the density of states. It is
obtained that the homogeneity of dot sizes in the described sample [41, 114,
115] is sufficient to preserve the discrete density of states characteristic of the
zero-dimensional system.
As shown previously, the energy spectrum of an electron confined in a
self-assembled dot can be to a good approximation described as a truncated
spectrum of a two-dimensional parabolic well. Let us now proceed to the
states of a valence-band hole. Due to the strain in the InGaAs layer, the sub-
bands of light and heavy holes in the valence band are strongly split, and the
mixing of states from these two subbands is considerably reduced. Thus, the
states of a hole in a dot, within the band-structure model, can be described
in a way similar to that of the electron states, only with different effective
mass (which for a hole is no longer isotropic) and potential discontinuity at
the interface. Assuming the appropriate parameters the energy spectrum of
a heavy hole in a dot was determined. It is very similar to the electron spec-
trum. The number of the bound, almost degenerate shells is also five, while
the distance between the shells nwh = 15 meV.
The Hamiltonians of the electron He and hole Hh confined in a two-
dimensional parabolic well in a magnetic field B along the z-axis can be
diagonalized analytically. The single-particle eigenstates are the Fock-Darwin
states described in Sect. 3.3. We have checked (carrying out exact numerical
calculations, similar to those described for a zero-field) that the magnetic-
field evolution of the electron and hole energy levels for the realistic confining
potentials V(r, z) is almost identical to that of the Fock-Darwin spectrum,
truncated to the appropriate number of the lowest levels.
150
~
g
>-
!?
(J) 100
c:
(J)
o 6 10 16 20 25 30
magnetic field (T)
Fig. 8.4. Exact energy levels of a self-assembled dot (circles) and the Fock-Darwin
levels (lines) in a magnetic field [133]
(8.18)
where c;t (co<) is the operator creating (annihilating) an electron in the single-
particle (Fock-Darwin) state a == In+n_a"), and Vee is the matrix element
of the Coulomb interaction, given explicitly in [56] (see 4.32 for the lowest
Landau level).
The Hamiltonian (8.18) conserves the total angular momentum L, as well
as length S and projection Sz of the total spin of the system S. The diago-
nalization will be carried out separately in the subspaces of states with fixed
values of (R, Sz)' The basis of N-electron states is constructed in the form
of the properly antisymmetrized products of the Fock-Darwin single-particle
states:
(8.19)
For each value of the magnetic field only the four lowest Fock-Darwin states
are used (marked with continuous lines in Fig. 8.4), which correspond to the
bound single-particle states and (in weak fields) to the resonance with angular
momentum L = 2. The presence of higher-energy states, i.e., the interaction
of the Fock-Darwin bound states with the continuum of scattering states is
neglected. However, the presence of the continuum is included indirectly, as
it has an effect on the calculated single-particle states and the characteristic
frequency Wo (see Sect. 3.3). In Fig. 8.5 we present the ground-state energies
of the system of 1-6 interacting electrons in a magnetic field, calculated by
the numerical diagonalization of the Hamiltonian (8.18). The curves that
correspond to different numbers of particles N are vertically shifted, so that
they can be shown in one frame. The energy values in the absence of a
magnetic field are given on the vertical axis, and the arrow in the top-left
corner shows the energy scale common to all curves. The pairs of numbers
in parentheses (total angular momentum, total spin projection) = (L, Sz)
define the system configuration. Due to the small dimensions of the quantum
dot, the characteristic interaction energy (00; OOIVeeIOO; 00) ~ 30 meV (100) is
the lowest Fock-Darwin level) is considerably smaller than the characteristic
confinement energy fiJ.,Jo = 50 meV. As a result, the N-electron ground states
are close to the configurations with the lowest single-particle energy (kinetic
energy plus the confining potential of the dot). Subsequent electrons occupy
the lowest available single-particle states (according to the Pauli exclusion
principle), and the coupling between the states with different single-particle
energies is weak. Thus, the main effect of the interaction is the displacement
of the energy spectrum of the noninteracting system toward higher values
by the interaction energy, weakly dependent on the magnetic field and the
system configuration (but strongly dependent on the number of particles).
The Coulomb interaction and the spin configuration of the system play
a crucial role when in the absence of interactions the ground state is de-
generate (partially filled shells). The ground states of the system of one to
106 8. Properties of Self-Assembled Quantum Dots
~
g (0,0)
6; 804 5
a;c: 606
Q)
Q)
+-'
ctI 4
+-'
C/)
I
"0
c:
::J
o
L-
0)
1301------
50~-------------
o 5 10 15 20 25 30
magnetic field (T)
Fig. 8.5. Dependence of the ground-state energy of two to six electrons on the
magnetic field. The curves are vertically shifted, and the vertical axis gives the
energies in the absence of a magnetic field. The arrow in the top-left corner gives
the energy scale that is common to all curves. Pairs of numbers on the curves are
(L, Sz) [133]
its ground state. In the new configuration the pair of electrons, primarily spin
polarized, occupies the orbital with L = +1, and the total spin of the system
Sz = O. This is the configuration with the lowest single-particle energy.
The change of the ground state in the system of five electrons at the
magnetic field of ~ 15 T corresponds to the transfer of an electron from the
L = -1 orbital to the L = +2 orbital, in the presence of a rigid core composed
oHour electrons in the two lowest orbitals L = 0, +1. The transfer takes place
earlier than the crossing of the corresponding single-particle levels, because
the Coulomb energy of the new ground state is lower.
In the case of six electrons, the consecutive two electrons jump from the
L = -1 orbital to the L = +2 orbital. Between the transitions, (when the
pair of jumping electrons occupy different orbitals, the system asSumes the
largest possible length of spin, Sz = 1, in order to decrease the total energy
by the exchange term (analogously as for four electrons).
Figure 8.6 presents the chemical potential of one to six electrons confined
in a self-assembled dot and in the magnetic field, which was calculated within
the band-structure model of a quantum dot. The chemical potential J-lN is
defined as the difference of ground-state energies of Nand N - 1 electrons
(drawn in figure 8.5), i.e., as the energy required to add the Nth electron to
the quantum dot containing N -1 electrons (see Sect. 7.1). The main graph
presents the difference between the chemical potentials of the interacting and
noninteracting systems, J-l - J-lni, i.e., the energy of the Coulomb interaction
between the dot containing N - 1 electrons and the added Nth electron
(the charging energy). The chemical potential of the noninteracting system is
equal to the energy of the Fock-Darwin level to which the electron is added,
i.e., the first unoccupied level (see Fig. 8.4). The transitions in the ground
states of four, five, and six electrons in the magnetic field are accompanied
by the changes of slope of the curves J-l- J-ln;, marked in Fig. 8.6 with circles.
The change of slope for five electrons in the magnetic field of 20.5 T is due
to the crossing of the pair of Fock-Darwin levels (hence this is a change of
ground state in the noninteracting system).
The exact N-electron states are close to the noninteracting, single-particle
configurations, which are only slightly modified by the Coulomb interaction.
Therefore, it can be approximately assumed that the Nth electron is added
to a given, unoccupied single-particle Fock-Darwin state, in the presence of
a repulsive electrical potential, which is produced by the charge of N - 1
initially confined electrons. On the curves in Fig. 8.6 we have marked the
angular momentum and spin of the state to which the Nth electron is added.
The smaller graph in the inset to Fig. 8.6 shows the total chemical po-
tential of the quantum dot J-l, which is the directly measured quantity in the
capacitance-spectroscopy experiments (see Chap. 7). The dashe'd line repre-
sents the energy of the lower edge of the continuum of scattering states in the
quantum well. As can be seen in the figure, only three to four electrons can
be bound in the dot with energy below the continuum. However, a couple of
108 8. Properties of Self-Assembled Quantum Dots
~ -It 1t 4
---
60
.5 V
'c
::i.
I
::i. 6
40 1t 3 200
~
5
-
ot 2
_-------4-
--- --- ---
150
3
20 J..L
100
2
o ot N=1
50
1
0 5 10 15 20 25 30
o 5 10 15 20 25 30
magnetic field (T)
Fig. 8.6. Addition energy (chemical potential) of one to six electrons in a quan-
tum dot, as a function of the magnetic field. Angular momenta and spins of the
single-particle states to which electrons are added are indicated. Main frame: differ-
ence between the chemical potentials of the interacting and noninteracting systems.
Inset: chemical potential of the interacting system [133]
additional electrons can be captured in the resonance states above the con-
tinuum edge, which may be stabilized by the potential barrier that appears
at the edge of the dot due to the drop of the confining potential.
The number of electrons that can be bound by a dot depends on its size.
Assuming that the dot radius is 25 nm (instead of 20 nm), we have obtained
the distance between the single-particle energy levels actually measured by
Drexler et al. [37] (41 meV). As a result of the calculations cafl'ied out for
s = 25 nm we have obtained that the maximum number of bound interacting
electrons in a dot is five.
It should also be noticed that the real strength of the Coulomb interaction
between electrons is slightly weaker than that included here. This is due to
8.2 Electron System in a Magnetic Field 109
the finite broadening of the electron wave function across the dot [56] and the
screening by the charged electrode [50] (see also Sect. 4.6). We have checked
that the assumption of the effective broadening of the electron charge across
a dot over a length of 5 nm leads to a reduction of the values of Coulomb
matrix elements by ~ 10%.
Figure 8.6 describes only those processes in which the dot passes from
one ground state (N - 1 electrons) to the other (N electrons). However, in
the case of reduced probability (intensity) of a transfer of an electron from
the electrode to the final ground state of the dot, the transfer of an electron
to an excited state of the system can be observed [107]. This can happen,
for instance, in strong magnetic fields, when the electrons in the electrode
from which they are injected to the dot are spin polarized (transfer of an
electron between the electrode and the dot takes place without a change of
spin). Hence, the capacitance spectrum can additionally reflect the effects
connected with the changes of the state of the reservoir of electrons, i.e., the
metal electrode, induced by a strong magnetic field.
In the first order of perturbation, the probability of transferring an elec-
tron from the electrode to the dot is given by the golden Fermi rule (written
here separately for each spin projection of the transferred electron):
210
200
190
180
170
160
150
240
230 .. ' o ~. ..'
>a;
0 ••••
220
~
.-z 210
LlJ 200
CI)
(!J
I 190
z
LlJ 180
170
250
240
230
220
210
200
190 N=6
o 5 10 15 20 25 o 5 10 15 20 25 30
magnetic field (T)
Fig. 8.7. Evolution of the electron addition spectrum of a quantum dot in a mag-
netic field. Areas of circles are proportional to the intensities of individual transi-
tions; continuous lines give the chemical potential [133]
90
80
70
60
50
40
30
20
90
~ 80
..s 70
z 60
UJ
CfJ 50
(.!)
'z 40
UJ 30
20
90
80
70
60
50
40
30
20
o 5 10 15 20 25 o 5 10 15 20 25 30
magnetic field (T)
Fig. 8.8. Magnetic-field evolution of the FIR absorption spectrum of a self-
assembled dot. Areas of circles are proportional to the intensities of individual
transitions; continuous lines give the energies of single-particle excitations [133]
N
A(w) ex :L I (fl :L(aj + at + bj + bj) Ii) 2 8(EJ
1 - Ei - w), (8.21 )
J j=l
where Ii) is the initial (ground) state ofthe quantum dot, and the summations
run over all bound final states If), and over all electrons. The operator of the
interaction with the FIR radiation connects the electron states Ii) and If)
with equal total spins and orbital angular momenta differing by ±1.
In Fig. 8.8 we present the evolution of the FIR absorption spectrum of
one to six electrons in an increasing magnetic field. The areas of circles are
proportional to the intensities of individual transitions A(w). The continuous
lines give the energies of resonance single-electron (center-of-mass) excita-
tions nw±, defined by (3.16). The visible deviations from the single-particle
spectrum (an effect of coupling between the center-of-mass and relative mo-
tions of the system) increase when the number of particles increases. For
larger N the small number of the bound single-particle states becomes par-
ticularly important. For instance, at the magnetic field B = 30 T it is not
possible to construct a state of six electrons with total angular momentum
L = 7, and there is no line that corresponds to the energy>::: w_ in the FIR
spectrum. The deviations disappear with an increase in the number of bound
Fock-Darwin states, i.e., when the dimensions of the dot increase.
We can take advantage of the fact that the single-particle states of self-
assembled quantum dots are almost exactly the states of a two-dimensional
harmonic well, and write the approximated Hamiltonian of an exciton (an
electron-hole pair) in a magnetic field in the form
(8.22)
where (the index e refers to the electron and h to the hole) m* are the
effective masses (in the case of the hole it is the mass in the plane of the
quantum well), r are the positions, p are the momenta, A = ~B x r is
the vector potential of a magnetic field B (in the symmetric gauge), and
ware the characteristic frequencies of the effective confining potentials V,
determined by the diagonalization of the single-particle electron and hole
Hamiltonians, as described in Sect. 8.1. The last term of the Hamiltonian
(8.22), Veh, describes the electron-hole Coulomb attraction. For simplicity,
we omit here the Zeeman spin splitting (negligible for GaAs).
8.3 Exciton in a Magnetic Field 113
X
L
Pe=O
Pel L
qe=O
qe! L
Ph=O
Ph! L
qh=O
qh!
(8.24)
Here (in the case of absorption) Ii) denotes the initial state of the system (an
empty dot), and If) runs over all possible final states (a single exciton in the
dot). P is the dipole transition operator, which, neglecting spin and using
the composite index i = [n+, n_], can be written in the form
where c+ and h+ are the operators creating an electron and a hole in a given
single-particle state. In terms of wave functions, the dipole matrix element
(fIPli) can be written in the form
P+ IX L
io,ih
ht.r (ielih) ,
<1
The linearly polarized photon (L) excites an electron with the spin function
in the form of the symmetric combination of states 1 and i:
(8.29)
j =m+(j
+112 t @
± 112 electron
-112 ~ @
heavy
±3/2
hole
-3/2 ~
~
+3/2 t
t
light +112 ~ t
hole
±112
-112 t !
Fig. 8.9. Interband optical transitions between the heavy-hole (j = ±~) and light-
hole (j = ±~) subbands of the valence band (m = ±1), and the conduction band
(m = 0, j = ±~), for the two circular polarizations of light: 0"+ and 0"_
(creating electrons and holes with different spins) are equal. Denoting the
expansion coefficients of the exciton eigenstates in the basis (8.23) by
On the other hand, the polarization of light (spin) plays an important role in
the investigation of emission, when it is possible to control the spin config-
uration in the initial state by the application of an external magnetic field,
and thus to change the distribution of the emitted light into the pair of com-
ponents (J + and (J _ •
As shown in [132]' the effect of polarization appears in the absorption
spectrum when a dot in the initial state is not empty, but contains a confined
electron (a hole). The presence of a particle in the initial state, with a spin
that is controlled, for instance, by the magnetic field, partly blocks the space
of available final states (due to the Pauli principle). For instance, if there
was an electron with spin 1 in the initial state, only the absorption of a (J_
photon can lead to the creation of a bound complex X- (negatively charged
exciton) with a pair of electrons in the spin-singlet configuration 1i - i 1
(zero total spin of the pair). Thus, if we compare a pair of absorption spectra
116 8. Properties of Self-Assembled Quantum Dots
that were registered for the two polarizations of light (J" _ and (J" +, then for the
process "y -+ X (initially an empty dot) they will be identical, whereas for the
process e- + "y -+ X- (initially a bound electron) they will be different: In
the spectrum (J" _ a new peak with the lowest energy will appear (lower than
the energy of the first peak in the spectrum of an empty dot by the electron-
exciton binding energy). The experimental identification of a bound complex
X-, based on a comparison of the two spectra (J"+ and (J" _ , is reported in
[82,83].
Below we present some selected results concerning the calculations of
the absorption spectra within the band-structure model, applied to the self-
assembled dots described in [114, 115]. Figure 8.10 presents the evolution
of the absorption spectrum in an increasing magnetic field B, determined
for the same parameters as in Fig. 8.2. The upper frame corresponds to
the noninteracting electron-hole pair, and the lower frame to the interacting
magneto-exciton. The areas of black circles are proportional to the intensities
of individual optical transitions (peaks in the absorption spectrum), while the
energies of these transitions (measured from the band gap) are given on the
vertical axis.
In the absence of the electron-hole interaction all allowed transitions have
the same intensity, and their evolution in a magnetic field is similar to that
of the Fock-Darwin spectrum of each of the particles. For chosen transitions
we have indicated the orbitals In+n-), in which the electron-hole pair is
excited. Figure 8.10 demonstrates the magnetic-field-induced breakup and
restoration of the dynamical symmetries of the Fock-Darwin spectrum. At
certain magnetic fields (B = 0, 12, 19, and 25 T) the levels cross, and the
intensities of neighboring peaks add up. For instance, at B = 0 the observed
overall intensity increases linearly with energy.
The Coulomb interaction leads to a certain rearrangement of the spec-
trum, as shown in the lower frame in Fig. 8.10. However, the spectrum of
a magneto-exciton slightly resembles the spectrum of a noninteracting pair;
in particular, at B ~ 13 T we observe a reconstruction of almost degen-
erate groups of strong transitions, separated by wide gaps. The reason for
this resemblance are the small dimensions of typical self-assembled dots. The
characteristic energy of a confining potential: fiJ..J e + fiJ..Jh (~ 45 me V) exceeds
the characteristic energy of the Coulomb interaction (~ 25 meV). The main
effect of the interaction is thus a parallel shift of the entire spectrum toward
lower energies (red shift), by the (approximately constant) binding energy of
the pair.
Figure 8.11 presents the absorption spectra in the absence of a magnetic
field, with the inclusion of the inhomogeneous broadening of individual peaks
due to the distribution of dot sizes in the sample. In both diagrams (the non-
interacting electron-hole pair and the interacting exciton) the broadening of
peaks does not exceed fiJ..J e + fiJ..J h , and there are five strong, clearly resolved
maxima, which correspond to five shells in the electron and hole energy spec-
8.3 Exciton in a Magnetic Field 117
..
x .' • ••••••••
'"~
o>
100 x2 [!Q]... ••• •••••••••
••••• , •• • •••••• ~
~
,::: ........•.•.....•.•..• ~
~ ~
~
•••••••••••••••••• • • • • • • • • • • !QQlo
50 x1
I without interaction
O~~~~~~~~~rr~~~~~~~~
250.-------------------r------------,
· .• ' .... i· .jwith interaction
,:• ...••
• • • :.
• ·a· ... · .~. e.. ..•.
.- :., .._, •
• • •• • ••• io-.......-c..--....---.---=---!
.~~.
200 • •- •• •• z.
••'. :·i.···
.. ~~. .::",i'~~
... .... ,..
:: •.••.. ' - •••
~ ~·l.;·~!·
: ..•••..••
:~.
150
.. ;
'
•••..
... .
....!!~.;:.' •••.
.'
':'.i;~~: :::.
. : •••• !t , . . . . . . . .
. ... , .:'.'.Ii
~~;.'i·· •• : •
' ·~········i
. ' ..
...... ,!
.1 .. '
• ··'~.....
..
•••••• I . "~,.::: • • • i ·' •• '
.
100
::::: :;;
.. .Iil' •••••••••••..
. .....
, ••
•••••••• ....... .
• • • • • • •• ••••••••••••••••••••••
50
••••••••••••••••••••• ••••••••••
o 5 10 15 20 25 30
magnetic field (T)
Fig. B.10. Dependence of the absorption spectrum of an empty self-assembled dot
on the magnetic field. Areas of circles are proportional to the transition intensities.
Upper frame: noninteracting electron-hole pair (degeneracies in the absence of a
field and the Fock-Darwin states for chosen transitions are indicated). Lower frame:
interacting exciton [134]
5 without interaction
=i 4
.3- 8=0 , CT s =10A
§ 3
'';:::;
o
0.
(/)
2
.0
co
04-~~~~~~~~~~~~~~~
5 with interaction
::j Fig. 8.11. Absorption
.3 4 spectrum of a self assem-
c bled dot (in the absence
o 3 of a magnetic field). Up-
'';:::;
per frame: noninteracting
o
0.
(/)
2 electron-hole pair. Lower
.0 frame: interacting exciton .
co Broadening of peaks re-
flects the distribution of
O~~~~~~~~~~~~~~~~ dot sizes in the sample
o 50 100 150 200 250 ((8) = 18 nm, (Js = 1 nm)
energy (meV) [134]
between the peaks agrees very well with the results of calculations presented
here.
+~ L (ijIVeel kl ) ctcja,Cka'Cla
ijk/aa'
8.4 Condensation of Excitons 119
(8.35)
counts the number of created pairs. The commutation relations that connect
p± and Pz are those of the three-dimensional angular-momentum algebra
[135J
(8.36)
[H,P:]
ijk
+2
1
L ((ijlv"el kl ) - (iklVehlJ l ))
ijkla'
+ h+kaCia'
x (Cja + C/fI' + CjfI'
+ h+ + fI )
kfI' CiaCl
+2
1
L ((ijlVhhl kl ) - (iklv"hljl))
ij klfI'
(8.41 )
Using a convenient analogy between P and the total spin N of a set of spin-~
particles (the mapping c± f--+ at and h± f--+ af), the addition (subtraction)
of excitons to (from) the shell can be viewed as rotation of the polarization
vector P without changing its length P. An empty shell corresponds to P
pointing down (Pz = -~N), whereas a completely filled shell corresponds to
P pointing up (Pz = +~N). The ground-state energy of the shell is linear in
N, and the exciton addition/subtraction energy JL(N) = E(N) - E(N -1) is
a constant. Thus, despite the occurrence of strong correlations in the system,
the consecutive excitons are added to a shell with the same energy, forming
a condensate. If the excitons of both types are added (a = 1, i), the joint
CMES is simply a product of two spin polarized CMES's, and the exciton
addition/subtraction energy does not depend on a.
Dynamical symmetries that lead to the Bose-Einstein condensation of
excitons in a two-dimensional electron-hole system in very strong magnetic
fields are described in [24, 96, 99, 108].
As an illustration, in Fig. 8.12a we have drawn the energy of addi-
tion/subtraction of an exciton JL(N), calculated for the dot that was de-
scribed by Raymond et al. [ll4, ll5]. We have subtracted here the kinetic
energy (constant within each shell), so that the quantity on the vertical axis
contains only the energy of the electron-hole attraction within the added
exciton and the energy of the interaction of this exciton with otherexcitons
in the dot. The deviations from a perfectly flat dependence within each shell
« 0.25 meV) are small compared to the sharp jumps Ex at the transitions
between neighboring shells (1-3 meV), and negligible compared to the char-
acteristic energy of electron-hole attraction (16-23 meV) , or the jump of
kinetic energy between the shells (45 me V).
In the next step we shall include the scattering of electrons and holes to
higher (empty) shells. The main effect of adding the respective terms to the
Hamiltonian (8.32) is the formation of bound bi-excitons, composed of a pair
of electrons and a pair of holes, both in the spin-singlet configuration. Such
spin-singlet bi-excitons, within an isolated shell created with the following
operator,
Q+ -- '12 " + cn
0 ( cil + + Cj1
+ CiT
+)(h+h+ h+ h+)
iT jl + n il ' (8.44)
ij
interact weakly with each another and with excess spin-polarized excitons.
Denoting the bi-exciton binding energy in a given shell by Llxx, we can
write the approximate energy of the ground state (without the kinetic-energy
terms, for Nl > NT):
(8.45)
The consecutive excitons are added to a shell alternately, L 1, L ... (so as
to maximize the number of 1i pairs), and the addition/subtraction energy
splits into a pair of lines, Ex and Ex - Ll xx .
122 8. Properties of Self-Assembled Quantum Dots
-15~-----------------------,
(a) f
-17
d ~
-19
~~
p ,/ P
-21 . ~Ex
....
I
S :
-23 ~
,--....
>Q) 2 5 -'-_ _~. laolated ehelle
*
-
E with sGBtterine
- 15 (b) to hleher shells 1-----,
>-.
..... ..- ........
,.....--- . -....
0)
~
-17 , ~
Q)
~ .~
cQ) -19
/~ Af
c -21
r-..... ·~ ~
o :<!~ ~
~
u
-23 ....,'K"r':,p
,' !:lxx
]
§ - 27
-25
~~
-'-----1* without lower ehelle;
~ - 15 - r - - - - - I . with lower e;hells
~ (C) aomplt:tely flllM
-20 ~~
¢
-25 .,,1 ~~
.. ~B
1 ";tro~ f
IDI:>..
. F~ ~~~-~~-I
-30 , Si""tS
\ g
-35
~,, Fig. 8.12. Exciton addition en-
ergy of a self-assembled dot
,, o 50 100 150 200
(without the single-particle en-
,, energy (meV)
ergy): (a) squares - isolated
shells; (b) stars - with scatter-
-40 ~,, ing to higher shells; (c) circles
,, - with interaction with com-
, pletely filled shells. Inset: en-
-45
~ ergy of addition of a single ex-
citon to different shells (upper
frame), and energies of addition
o 5 10 15 20 of consecutive electrons to the
number of excitons ground state (low'er frame)
8.4 Condensation of Excitons 123
The results of the calculations for a real system are given in Fig. 8.12b,
where for each shell we have included the scattering of one electron and/or
one hole to the higher shell. Such a choice of the Hilbert space is sufficient to
obtain the effect of the bi-exciton binding. It also allows for carrying out the
calculations as far as for the four lowest shells, i.e., up to eight excitons on
shell f. The inclusion of higher-order scattering processes, which limits the
possibility of performing the calculations to lower shells, does not qualita-
tively change the curve shown in Fig. 8.12b. The main effect is the decrease
of the slope of the J.L( N) line within each shell, which then turns out to be
almost perfectly fiat (as in Fig. 8.12a). This means that the bi-exciton bind-
ing energy considerably exceeds the binding energies of larger complexes, and
the system consists of a gas of weakly interacting bi-excitons.
In the last step we shall fill all the shells below the valence shell with
excitons, so that the entire system can be divided into a compact (rigid) core
and a partially filled valence shell. The electrons and holes feel the presence of
the charge-neutral core mainly through the exchange interaction. The inter-
action between the core and the valence shell can be very well approximated
by the single-particle potentials that acts independently on electrons and
holes. Within a given shell these potentials are almost perfectly fiat, so that
the main effect of the presence of the core is a parallel shift of the exciton
addition/subtraction to/from the shell toward higher energies (blue shift).
The size of this shift (approximately constant within the shell) is the energy
of exchange attraction between the valence shell and the core. In particular,
the inclusion of the presence of the core has no influence on the occurrence
of the oscillations of J.L(N) within the shell (bi-excitons binding), or on the
slope of J.L(N) (the lack of interaction between the bi-excitons).
As shown in Fig. 8.12c, the effective renormalization of the energy of
exciton addition/subtraction (i.e., the band-gap renormalization) is a strong
effect, on a scale exceeding the oscillations within the shells (L\xx) by an order
of magnitude. In the inset to this figure we give the addition/subtraction
energies of an exciton with the inclusion of the so far omitted kinetic energy
(constant within each shell). The positions of bars correspond to the energies
of peaks that were measured in the photoluminescence spectrum.
The upper diagram describes the situation where a single exciton is added
to an empty dot (or a single exciton recombines leaving an empty dot). An
exciton can be added to any shell; the four columns correspond to the data for
N = 1, 3, 7, and 13 in Fig. 8.12a. The lower diagram summarizes the results
concerning the filling of the consecutive shells with subsequent excitons. The
following features can be seen: (i) the energy J.L(N) is practically constant
within each shell (the bi-exciton binding energy is not visible in this scale),
(ii) the bars that correspond to consecutive shells are almost equidistant, and
(iii) the distance between them is effectively reduced by ;::::: 25%, compared to
the upper diagram.
124 8. Properties of Self-Assembled Quantum Dots
s g
(f)
c
Q)
+-
c
c
o
+-
0..
\...
o
(f)
..0
o
between an exciton on shell d and a single exciton from the core (from shells
sand p) as 5.7 meV, visibly exceeding the bi-exciton binding energy on each
of these shells (e.g., Ll~x = 0.3 meV).
9. Description of a Many-Electron
Quantum Dot with the Inclusion
of the Spin-Orbit Interaction
In this chapter we shall present an analytical theory given by Jacak et al. [70],
which is based on the Hartree-Fock approximation and describes a quantum
dot that contains many electrons. The limitation of a large number of elec-
trons (a few tens) results from the perturbational character of the calculation.
However, it allows for the inclusion of the Hartree-Fock interaction with a
controlled accuracy. In addition, the spin-orbit interaction is taken into ac-
count, which seems to explain many subtle characteristics that are measured
for various dots. It should be added that the effects due to the spin-orbit inter-
action become more significant for larger numbers of electrons in a quantum
dot. Its role in this artificial atom, which is squeezed in the plane, is even
more important than in the case of ordinary, three-dimensional atoms.
Let us include the spin-orbit interaction in our model of a quasi-two-
dimensional quantum dot. This can be done in an analogous way as in a
many-electron atom, i.e., through the single-particle potential
VLS = ala, (9.1)
where l and a are the orbital and spin angular momenta of an electron. The
coupling constant a is connected with the average self-consistent field (8U),
that acts on the electron through the following relation [91]:
a = (3 (8U). (9.2)
Let us also reiterate that in an N-electron atom the dimensionless parameter
(3 equals
(9.3)
n
In the above equation is the Planck constant; m* is the effective mass; rare
the positions; A is the vector potential of the magnetic field B (B = rotA, in
the symmetric gauge: A = ~B[y, -x, 0]); land 0" are the components of the
orbital angular momentum l and of the spin ( j across the plane of motion.
In the Hartree-Fock (HF) approximation the equation for the HF wave
functions 'Ij.; has the form
Vi = e
2
jdr' ni(r') (9.6)
E Ir' - rl'
where
ni(r) = L: L:'I'Ij.;j(rO")1 2 , (9.7)
" j
31fNe ( r2 ) 2
VR(r)=-- 1-- (9.12)
4ER 2R2
(this form is also assumed for r > R). Neglecting for the moment the exchange
term, which later will be taken into account perturbatively, we obtain the
following Hartree equations:
(9.13)
parametrized by a variational variable - the dot radius R.
Let us first consider the case of a zero magnetic field. Equations (9.13) then
assume the form
n = 0,1, ... and m = -n, ... ,n, are given in Sect. 3.3.
and the explicit forms of the angular and radial wave functions, labeled by
(9.19)
t: = LN
o
. _ e22
c, E
Jd Jd' n(r)n(r')'I '
T T l T-T
(9.20)
i=l
where the subtracted integral is the energy of the direct Coulomb interaction
in the system, counted twice in the summation of Hartree energies Ci. By
introducing the Fermi energy CF, which separates the occupied and unoccu-
pied Hartree energy levels in the ground state, and calculating the interaction
integral, the following equation can be obtained:
37rN2e2
Eo = L 8(cF - c,) c, - 10ER (9.21)
i
In the above 8 stands for the Heaviside function. The Fermi energy is deter-
mined from the condition for the fixed electron number N:
(9.22)
Q = ~fJnS?b2ffi
3 . (9.26)
The details of calculation of the Hartree energy Eo defined by (9.21) are given
in [70], and here we present only the final result:
where aB = d'i,2 j(m*e 2 ) is the effective Bohr radius. Under the constraint of
a large number of electrons, the above equation can be solved perturbatively
with respect to the small parameter aBj R « 1. The zeroth-order approxi-
mation, which can be written as
R3 _ 31rNe 2 (9.29)
0 - 4fm*w2'
o
corresponds to the classical result of Shikin [120j. Assuming that the first-
order solution is of the form R = Ro(l + 8), we can obtain the expression for
the correction 8:
8= 100aB
811l"Ro
(1- (32 N ).
36
(9.30)
[2'2
o
= [22
0
(1- (32N)
36'
(9.31 )
The first term in this equation, given in [120], is the classical energy of N
interacting electrons, confined in a parabolic well:
91rN 2e2 -_ Jd r n ()
r ~2 m * wor
2 2 2
+ e2f Jd r Jd'
r n(r)n(r')
Ir - r' I . (9.34)
20f R 0
The second term, a quantum correction, is composed of the energy of oscil-
lation with frequency [20,
(9.35)
~ 70
to
a..
...
~ 60
>-
...<1>
0)
C
<1> 50
.:£
.8
(J)
"§ 40
Fig. 9.1. Dependence of
the average ground-state
o
'-
0) energy per one electron on
the number of electrons in
15 20 25 30 35 a quantum dot [70]
number of electrons
LlE = -
4V5 (
9v3 1-
3)
4VN
N7/4e 2
fRo (1 - 80 ), (9.37)
where 80 = 8({3 = 0). It has been verified numerically that the higher-order
corrections to the Fock term are negligibly small (decreasing by about an
order of magnitude with the order of perturbation). Thus we have obtained
the total ground-state energy E of the system of N electrons confined in
a parabolic well. The energy E contains the kinetic energy, the direct and
exchange Coulomb interaction energies, and the spin-orbit interaction energy
E = Eo + LlE. (9.38)
Figure 9.1 shows the average ground-state energy per one electron C = E/ N,
drawn as a function of the number of electrons N. The very good agreement
with the results of measurements is clearly visible. Two curves that corre-
spond to the values of parameter {3 = 0.3 and 0.5 lie between the classical
9.2 Quantum Dot in a Magnetic Field 133
result of Shikin et al. [120] and the experimental data reported by Ashoori
et al. [4].
Let us now consider the selection rules for the optical transitions of a
system under far infrared (FIR) radiation. The light from the far infrared
range excites the electron system, so the FIR absorption is an important tool
in experimental studies of quantum dots (see Chap. 5).
As we have already mentioned, the wavelength of light from this range
considerably exceeds the dot dimensions, and in the description of the cou-
pling of the FIR light with a quantum dot the dipole approximation can
be used (see Sect. 3.4). In the first order of perturbation, the probability of
an optical transition between the initial state Ii) and the final state If) is
proportional to the squared matrix element of the interaction,
(9.39)
where E is the electrical field, uniform over the area of the dot. The dipole
matrix element dfi does not vanish if and only if it is possible to choose the
pair of occupied Hartree-Fock states, one in the initial state Ii) and one in the
final state If), with equal spins (T and each of the orbital quantum numbers
[n, m] differing by unity,
(Tf = (Ti, Inf - nil = 1, Imf - mil = 1, (9.40)
and with the remaining occupied Hartree-Fock states being equal in pairs
in the states Ii) and If). In other words, the absorption of the FIR photon
leads to the excitation of a single electron from its (initial) Hartree-Fock
state to another (final) Hartree-Fock state with the same spin and both
orbital quantum numbers changed according to (9.40). In the Fock-Darwin
representation above selection rules take the form
(Tf = (Ti, n~ = n~ ± 1, n~ = n~,
f .
or (Tf = (Ti, n~ = n~ ± 1, n+ = n+, (9.41 )
i.e., the excited electron changes one of its orbital quantum numbers [n+, n_]
by unity. The above selection rules lead to the splitting of resonance energy:
in a magnetic field. The form of the Hartree equations with the inclusion of
a perpendicular magnetic field (9.13) is the following:
ti2 + -m
( ---Ll
2m-
1 * ( n B 1'2 + -we
2
1
4 2
2) 2
1 . - gj..tBa B + a I)
r - -nwel a 'Pi (
nl. ra )
31fNe2 )
= ( ci - 4cR{B) 'lfJi(ra), (9.43)
(9.46)
The operator BHI BB commutates with the spin ((j') and inversion (r -7 -r)
operators. The commutation with the angular-momentum operator requires
the (assumed here) circular symmetry of the confining potential. Thus, (9.46)
is always satisfied for a pair of states with different quantum numbers n and a.
However, it is generally violated for a pair of states that differ only in the
quantum number m. This leads to the forbidden crossings of levels, which
can be taken into account by changing the equation for eigenenergies (by
introducing a modulus in (9.44)):
In weak magnetic fields the function f B approaches unity and decreases for
an increasing field. With good accuracy it is possible to replace nk in the
definition of fB with no, which is defined by (9.32). The Hartree energy of
the system is expressed by equation [70]
8(B) = 100aB
8In Ro(B)
(1 _13 f~N)
2
36'
(9.55)
136 9. Description of a Many-Electron Quantum Dot
69
>-
Q)
N=32 >115
., N=32
E E
'--' ~110
Q) 67 N=31 .2
(J
t 15 105
0
0. N=30 0
0..
N=27
!o...
Q)
65 "0 100
0
0.
>-
N=29 ·E.,
OJ
!o...
.<: 95
0
Q)
63 0 2 3 4
c N=28
Q) magnetic field (T)
2
.E
(I) N=27
61
"U
c Fig. 9.2. Dependence of
:::J
0
the average ground-state
!o...
OJ ~=O.O energy per one electron on
59
the magnetic field for f3 =
0 2 3 4 0.0. Inset: chemical poten-
magnetic field (T) tial [70]
L'lE(B)
4V5 (
= - 9v'3 1 - 4VN 3) N 7 / 4 e2
fRo (B) (1 - c5 o(B)), (9.57)
where c5o(B) = c5(B; (3 = 0). The total ground-state energy of the system
reads
E(B) = Eo(B) + L1E(B). (9.58)
Figures 9.2-4 present the evolution of the average ground-state energy of a
quantum dot per one electron c(B) = E(B)/N, in a magnetic field (for GaAs,
nwo = 5.4 meV). The three diagrams correspond to the parameter (3 equal to
0.0 (without the spin-orbit interaction), 0.3, and 0.5. The curves that have
been calculated here are very similar to the experimental curves reported by
Ashoori et al. [4], obtained by means of the capacitance spectroscopy (see
the description on page 88 and Fig. 7.7). A comparison of the curves from
9.2 Quantum Dot in a Magnetic Field 137
69
;;:- N=32
~115
> N=32
"
Q)
E
........ E
......., 110
~ 67
u N=31
t
0
C1.
N=30
'-
Q)
65 -0 100
C1. .~
E
>- N=29
Ol
'- "
.r:: 95
Q)
c 63
0
a
Q) magnetic
N=28
.!
0
Vi 61 Fig. 9.3. Dependence of
N=27
u
c the average ground-state
::J
0 energy per one electron on
'-
Ol
59
13=0.3 the magnetic field for f3 =
0.3. Inset: chemical poten-
a 2 3 4 tial [70]
magnetic field (T)
69
;;:-
Q)
~115
>Ql
E E
N=32 ......., 110 N=32
~ 67 .Q
u
t N=31 ] 105
0 0
C1. 0.
'-
Q)
65 N=30 -0 100
C1. .~
>-
E
Ol
'- N=29 .r::"
0
95
a
Q)
63 2 3 4
c
Q) magnetic field (T)
.! N=28
2CIl
61
u
c N=27 Fig. 9.4. Dependence of
::J
0 the average ground-state
'-
Ol
59
13=0.5 energy per one electron on
the magnetic field for f3 =
0 2 3 4 0.5. Inset: chemical pot en-
magnetic field (T) tial [70]
138 9. Description of a Many-Electron Quantum Dot
8
GaAs, N=25
>-
Ol (3=0.3
~
E
>-
~ 6
Ol
C
Ol
C
o
~c 4
o
.;::
co
§ 2 Fig. 9.5. Dependence of the
CIl FIR absorption spectrum of
~
a quantum dot containing
25 electrons on the magnetic
O-r---.---r--.---.---~--.---.---~ field; squares - the experi-
a 2 3 4
ment [34); lines - the model
magnetic field (T) [70]
Figs. 9.2-4, which were calculated for different values of {3, shows that the
inclusion of the spin--orbit interaction allows for a visible improvement of the
model curves toward the experimental data (the agreement is particularly
good for (3 = 0.3).
Let us now proceed to the selection rules for the FIR optical transitions
in a magnetic field. Since the magnetic field does not affect the form of
the Hartree-Fock wave functions, the selection rules are the same as in the
absence of the field (9.40). Hence, the resonance energies have the form
We shall assume that the sign "-" (attraction) refers to an electron and
the sign "+" (repulsion) to a hole. It can certainly be reversed, but with no
effect on the following considerations. The model potential (10.1) is smooth
and has a finite depth (Vo) and a characteristic finite radius L. Denoting the
positions T, momenta p, projections of angular momenta onto direction of the
field I = -i(x8y - y8x ), effective masses m*, and the cyclotron frequencies
We = eB / (em *) of the pair of particles with indices e (electron) and h (hole),
the Hamiltonian of the system can be written in the form
p; 1
H 2m; + v,,(re) + '2tiweele
p~ 1 e2
+-2
* + Vh(rh)
mh
- -2tiwchlh - I
E Te - Th
I + Eg , (10.2)
where Eg is the band gap of the semiconductor in which the dot is created.
v" and Vh are the bare single-particle potentials of an electron and a hole in
a magnetic field (the sign "-" refers to the electron and "+" to the hole):
i = e,h. (10.3)
The last term in the above expression describes the confining potential due
to the magnetic field. It should be observed that independently of the charge
of a carrier, the magnetic field enhances its binding in the dot.
The eigenfunctions of the Hamiltonian (10.2) are postulated in the Hartree
form
(10.4)
In such an approximation the equation for the eigenstates of (10.2) is equiv-
alent to the following system of equations (sign "-" refers to the electron,
and "+" to the hole):
p; + Ui(ri) ± 1)
( 2m* '2 tiwci 1i (MTi) = Ei(/Ji(Ti) , i = e, h, (10.5)
•
where the self-consistent effective field that acts on the electron Ue is given
by the formula
Ue(re) = v,,(re) - -
e2
E
J
dTh
I(Ph(Th)1 2
ITe - Th
I' (10.6)
10.1 Exciton in the Absence of a Magnetic Field 143
and the self-consistent effective field that acts on the hole Uh is obtained by
changing of indices in the above formula: e into h and vice versa. The total
energy of the pair E is given by
AOe =
~
---,
m~WOe
nwOe
K= Vo . (10.11)
The ground-state energy and wave function of the electron in the zeroth-order
approximation can be written in the form
E~O) nwoe(1- K- I ) (10.12)
8
o'"
>E
..r::.
~
r lADe
p~
( 2m* + u.(0)) ¢(O)(r) = E(O)¢(O\r) (10.15)
h h h h '
h
where
U~O)(r) = Vh(r) - 2
v;e exp [-
f Oe
2~ Oe
] [2:: ],
10
Oe
(10.16)
and 10 is the Bessel function. The characteristic profile of the effective self-
consistent potential of the hole is presented in Fig. 10.1. This potential has
two minima: at r = 0 and r = r3h (see Fig. 10.2). Their positions and the
extreme values of the potential depend on the value of the parameter K. With
an increase of K (i.e., with a decrease of dot diameter) the second minimum
moves toward the dot center, and both minimum values of the potential attain
equal values. As a result, for K ~ 0.8 we can observe only one minimum of the
potential. Thus, in the zeroth approximation for K < 0.8, the self-consistent
effective field that acts on the hole is a double potential well.
When the potential structure is of the double-well type, the usual pro-
cedure is to search for the states of a particle in both wells simultaneously,
and then a superposition of these states is made. Near the dot center the
potential curvature is described by the frequency Wlh:
10.1 Exciton in the Absence of a Magnetic Field 145
0.4
2h
0.2
we can obtain the ground-state energy and wave function of the hole in the
"left" well in the form
(10.20)
* 2 d2Uh
mh w3h = dr2
I (10.22)
r=r3h
Thus, the ground-state energy and wave function of the hole in this well are
obtained by solving the equation:
As a result we obtain
146 10. Description of an Exciton in a Quantum Dot
(10.25)
(10.26)
Ph = J
dr¢lh(r)¢3h(r) (10.31 )
is the overlap integral of the pair of functions in the two potential wells. The
following system of equations is obtained for the new coefficients:
U 0"32 ) U * w1h
m h 2 ( r3h 0"32 ) 2
h ( r3h 2 2 - 1h - * 2 - 2 2
0"1 + 0"3 2mewOe AOe 0"1 + 0"3
U ( 0"32 ) U * w3h
m h 2 ( r3h 0"32 ) 2
(10.34)
h r3h 2 2 - 3h - * 2 - 2 2
0"1 + 0"3 2mewOe AOe 0"1 + 0"3
The condition for the existence of nonzero solutions of the system of equations
(10.32) is the vanishing of its determinant,
(10.35)
In further considerations we can use the relation ELh > E Rh . This assumption
is justified by the fact that the left well Uh (r) of the potential is always more
shallow than the right one [71]. Therefore, the solutions of (10.35) have the
form
Eh1 = ELh + Ih, Eh2 = ERh -Ih, (10.36)
where
4 (a) 4 (b)
-
~3 ~3
.r:::.
~2 W
2
<:I
1 1
0 0
0 0.4 0.8 0 0.4 0.8
K K
Fig. 10.3. Dependence of (a) energies Ehl and Eh2, (b) difference between them
L1E, on parameter '"
1 1 + BLhPf,
VI - Pf, VI + 2BRh pf, + B~hPf, ,
!'h(1 - Pf,)
(10.43)
Pf,bRh
An important property of the pair of states (10.39) and (10.42) is that they are
of the same axial symmetry. The investigation of the dependence of energies
Ehl and Eh2 on the size of the quantum dot, shown in Fig. 10.3, turns out
to be very important. It appears that in the whole range of the parameter
'" energy Ehl is positive, while energy Eh2 is negative. This means that in
the state described by the wave function ¢hl the hole is not localized in the
quantum dot. On the other hand, from the analysis of coefficients C12 and C32
it follows that for any value of Ii the relation IC121 < IC321 is fulfilled. Hence,
in the state ¢h2 the hole resides near the second minimum of the potential
U~O) .
Let us now calculate the next correction to the electron state. Taking
into account the interaction of the electron with the hole, the effective self-
consistent potential that acts on the electron can be written as
Ur (i)( )
e
= -Vr
0 exp
[_~]
L2
_ e2
E
Jd r I l¢hi(r')jZ
Ir _ r'l ' (10.44)
where index i = I, 2 refers to the two states of the hole (in a zero magnetic
field only the case of the bound state of the hole is significant, i.e., i = 2).
The explicit form of the above equation is the following:
[K,r
2 e 2 y'7f
11;.;.;0 { - -I exp - - - ] - --:--:---
e K, 2A5e EAoe11;.;.;oe
10.1 Exciton in the Absence of a Magnetic Field 149
J
+ 2Cil Ci3Ph err ; cr§ exp [- cr~~6~§ (r - r3h err ~cr§ ) 2]
xIo [cr~~6~§ (r - r3h err ~ cr§ r]) }. (10.45)
The potential U~2) for i = 2 will be denoted simply by Ue . The profile of this
potential, in dependence on the dot size, is shown in Fig. 10.4. As can be
seen, the double-well structure in the variable r is more distinct here than
in the case of the hole. The existence of the first minimum (in the center of
the dot) is due to the minimum in the confining potential V. The existence
of the second minimum is due to the attractive potential of the hole. The
relative depths of the pair of minima of potential Ue depend on the dot size,
parametrized by /'£. Both situations are possible: the two minima can have
comparable depths, or one minimum can be clearly deeper than the other.
The first case is illustrated in Fig. 10.5, where we present a characteristic
profile of the potential Ue for /'£ = 0.5.
The analysis of the electron motion in the obtained potential is carried
out in an analogous way as for the hole. In the vicinity of the minima rle = 0
and r3e, the double-well structure of the potential Ue is approximated by a
pair of parabolas,
(10.46)
(10.47)
150 10. Description of an Exciton in a Quantum Dot
r/AOe
o -r----r----r----r----r---,----,---~--~
3e
Fig. 10.5. Electron effective self-consistent potential for Ii. = 0.5 (nwo e = 7.5meV)
two minima (Ie) and (3e) are separated by a maximum (2e)
The frequencies that determine the curvatures of the parabolas are given by
the equations
(10.48)
For each of the approximated potentials we can now solve the equation for
the ground-state energy and wave function
(10.49)
where 8r = Wle/WOe and Ale = 81/ ,fifAOe. For the potential (10.47) we obtain
(10.52)
(10.53)
where 8§ = W3e/WOe. The function Ie in the above expression plays the same
role as the function Ih for the hole. It ensures a smooth connection between
~le and ~3e. Its analytical form is given in [71]. This leads to the following
form of coefficient A3e:
83e exp
.,fiKAoe
[Ie (s:UAOe
T3e)]
3-
(10.54)
10.1 Exciton in the Absence of a Magnetic Field 151
The function P in the above stands for the usual error integral:
p(x) =
2
,;:rr r e-
io Y
2
dy. (10.55)
o (a) (b)
Q)
~-1
8 ~-
.r:= .r:=
-r.,-2 LiJ·2
W -<:l
-3
4+---.----.---.---.
o 0.4 0.8 o 0.4 0.8
K K.
Fig. 10.6. Dependence of (a) energies Eel and E e2 ) (b) difference between them
L1E) on parameter K,
the electron that occupies its ground state described by (10.58) is localized
closer to the dot center, and the electron in the excited state (10.61) resides
closer to the second minimum of the potential Ue . These states have the same
axial symmetry, which results from the fact that with respect to the radius
the potential Ue has the double-well structure.
When we know the electron and hole states it is possible to construct
the states of an electron-hole pair that is confined in a quantum dot. They
assume the form
Pi(rh, re) = ¢h2(rh)¢ei(r e ), i = 1,2. (10.63)
These states correspond to the energies
X [ (r3h
I O 1
-- 22 ) ()~ 2] } . (10.65)
2 AOe (}l (}3 +
Due to the fact that the hole in the state with energy Eh2 is localized near
the dot and the localized electron can assume a pair of energies Eel and E e2 )
the energies of the ground and excited states of the exciton have the form
10.1 Exciton in the Absence of a Magnetic Field 153
The fundamental property of the pair of exciton states, the ground and first
excited state, is that they have identical axial symmetry, which leads to the
vanishing of the dipole matrix element between them:
This is because in both states both the electron and the hole have zero orbital
angular momentum. This means that the radiative dipole transition between
this pair of states (by means of absorption or emission of an FIR photon)
is forbidden. The blocking of this transition should have a striking effect
on the photoluminescence spectrum of a quantum dot. At low temperatures
and in small dots the relaxation of a bound exciton through the interaction
with phonons is considerably weakened (see Sect. 6.2). Hence, the additional
blocking of the relaxation through the emission of an FIR photon leads to the
occurrence of a metastable excited state in the exciton spectrum. It has to
manifest itself by the splitting of the photoluminescence peak for a quantum
dot. A strong additional peak, which appears in the photoluminescence spec-
trum, corresponds to the radiative recombination from the metastable state.
As illustrated in Fig. 10.6, the difference of energies f1E12 (i.e., the distance
between the ground peak and the additional peak in the photoluminescence
spectrum) is strongly dependent on the parameter /'i, and reaches its mini-
mum at /'i, ~ 0.7, when the two minima of the potential Ue have a similar
depth. An increase or decrease of the parameter /'i, (i.e., the introduction of a
difference between the depths of the two potential minima Ue ) leads to the
increase of f1E12 (see Fig. 10.7 and the above table).
154 10. Description of an Exciton in a Quantum Dot
E, I:::=,L-..;'------
(a)
E,I-----,----!---
Etf-::;,.~=>-,,=,,'-=--
(b)
T;~ ~
TI
:¢e2
¢el t3h~ :: =
T3h
{ 2.413 if /'i, = 0.68, (10.71)
10.625 if /'i, = 0.8.
Hence, an increase in the intensity of the second peak is accompanied by a
decrease in its broadening. A more rigorous analysis, using the electron-hole
10.1 Exciton in the Absence of a Magnetic Field 155
V
0.15 e
"';" ....
N
::::::: 0.10 .,t4
-: ";"pN
0.05 2
0.00 0
0 0.4 0.8 0 0.4 0.8
K K
Fig. 10.S. Dependence of (a) ratio of recombination intensities for the recombina-
tion from the ground and metastable states of an exciton, at a temperature of 5 K
and nwOe = 7.5 meV, and (b) ratio of widths of corresponding photoluminescence
peaks, on parameter K
;: 1.76
Q)
...., 1.75 10 ~
> E
(!) 1.74
Q::!
w 5(!)
z 1.73 Z
w
l=
~ 1.72 O~
(!) en
o 1.71 ::.::
Z -0(
Fig. 10.9. Splitting of
:i 1.70
w
a..
the photoluminescence
1.69 peaks and the main-
0 200 400 600 800 1000 peak energy as a func-
DOT SIZE w (nm) tion of the dot size [20]
. . Dot Barrier
S . ..... ,. .
Interdlffused Riljeg.,on
..
Interdiffusion
"§ 1000A Sh N4 ." " " " I
.e..!!.
10M GaAs
2~g~ ~-:s
200 A AIGaAs
.
>-
1-
(x=0.35) Quantum Dot VB
t..
E ~
~ ~B
W w=
I-
~
W
U 400nm
Z
W
U
CI)
W
z
:E
~
...J 450nm
~
o Fig. 10.10. Photoluminescence spec-
J:
D..
500nm tra of quantum dots with different di-
ameters; the strongest splitting is ob-
1690 1700 1710 1720 1730 served for a dot with diameter 450 nm
ENERGY (meV) [11]
~
I::
::J
.ci
p Exc .==
~
~
iii
z
W
I-
~
W
U
Z 1. 25 1lW
W
U
If)
w
z
:iE
~ 125nW
...J
~
J: 125nW
D.. Fig. 10.11. Photoluminescence spec-
tra of a quantum dot with diameter
1.68 1.70 1.72 1.7.<1 1.76 450 nm for various excitation powers
ENERGY (eV) [20]
10.2 Exciton in a Magnetic Field 157
9 8 7
+ + +
PLE
InGaAs OD's
~
Lz confinement only: 5ML
visible, independently of the laser excitation power (see Fig. 10.11). The fact
that the splitting remained unchanged even at small excitation powers proves
the occurrence of the metastable exciton states in a dot. Moreover, it is the
experimental confirmation of the result obtained in a theoretical way. A sim-
ilar structure of the photoluminescence spectrum of self-assembled dots was
by observed Fafard et al. [39] (see Fig. 10.12).
(J= (10.72)
and the dimensionless parameter that determines the dot size (and hence the
number of bound electron states)
r;, -+ r;,(B) = (Jr;,. (10.75)
The electron energy and wave function in the zeroth-order approximation
can be calculated by solving the equation
p~ - Vr0
[ 2m~ + ~m*w2r2
2 e e
~(O)(r e ) = E(O)~(O)(r
+ mv2cel ] '+'e Z e '+'e e
). (10.76)
As a result, we obtain
E~O) mve((J - r;,-l), (10.77)
(10.79)
where Io is the Bessel function. Due to the occurrence of the Landau term
~mhw~r2 (see (10.3)), the profile of potential Uh strongly depends on the
magnetic field. Figure 10.13 presents a sample curve that is determined for
r;, = 0.5, mvOe = 7.5 meV, and B = 2 T.
As described previously for the zero field, at weak magnetic fields the
potential Uh has two minima: one for r3h and the other in the center of the
dot. For the intermediate values of the magnetic field (2-4 T) both minima
have similar depths. At a strong field, however, the Landau term dominates,
and the potential Uh has only a single minimum, in the center' of the dot.
Since at weak and medium fields we are dealing with a double-well potential,
the search for the energy and wave functions of the hole in the zeroth-order
approximation is identical to the case of a zero field. It shows, however, (see
Fig. 10.14) that both energies Ehl and Eh2 are positive. But due to the fact
10.2 Exciton in a Magnetic Field 159
1.0
______ ~:L _______ _
0.5
-
CD 1.5 CD 1.5
8
.c. 1.0
8
.c. 1.0
;:a= W
~
0.5 <1 0.5
0.0 0.0
0 0.4 0.8 0 0.4 0.8
K K
Fig. 10.14. Dependence of (a) energies Ehl and Eh2, (b) difference between them
,dE, on parameter K,; magnetic field B = 2 T
that in a magnetic field Uh - t 00 for r - t 00, the hole can be localized near
the dot also for Eh > O. In addition, the analysis of the coefficients c shows
that the hole with energy Ehl resides closer to the dot center and the hole
with energy Eh2 closer to the second minimum of the potential.
The increase of a magnetic field drives the hole spectrum through the
three distinct regimes. In weak fields (B =0-4 T) it is possible to bind the
hole in the second minimum of the potential and in the dot center. However,
the probability that the second case will occur is limited (the energy Ehl is
much higher than Eh2; see Fig. 10.14). For intermediate values of the field
(B =4-6 T) a pair of states with similar energies occur in the spectrum that
correspond to the hole localized in the center of the dot and in the second
minimum of the potential. This pair of states have the same zero orbital
angular momentum (s-type states). Finally, at strong fields (B >6 T) the
hole is bound in the dot center. It should be stressed that the transitions
between consecutive stages are continuous and consist in the transformation
of one potential minimum into two potential minima, or in the meeting of
the two minima in the dot center.
If the hole is localized in only one potential minimum Uh , then the first-
order approximation of the electron state is identical, as in the case of a zero
field. This is out of the question as far as the weak fields are concerned. For
intermediate fields, however, we are dealing with two bound hole states and
160 10. Description of an Exciton in a Quantum Dot
r/AOe
2~----~--~----~--~--~----~--~--~
2 4 6 8
-6
Fig. 10.15. Electron effective self-consistent potentials U~l) and U~2), for magnetic
field B = 2 T and K. = 0.4 (nwo e = 7.5 meV)
1.25
8 -2
r
CI) CI)
~
8 1.00
~
~-4 W
-<3 0.75
-6 0.50
0 0.4 0.8 0 0.4 0.8
K K
Fig. 10.16. Dependence of (a) energies E~~) and E~i), (b) difference between them
iJ.E, on parameter K.; magnetic field B = 2 T
thus with two effective self-consistent electron potentials - in (10.45) the index
i can assume the values 1 or 2. The profiles of electron potentials U~l) and
U~2) for K. = 0.4 and B = 2 T are presented in Fig. 10.15. A rigorous analysis
of the model shows that for intermediate fields the potential U~l) has always
only one minimum - in the dot center. Similar behavior is observed for the
potential U~2), but for some values of the magnetic field and of parameter K.
(e.g., B = 4 T and K. = 0.4, or B = 6 T and K. = 0.33), the second minimum
appears at T = T3e and disappears with a decrease or increase of K.. The
transition of the potential UP) from a single well into a double well and vice
versa is continuous.
Let us first consider the case, where each of the potentials (hole and
electron) has a single minimum - in the dot center. The electron state <p~i)
corresponds to the hole state <PhI, and the electron state <p~;) corresponds
10.2 Exciton in a Magnetic Field 161
0 (a) 4 (b)
;;
e(2)
~
•2
8-
.3
..c:
8
..c:2
i:Lr-4 e1 W
-<l
-6 0
0 0.4 0.8 0 0.4 0.8
1C K
Fig. 10.17. Dependence of (a) energies E~~) and E~;), (b) difference between them
dE, on parameter K; magnetic field B = 4 T
to the hole state ¢h2. The energies of these states (see Fig. 10.16) and the
explicit forms of corresponding wave functions can be calculated through the
procedure described in Sect. 10.1, but the calculation is even easier here due
to a simpler structure of the potential. When the potential U~2) has two
minima, two electron states ¢~i) and ¢i;) correspond to the hole state ¢h2.
The energies that correspond to these states are presented in Fig. 10.17. In
that case we have to deal with three electron states (see Figs. 10.18 and
10.19). When the magnetic field becomes too strong (B ~ 6 T), the double-
well structure is washed out, and there are no excited states with the same
axial symmetry as the ground state.
162 10. Description of an Exciton in a Quantum Dot
.... 1
B=8T
no corresponding
.... 1 hole state (h2) for
O.2<K<O.7
c c·
1(
c c ·
(e) (d) ""Y
a dot with diameter 35 nm in a zero magnetic field they report the existence
of two photoluminescence peaks, and also the appearance of the third one at
B ~ 4 T, and finally its disappearance when the. field was increased to 8 T.
Similar, but more complex photoluminescence spectra were also observed
by Raymond et al. [115] (see Fig. 6.17). However, their experiment was carried
out on highly excited dots, where a larger number of excitons (even up to 20)
were bound in a dot. The characteristic property of highly excited dots is the
the existence of three peaks in the absence of a magnetic field, which further
split in the magnetic field. In order to explain it within the presented above
model it is crucial to consider the problem of three particles in a dot: two
electrons and one hole (or two holes and one electron). As follows from the
detailed analysis [72], in these cases four states with zero angular momentum
of the recombining particles occur in the energy spectrum of the system. They
correspond to the two states of each electron (singlet and triplet states of the
electron pair). For GaAs, in the absence of a magnetic field two of these four
states are almost degenerate, and hence the three peaks are observed. The
inclusion of a magnetic field removes the degeneracy and unravels the fourth
transition.
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