DOTTORATO DI RICERCA IN FISICA - XII CICLO

Sede Amministrativa
Universita degli Studi di MODENA e REGGIO EMILIA

TESI PER IL CONSEGUIMENTO DEL TITOLO DI DOTTORE DI RICERCA

Electronic States in Semiconductor Quantum Dots

CANDIDATO Massimo Rontani

SUPERVISORI Prof. Franca Manghi

Prof. Elisa Molinari

Ottobre 1999
a Philip Marlowe, Ciccio Ingravallo,
Santamaria e tutti gli altri
Contents

Introduction 1

1 Quantum Dots: a Survey 5

1.1 Energy and Charge Quantization . . . . . . . . . . . . . . . . . . 5
1.1.1 Charge quantization . . . . . . . . . . . . . . . . . . . . 5
1.1.2 Coulomb Oscillations and Coulomb Staircase . . . . . . . 7
1.1.3 Energy Quantization . . . . . . . . . . . . . . . . . . . . 9
1.2 Construction and Measurement . . . . . . . . . . . . . . . . . . . 10
1.2.1 Single-Electron Capacitance Spectroscopy . . . . . . . . 10
1.2.2 Single-Electron Tunneling Spectroscopy . . . . . . . . . . 12
1.3 Single-Electron Transport . . . . . . . . . . . . . . . . . . . . . . 18
1.3.1 “Classical” Theory of Coulomb Blockade . . . . . . . . . 19
1.4 Survey of the Theoretical Work . . . . . . . . . . . . . . . . . . . 23
1.4.1 Single Quantum Dot . . . . . . . . . . . . . . . . . . . . 23
1.4.2 Coupled Quantum Dots . . . . . . . . . . . . . . . . . . 27

2 Theory I: Single-Particle States 29

2.1 Model . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 29
2.1.1 The Envelope Function Approximation . . . . . . . . . . 29
2.1.2 Hamiltonian . . . . . . . . . . . . . . . . . . . . . . . . 31
2.1.3 Cylindrical Symmetry and Magnetic Field . . . . . . . . . 33
2.1.4 Dot Confining Potential . . . . . . . . . . . . . . . . . . 35
2.2 Single-Particle States . . . . . . . . . . . . . . . . . . . . . . . . 39
2.2.1 General Considerations . . . . . . . . . . . . . . . . . . . 39
2.2.2 Fock-Darwin States . . . . . . . . . . . . . . . . . . . . . 43
ii Contents

2.3 The Hartree-Fock Method . . . . . . . . . . . . . . . . . . . . . 53

2.3.1 The Variational Principle . . . . . . . . . . . . . . . . . . 55
2.3.2 Roothaan’s Equations . . . . . . . . . . . . . . . . . . . 61
2.3.3 Discussion . . . . . . . . . . . . . . . . . . . . . . . . . 62

3 Theory II: Many-Electron States 65

3.1 Generalized Hubbard Hamiltonian . . . . . . . . . . . . . . . . . 65
3.1.1 The Choice of the Basis . . . . . . . . . . . . . . . . . . 67
3.1.2 Single and Coupled Vertical Quantum Dots . . . . . . . . 68
3.1.3 Diagonalization and Addition Spectra . . . . . . . . . . . 71
3.2 Symmetries and Wigner-von Neumann Theorem . . . . . . . . . 73

4 Addition Spectra in Single Vertical Quantum Dots 75

5 The Importance of Electronic Correlation 81

6 The Double-Dot Molecule 95

Conclusions 109

A Second Quantization 111

B Coulomb Matrix Elements 115

C Wigner-von Neumann Theorem 121

Acknowledgements 125

Bibliography 127
Introduction 1

The experimental and theoretical study of electronic systems was limited for a
long time to naturally occurrying atoms, molecules and crystals. Ideal crystals
are three-dimensional systems, while an effective reduction of geometry to
lower dimensions — by a strong spatial localization, namely confinement of
an electron in at least one direction at the de Broglie wavelength — occurs
only in the case of crystal imperfections.
The beginning of the 70s marked the new era of research on electronic struc-
tures of lower dimensions. The first to appear were quantum wells[1, 2]. A
quantum well is a thin, flat layer of semiconductor sandwiched between two
layers of another semiconductor with larger bandgap. Owing to this bandgap
difference, the conduction and valence band edges of the two materials do not
align with each other (band off-set). The band off-set produces the potential
responsible for confining the carriers in the thin layer. In a semiconductor the
de Broglie wavelength is relatively large, hence the motion of electrons bound
in a layer as thin as several crystalline monolayers is quasi-two-dimensional,
and the excitations in the perpendicular (growth) direction are strongly quan-
tized. A material that is commonly used for creating quantum wells is GaAs,
which in combination with a ternary solution Alx Ga1;x As serving as a bar-
rier allows for the creation of epitaxial layers with high crystalline quality as a
result of the almost equal lattice constants.
The new, unusual properties of quasi-two-dimensional systems, which promised
applications in electronics and opto-electronics, attracted the attention of many
research laboratories. This in turn resulted in a rapid development of produc-
tion technology and extensive research, which culminated in the discovery of
the Quantum Hall Effect[3] in 1979. At present, many 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,
such as laser diodes used in CD players or microwave receivers used in satel-
lite television.
Since the beginning of the 80s, the rapid progress in technology, including
very accurate lithographic techniques, possibly combined with self-organized
growth techniques, made it possible to confine electrons in quantum wires,
i.e. quasi-one-dimensional structures. Quantum wires are produced, for exam-
ple, in the form of miniature strips, etched in a sample containing a quantum
well, or in V- and T-shapes obtained by controlled overgrowth processes[4].
Complete quantization of the electron’s free motion is implemented by trap-
ping it in a quasi-zero-dimensional quantum dot (QD). For example, Reed et
al.[5] at Texas Inst. reported the creation of a square QD with a side length of
250 nm, etched by lithography. Subsequent publications reporting the creation
of QDs in other laboratories soon appeared[6, 7, 8], with diameters already re-
duced to 30-45 nm.
The name “dot” suggests an exceedingly small region of space. A semicon-
ductor QD, however, is made out of roughly a million atoms with all their
electrons. Virtually all electrons are tightly bound to the nuclei of the mate-
rial, however, and the number of free electrons in the dot can be very small;
between one and a few hundreds. The de Broglie wavelength of these elec-
trons is comparable to the size of the dot, and the electrons occupy discrete
quantum levels (akin to atomic orbitals in atoms) and have a discrete excita-
tion spectrum. If the number of free electrons Ne is large, it is reasonable to
expect that their electronic properties may be qualitatively described by ap-
pealing to known properties of the infinite (Ne ! 1) electron gas. However
for small numbers of electrons (e.g. Ne < 20) the electronic properties of the
2 Introduction

system are likely to be strongly Ne -dependent, particularly if the dot is small.

A characteristic quantity for QDs is the addition energy, which is analogous to
the ionization energy of an atom. This is the energy required to add or remove
a single electron from the dot. It is a finite, measurable quantity that depends
on Ne and arises from quantization of charge in units of e.
Because of the analogies to real atoms, QDs are frequently referred to as arti-
ficial atoms[9]. As in real atoms, electrons are attracted to a central location.
In a natural atom, this central location is a positively charged nucleus; in an ar-
tificial atom, electrons are typically trapped in a bowl-like parabolic potential
well in which they tend to fall in towards the bottom of the bowl. Moreover,
QDs can be coupled one to each other, if the heterostructure barriers are suffi-
ciently thin, thus one can extend the analogy with “natural” systems speaking
of artificial molecules.
The basic technological motivation to study QDs is that smaller components
should be faster and may also dissipate less heat. There is also the added fea-
ture that quantum-mechanical effects are so important in such systems that
devices with fundamentally new properties could be obtained. In this per-
spective a relevant example are single electron transistor devices. Otherwise,
since QDs absorb and emit light in a very narrow spectral range, they might
find application in the construction of more efficient and more controllable
semiconductor lasers. The strong quantization of electron energy, with pa-
rameters suitable for laser action, particularly in the so-called self-assembled
QDs, will probably allow QD-based lasers to work at higher temperatures and
at lower injection currents[10]. The small dimensions and the possibility of
dense packing of QD-matrices could also permit them to be used for computer
memory media of huge capacity. In addition, an intriguing challenge that is
now being explored is the possibility to use QDs for implementing quantum
information devices[11].
Apart from their potential use as novel devices, QDs are interesting from a fun-
damental point of view. First of all it is possible to control their shape, their
dimensions, the structure of energy levels, and the number of confined elec-
trons Ne . Applying external fields generated by standard laboratory sources
transitions never observed in the spectra of “natural” atoms can be readily seen
in artificial ones. Second, the energy spectrum of the few-electron QD is ex-
pected to be extremely rich since the single-electron confinement energy, the
cyclotron energy for modest fields and the electron-electron interaction en-
ergy can all be of similar magnitude (typically a few meV), and they scale
differently as far as one varies dot parameters. The energy spectrum is also
likely to be strongly Ne -dependent. Of particular interest is the investigation of
small-Ne precursors of exotic many-body states such as fractional-quantum-
Hall-effect states[12] and Wigner solids[13]. To summarize, QDs are an ideal
laboratory to investigate electronic correlation, and this is the issue the present
Thesis is mainly addressed to.
Current experiments concerned with QDs focus mainly on studying their op-
tical properties (absorption and emission of light in the visible or far infrared
range, and the Raman scattering of light) and electric properties (capacitance
and transport studies). QDs are therefore artificial atoms with the additional
intriguing possibility of connecting source and drain contacts to probe their
atomic states.
In this Thesis we investigate the electronic structure of few-electron QDs. In
such systems the strongly correlated electronic states show a rich phenomenol-
ogy and require a many-body approach. We study the dependence of elec-
tronic configurations on the variation of external tunable parameters such as
Introduction 3

an applied homogeneous magnetic field, the geometry of the dot, the coupling
to another QD, and the number of electrons. Approximate theoretical schemes
are also discussed and compared, and the role of electronic correlation is ana-
lyzed.
We focus on the so-called vertical QDs[14, 15], single and coupled. These
structures, to be described later, have abrupt and thin tunnel barriers, present
a relatively low rate of disorder (impurities, electrode potential fluctuations,
etc), and are sufficiently well defined to allow for the formation of systemati-
cally degenerate sets of electronic energy levels. We will see that the presence
of degeneracies (or, equivalently, of symmetries) has important consequences
including: (i) The appearance of an electronic shell structure reminiscent of
periodic table of elements of atomic physics. (ii) Ground state configurations
with non-zero values of magnetization and spin.
As mentioned above, transport measurements (Single-Electron-Tunneling- and
Capacitance-Spetroscopies) are a direct spectroscopic tool to probe ground
state energies of few-particle, strongly correlated artificial atoms and molecules.
The relevant quantity measured, that is the addition energy, will be easily ex-
tracted from our calculations and then compared with experimental findings.
The structure of the present Thesis is the following:

 In Chapter 1 we briefly review construction and measurement methods

of QDs. After recalling the simplest phenomenological models for elec-
tron transport through dots (Coulomb blockade), basic single electron
experiments are presented. The Chapter is a primer about the concept of
addition spectrum which is essential throughout this work. It ends with
a survey of existent theoretical work.
 In Chapters 2 and 3 we illustrate the theoretical framework for the com-
putation of many-body electronic states. After an analysis of the model
system, Chap. 2 is concerned with single-particle states, including mean-
field solutions of the many-body problem. The Self-Consistent methods
are presented and discussed. In Chap. 3 we introduce a many-body ap-
proximate Hamiltonian to correctly treat the electronic correlation. The
Wigner-von Neumann theorem which rules over transitions between dif-
ferent electronic configurations is reviewed.
 Chap. 4 displays our results on the addition spectra of single QDs. The
main points are the evidence of an electronic shell structure and spon-
taneous magnetization and spin-polarization brought about by electro-
static and exchange effects (Hund’s rules). Data agree with measure-
ments in presence of an external magnetic field.
 Chap. 5 is a critique of the results of the previous Chapter. The influence
of dot geometry on the addition energy is analyzed, different theoretical
approaches such as many-body Hamiltonian, Hartree-Fock method and
exact diagonalization technique are compared, and the importance of
electronic correlation in the approximations introduced is discussed.
 Chap. 6 analyzes the energy spectrum of an artificial molecule. Here
we vary also the coupling between dots: unexpected configurations are
found in intermediate regimes, in addition to those pertaining to the two
limiting cases of two well separated QDs or a unique, strongly connected
system, respectively.
 Final conclusions stress the main findings of this Thesis.
4 Introduction

The main reviews on the subject are Refs. [16, 17, 18, 19, 20]. Ref. [21] is an
introduction to single charge tunneling.
Chapter 1

Quantum Dots: a Survey

QDs are the object of our investigation, atom-like systems whose electronic
properties are probed by single-electron transport spectroscopies. This Chap-
ter has two main objectives: first, it aims at reviewing basic experimen-
tal facts and at elucidating the concept of Coulomb blockade and single-
electron spectroscopy. Second, it surveys exsistent electronic structure stud-
ies. We start reminding the conditions to observe energy and charge quan-
tization, whose experimental evidences are the so-called Coulomb oscilla-
tions (Section 1.1). After, we describe some state-of-the-art QD devices
together with the main transport measurement techniques (Sec. 1.2). A sim-
ple theory of electron transport through dots is outlined in Sec. 1.3. Section
1.4 is a survey of theoretical works on QD electronic properties.

1.1 Energy and Charge Quantization

In this Section we examine the circumstances under which Coulomb charging and
energy quantization effects are important.

1.1.1 Charge quantization

Let us consider the electronic properties of the small conductor depicted in Fig. 1.1
(a), which is coupled to three terminals. Particle exchange can occurr with only
two of the terminals, as indicated by the arrows. These source and drain terminals
connect the small conductor to macroscopic current and voltage meters. The third
terminal provides an electrostatic or capacitive coupling and can be used as a gate
6 Quantum Dots: a Survey

Figure 1.1: Schematic of a quantum dot, in the shape of a disk, connected to

source and drain contacts by tunnel junctions and to a gate by a capacitor. (a)
shows the lateral geometry and (b) the vertical geometry.

electrode. If we first assume that there is no coupling to the source and drain
contacts, then the small conductor acts as an island for electrons. The number of
electrons on this island is an integer Ne , i.e. the charge on the island is quantized
and equal to Ne e. If we now allow tunneling to the source and drain electrodes,
then the number of electrons Ne adjusts itself until the energy of the whole circuit
is minimized.
When tunneling occurs, the charge on the island suddendly changes by the
quantized amount e. The associated change in the Coulomb energy is conveniently
expressed in terms of the capacitance C of the island. An extra charge e changes
the electrostatic potential by the additon energy e2 =C . This addition energy be-
comes important when it exceeds the thermal energy KB T . A second requirement
is that the barriers are sufficiently opaque such that the electrons are located either
in the source, in the drain, or on the island. This means that quantum fluctuations
in the number Ne due to tunneling through the barriers is much less than one over
the time scale of the measurement (this time scale is roughly e divided by the cur-
1.1 Energy and Charge Quantization 7

rent). This requirement becomes a lower bound for the tunnel resistances Rt of
the barriers. To see this, consider the typical time to charge or discharge the island

t = Rt C . The Heisenberg uncertainty relation:
E
t = (e2 =C )Rt C  h
implies that Rt should be much larger than the resistance quantum h=e2 = 25.813
k in order for the energy uncertainty to be much smaller than the addition en-
ergy. To summarize, the two conditions for observing effects due to the discrete
nature of charge are[19]:

Rt  h=e2 ; (1.1)
e2 =C  KB T: (1.2)

The first criterion can be met by weakly coupling the dot to the source and drain
leads. The second criterion can be met by making the QD small (the capacitance
of an object scales roughly with its radius R).

1.1.2 Coulomb Oscillations and Coulomb Staircase

While the tunneling of a single charge changes the electrostatic energy of the
island by a discrete value, a voltage Vg applied to the gate (with capacitance Cg )
can change the island’s electrostatic energy in a continuous manner. In terms of
charge, tunneling changes the island’s charge by an integer while the gate voltage
induces an effective continuous charge q = Cg Vg that represents, in some sense,
the charge that the dot would like to have. This charge is continuous even on
the scale of the elementary charge e. If we sweep Vg the build up of the induced
charge will be compensated in periodic intervals by tunneling of discrete charges
onto the dot. This competition between continuously induced charge and discrete
compensation leads to so-called Coulomb Oscillations in a measurements of the
current as a function of gate voltage at a fixed source-drain voltage. This is the
essence of the Single Electron Tunneling Spectroscopy (SETS).
An example of a SETS measurement[22] is shown in Fig. 1.2 (a). In the valley
of the oscillations, the number of electrons in the dot is fixed and necessarily equal
to an integer Ne . In the next valley to the right the number of electrons is increased
to Ne + 1. At the crossover between the two stable configurations Ne and Ne + 1,
a “charge degeneracy”[23] exists where the number can alternate between Ne and
8 Quantum Dots: a Survey

Figure 1.2: (a) An example of a measurement of Coulomb oscillations to illustrate

the effect of single electron charges on the macroscopic conductance. The con-
ductance is the ratio I=Vsd and the period in gate voltage Vg is about e=Cg [22]. (b)
An example of a measurement of the Coulomb staircase in I ; Vsd characteristic.
The different curves have an offset for clarity (I = 0 occurs at Vsd = 0) and are
taken for five different gate voltages to illustrate periodicity in accordance with
the oscillations shown in (a)[24].
1.1 Energy and Charge Quantization 9

Ne + 1. This allowed fluctuation in the number (i.e. according to the sequence

Ne ! Ne + 1 ! Ne ! : : :) leads to a current flow and results in the observed
peaks.
An alternative measurement is performed by fixing the gate voltage, but vary-
ing the source-drain voltage Vsd (non-linear transport). As shown in Fig. 1.2
(b)[24] one observes in this case a non-linear current-voltage characteristic ex-
hibiting a Coulomb Staircase. A new current step occurs at a threshold voltage
( e2 =C ) at which an extra electron is energetically allowed to enter the island.
It is seen in Fig. 1.2 (b) that the threshold voltage is periodic in gate voltage, in
accordance with the Coulomb oscillations of Fig. 1.2 (a).

1.1.3 Energy Quantization

Electrons residing on the dot occupy quantized energy levels. To be able to resolve
these levels, the energy level spacing
E must be greater than the thermal noise:

E  KB T:
The level spacing at the Fermi energy for a box of size L depends on the dimen-
sionality. Including spin degeneracy, we have:

E = (Ne =4) ~2  2 =mL2 1D; (1.3)

= (1= ) ~2  2 =mL2 2D; (1.4)
;

= 1=3 2 Ne 1=3 ~2  2 =mL2 3D: (1.5)

The characteristic energy scale is thus ~2  2 =mL2 . The level spacing of a 100 nm
2D dot is  0.03 meV, which is large enough to be observable at dilution refrig-
erator temperatures of 100 mK = 0.009 meV. In addition, electrons in semi-
conductor heterostructures have a small effective mass which further increases the
level spacing. As a results, semiconductor QDs are true artificial atoms, with both
observable quantized charge states and quantized energy levels.Using 3D metals
to form a dot, one needs to make dots as small as 5 nm in order to observe
atom-like properties.
The fact that quantization of charge and energy can drastically influence trans-
port through a QD is demonstrated by the Coulomb oscillations in Fig. 1.2 (a) and
10 Quantum Dots: a Survey

the Coulomb staircase in Fig. 1.2 (b). One can obtain spectroscopic information
about the charge state and energy levels of the interacting QD electrons by ana-
lyzing the precise shape of the Coulomb oscillations and the Coulomb staircase.
In this way, single electron transport can be used as a spectroscopic tool.

1.2 Construction and Measurement

We focus here on results from two techniques[25, 26, 27, 28] which have partic-
ularly affected our understanding of QDs. These methods are unique in allowing
extraordinarily high-resolution spectroscopy of QDs. The energy resolution of
these spectroscopies is limited solely by the sample temperature.

1.2.1 Single-Electron Capacitance Spectroscopy

Fig. 1.3 (a) shows schematically the type of sample used in one of these experi-
ments. The QD is located between two capacitor plates. It is close enough to one
of the plates to allow single electrons to tunnel between the QD and the nearby
plate. The artificial atom is far enough from the other capacitor plate to prohibit
tunneling to this plate.
Fig. 1.3 (b) shows how the sample is actually realized. A crystal wafer is
grown layer by layer, starting from the bottom of the diagram. The first layer is
a silicon-doped GaAs layer. The silicon doping makes this layer metallic, and it
acts as the bottom capacitor plate of Fig. 1.3 (a). Then a thin (10-nm) AlGaAs
barrier layer is grown. This barrier is thin enough that electrons can leak through
it. Above that, there is a GaAs quantum well, and grown on the top of the well
is a thick (not leaky) AlGaAs barrier. On top of the crystal wafer, chromium
is deposited to form the top capacitor plate, which is referred to as the “gate”.
Additional sample processing on the sample surface is used to create a gate which
laterally confines electrons in the quantum well below, creating a QD.
Electric fields can be created by applying a voltage between the plates of the
capacitor. If the top plate (gate) is made positive compared to the bottom one,
electrons from the bottom plate will be attracted in the direction of the top plate,
towards the artificial atom. Single electrons can thus be coaxed to tunnel into the
1.2 Construction and Measurement 11

Figure 1.3: (a) Schematic diagram of a quantum dot located between two capaci-
tor plates. The artificial atom is actually two-dimensional; the bowl-like shape is
to represent the force tending to move electrons to the centre of the dot. (b) Di-
agram of the sample used in Single-Electron Capacitance Spectroscopy (SECS)
experiments in a crystal grown using molecular-beam epitaxy. The QD is the
black disk in the quantum well. (c) Capacitance of the sample containing the QD
as a function of the top plate (gate) voltage. The first peak on the left represents
the first electron entering the QD[18].
12 Quantum Dots: a Survey

dot or expelled from it through the application of voltages on the top plate. After
each electron is added to the dot, additional gate voltage is usually needed to coax
another electron onto the dot. There are therefore specific gate voltages at which
an electron is added to the dot, and it is this spectrum of voltages which is known
as addition spectrum.
The motion of the single electrons into or out of the dot can be detected using
a simple physical principle. When a single electron tunnels into the QD, it moves
closer to the top plate of the capacitor, and electrons in the top plate tend to be
pushed away from the plate; that is, some charge is induced on the top plate. In
these samples, the amount of charge induced is about half of an electron’s charge.
A specialized transistor enables detection of this charge and thereby allows mea-
surement of the gate voltages at which single electrons were added to the QD. A
small a.c. voltage of frequency around 100 kHz is added to the d.c. gate voltage.
When the gate voltage is adjusted to a voltage at which an electron can be added
to the dot, the a.c. voltage causes the electron to tunnel back and forth between the
dot and the bottom plate. At these gate voltages, charge appears synchronously
with the a.c. voltage. A synchronous detector then registers a signal only at these
voltages, yelding a peak in the response. The scheme measures the capacitance
signal due to a single electron and is known as Single-Electron Capacitance Spec-
troscopy (SECS).
Results from this method, taken on a sample cooled to 0.3K, are shown in
Fig. 1.3 (c). The first peak on the left of the graph corresponds to the first electron
in the QD. Subsequent peaks correspond to additional electrons added to the QD.
The peak structure is completely reproducible as one scans the gate voltage up and
down, and the widths of the peaks directly reflect the temperature of the sample.

1.2.2 Single-Electron Tunneling Spectroscopy

One structure commonly studied by means of SETS, which will be referred to as a
planar QD, is created by patterning several metal electrodes, or gates, on the sur-
face of a two-dimensional electron gas heterostructure, in a similar manner to the
construction of the SECS device we examined above. Fig. 1.4 depicts the struc-
ture of a representative planar QD. A negative voltage applied to a gate raises the
1.2 Construction and Measurement 13

Figure 1.4: Quantum dot on the intersection of electrodes; four internal electrodes
localize the electrons, and four external ones serve as contacts for the electron
tunneling to and from the dot[29].

electrostatic potential in its neighborhood and, typically around -0.5 V, depletes

the underlying two-dimensional electron gas in the vicinity of the gate. Conse-
quently, under suitable biasing conditions, a small region of electron gas remains
at the center of the structure, and is isolated from the remainder of the electron
gas.
We have already outlined the SETS experiment in Subsection 1.1.2: like the
SECS method, this experiment also measures the gate voltages at which electrons
are added to the dot. The detection method is however completely different. Two
current leads are in such proximity to the dot that electrons may tunnel between
the leads and the dot. A small voltage difference is applied between the left and
right leads, and the experiment consists of monitoring the current through the QD
as the gate voltage is varied. Owing to the simple geometry of these structures,
this energy change varies in linear proportion to the gate voltage. Multiplying Vg
scales in Fig. 1.2 (a) or Fig. 1.3 (c) by a geometric factor converts this scale into
an energy scale for the QD.
14 Quantum Dots: a Survey

However, SETS experiments in planar QDs have some serious shortcomings.

The tunneling barriers which form a QD do not have a well defined shape, and
are strongly influenced by the voltage applied to the gates. Consequently, it is not
possible to investigate the regime where Ne approaches zero. Furthermore, the
zero-dimensional quantization energy is much smaller than the “classical” addi-
tion energy e2 =C . Therefore, the Coulomb oscillations are usually very periodic,
and quantum mechanical many-body effects which lead to aperiodicity in the ad-
dition spectra cannot be observed. An alternative approach is to investigate SETS
with a vertical geometry[14, 27, 30, 31, 32].

Vertical Quantum Dots

In these structures current flows vertically with respect to the heterostructure lay-
ers. Like in their planar counterparts, in these vertical QDs the electrons are con-
fined by the combination of the heterostructure layers providing vertical confine-
ment and lithography to provide in-plane confinement; however, the details of
fabrication are quite different. Here no in-plane tunneling is required, allowing
strong lateral confinement which is achieved by eliminating all but a narrow pillar
in a modified double-barrier (single QD) or triple-barrier (double dot) tunneling
heterostructure.
Fig. 1.5 (a) shows a schematic diagram of a gated vertical QD made from a
double-barrier heterostructure (DBH)[33]. The DBH consists of an undoped 12.0-
nm In0:05 Ga0:95 As well and undoped Al0:22 Ga0:78 As barriers of thickness 9.0 and
7.5 nm. The source and drain contacts are made from n-GaAs and are lightly
doped close to the DBH. The DBH is processed to form a mesa with a top contact
geometrical diameter of 0.5 m through the use of a combined dry and wet etch
to a point just below the DBH region. The effective diameter for electron con-
duction is much smaller than the geometrical dot diameter, and is estimated to be
approximately 0.1 m when the dot contains a few electrons. A circular Schottky
gate is placed on the side of the mesa close to the DBH. The cross-sectional view
of the device appears in the scanning electron micrograph in Fig. 1.5 (b). The dot
in this device is strongly confined by the heterostructures in the vertical direction
and is parabolically confined by the depletion potential in the lateral direction.
1.2 Construction and Measurement 15

Figure 1.5: (a) Schematic diagram of the gated QD device. (b) Scanning electron
micrograph of the cross section of the device. The white bar indicates the position
of the double-barrier heterostructure[33].
16 Quantum Dots: a Survey

drain Vd
Id

gate
dot 1
Vg dot 2
D.G.Austing et al.
source Jpn.J.Appl.Phys. 1997
Figure 1.6: Schematic diagram of a vertical double QD structure[34].

The Schottky gate is suitable for squeezing the lateral size of the dot or to change
the number of electrons Ne in the dot without breaking the rotational symmetry.
The inclusion of In in the well reduces the conduction band edge below the Fermi
level of the contacts. This allows to study linear transport through a verical QD
without doping the barriers.

Double-dot vertical structures[34] are alike, except that a triple barrier replaces
the double barrier heterostructure. Fig. 1.6 schematically depicts a vertical dou-
ble QD structure. The resulting conduction band profile at zero bias is shown
pictorially in Fig. 1.7, along with the heterostructure parameters.

In this short review of QD devices we have completely neglected other impor-

tant types of semiconductor QDs such as semiconductor microcrystals or the so-
called “self-assembled” QDs. These devices can be characterized by strong spatial
confinement and consequently high values of quantization energies ( 50 ; 100
meV). The interested reader can refer to Refs. [20, 35].
1.2 Construction and Measurement 17

Figure 1.7: Pictorial profile of the conduction band for the triple barrier het-
erostructure at zero bias. The material parameters are also given[34].
18 Quantum Dots: a Survey

1.3 Single-Electron Transport

The electronic structure of QDs mimicks that of an isolated atom. It is possible
to attach wires to this “atom” and study transport through its discrete electronic
states. In this section we present the theory of Coulomb oscillations, following
Ref. [36].
We consider a SETS experiment, in the limit of zero source-drain bias Vsd ! 0
(linear transport). Since transport through a QD proceeds by tunneling through its
discrete electronic states, it will be clear that a net current can flow only for certain
values of the gate voltage Vg . In the absence of charging effects (non-interacting
system), a conductance peak due to resonant tunneling occurs when the chemical
potential  in the reservoirs lines up with one of the single-electron energy levels
in the dot. This condition is modified by the charging energy (i.e. electrons interact
via Coulomb repulsion). To determine the location of the conductance peaks as
a function of Vg requires only consideration of the equilibrium properties of the
system, as we now discuss.
The probability P (Ne ) to find Ne electrons in the QD in equilibrium with the
reservoirs is given by the grand canonical distribution function

P (Ne) / exp [; (F (Ne) ; Ne) = (KB T )];

where F (Ne ) is the free energy of the dot and T the temperature. The reservoir
chemical potential  is measured relative to the conduction band bottom in the
reservoirs. In general, P (Ne ) at T = 0 is non-zero for a single value of Ne only
(namely the integer which minimizes the thermodynamical potential (Ne ) =
F (Ne) ; Ne). In that case, the conductance G ! 0 in the limit T ! 0. As
pointed out in Ref. [23], a non-zero G is possible only if P (Ne ) and P (Ne + 1)
are both non-zero for some Ne . Then a small applied voltage is sufficient to induce
a current through the dot, via intermediate states Ne ! Ne +1 ! Ne ! Ne +1 !
: : :. To have P (Ne) and P (Ne + 1) both non-zero at T = 0 requires that both Ne
and Ne + 1 minimize . A necessary condition is (Ne + 1) = (Ne ), or

F (Ne + 1) ; F (Ne) = : (1.6)

This condition is also sufficient, unless has more than one minimum (which is
usually not the case).
1.3 Single-Electron Transport 19

Despite its apparent simplicity, Eq. (1.6) is the most important concept of
Chapter 1. It expresses the equality of the electrochemical potential of dot and
leads. The usefulness of this result is that it maps the problem of determining the
location of the conductance peaks onto the more familiar problem of calculating
the electrochemical potential F (Ne + 1) ; F (Ne ) of the QD, i.e. the energy cost
associated with the addition of a single electron to the dot. At T = 0, the addition
energy A(Ne ) takes the form

A(Ne) = E0 (Ne) ; E0(Ne ; 1) = EF ; (1.7)

where E0 (Ne ) is the ground state energy of the Ne -dependent interacting system,
and EF is the Fermi energy of the reservoirs (we have relabeled Ne by Ne ; 1).
This opens the way to a study of exchange and correlation effects on conductance
oscillations in a QD (see e.g. Figs. 4.1 and 4.2).

1.3.1 “Classical” Theory of Coulomb Blockade

At T = 0 the free energy F (Ne ) equals the ground state energy of the dot, for
P
which we take the simplified form U (Ne ) + p Ep . Here U (Ne ) is the charging
energy, and Ep (p = 1; 2; : : :) are single-electrons energy levels in ascending order,
measured relative to the bottom of the potential well in the QD. The term U (Ne )
accounts for the charge imbalance between dot and reservoirs. The sum over
energy levels accounts for the internal degrees of freedom of the QD. Each level
contains either one or zero electrons. Spin degeneracy, if present, can be included
by counting each level twice, and other degeneracies can be included similarly.
The energy levels Ep are assumed to be independent of Ne . We conclude from
Eq. (1.7) that a peak in the low-temperature conductance occurs whenever

ENe + U (Ne) ; U (Ne ; 1) = EF ; (1.8)

for some integer Ne .

We adopt the simple approximation of the “classical” model of taking the
charging energy into account macroscopically. This is also known as “constant-
interaction model”[37]. This simple model cannot explain addition spectra like the
20 Quantum Dots: a Survey

ones appearing in Figs. 4.1 and 4.2 which show correlation and exchange effects.
However, it is still useful to understand most SETS experiments. We write
Z Ne e
U ( Ne ) = d Q0 (Q0 ) ; (1.9)
0
where
(Q) = Q=C + ext : (1.10)

is the potential difference between dot and reservoir, including also a contribution
ext from external charges (in particular those on a nearby gate electrode). We
parameterize the Coulomb interactions among the electrons in the dot and between
electrons in the dot and those somewhere else in the environment (as in the leads)
by means of a capacitance C , which is assumed to be independent of Ne . This is a
reasonable assumption as long as the dot is much larger than the screening length
(i.e. no electric fields exist in the interior of the dot). The charging energy then
takes the form
(eNe )2
U (Ne) = 2C
+ eNe ext : (1.11)

Qext  Cext plays the role of an “externally induced charge” on the dot, which
can be varied continuously by means of an external gate voltage (in contrast to Q
which is restricted to integer multiples of e). In terms of Qext one can write

(eNe + Qext )2
U (Ne) = 2C
+ constant; (1.12)

which is equivalent to Eq. (1.11). We emphasize that Qext is an externally con-

trolled variable, via the gate voltage, regardless of the relative magnitude of the
various capacitances in the system.
Substitution of Eq. (1.11) into Eq. (1.8) gives
 
Ne ; 12 eC = EF ; eext
2
EN e = ENe + (1.13)

as the condition for a conductance peak. The left-hand-side of Eq. (1.13) defines
a renormalized energy level EN e . The renormalized level spacing
E  =
E +
e2=C is enhanced above the bare level spacing by the charging energy. In the
limit e2 =(C
E ) ! 0, Eq. (1.13) is the usual condition for resonant tunneling. In
1.3 Single-Electron Transport 21

Figure 1.8: Single-electron tunneling through a QD, under the conditions of

Eq. (1.13), for the case where the charging energy is comparable to the level spac-
ing. An infinitesimally small voltage difference is assumed between the left and
right reservoirs. Note that in the picture the symbol e is positive, contrary to the
convention followed in the main text. After Ref. [39].

the limit e2 =(C
E ) ! 1, Eq. (1.13) describes the periodicity of the classical
Coulomb-blockade oscillations in the conductance versus electron density[38].
In Fig. 1.8 we have illustrated the tunneling of an electron through the dot
under the conditions of Eq. (1.13). In panel (a) one has ENe + e2 =2C = EF ;
e  (Ne ; 1), with Ne referring to the lowest unoccupied level in the dot. In panel
(b) an electron has tunneled into the dot. One now has ENe ; e2 =2C = EF ;
e  (Ne), with Ne referring to the highest occupied level. The potential difference
 between dot and reservoir has decreased by jej =C (becoming negative), because
of the added electron. Finally, in panel (c) the added electron tunnels out of the
dot, resetting the potentials to the initial state of panel (a).
Let us now determine the periodicity of the oscillations. Theoretically, it is
convenient to consider the case of a variation of the Fermi energy of the reservoirs
at constant ext . The periodicity
EF follows from Eq. (1.13),

EF =
E  =
E +
e2 : (1.14)
C
In the absence of charging effects,
EF is determined by the irregular spacing

E of the single-electron levels in the QD. The charging energy e2 =C regulates
22 Quantum Dots: a Survey

Figure 1.9: Diagram of the bare energy levels (a) and the renormalized energy
levels (b) (or additon spectrum) in a QD for the case e2 =C  2 h
E i. The renor-
malized level spacing is much more regular than the average bare level spacing
h
E i. Note that the spin degeneracy of the bare levels is lifted by the charging
energy. After Ref. [40].

the spacing, once e2 =C 
E . This is illustrated in Fig. 1.9, for the case that
there is no degeneracy. The spin degeneracy of the levels is lifted by the charging
energy. In a plot of G versus EF this leads to a doublet structure of the oscillations,
with a spacing alternating between e2 =C and
E + e2 =C .
Experimentally, one studies the Coulomb-blockade oscillations as a function
of gate voltage. To determine the periodicity in that case, we first need to know
how EF and the set of single-particle energy levels Ep depend on ext . In a two-
dimensional electron gas, the external charges are supplied by ionized donors and
by a gate electrode (with an electrostatic potential difference gate between gate
and electron-gas reservoir). One has

ext = donors + gate ; (1.15)

where (as well as C ) is a rational function of the capacitance matrix elements of

the system. The value of depends on the geometry. It is reasonable to assume
that the electron gas densities in the dot and in the leads increase, on average,
equally fast with gate , in a planar QD. For equidistant energy levels in the dot we
may then assume that EF ; EN has the same value at each conductance peak. The
1.4 Survey of the Theoretical Work 23

period of oscillations now follows from Eqs. (1.13) and (1.15),

gate =
e : (1.16)
C

1.4 Survey of the Theoretical Work

In this Section we survey the theoretical literature on the electronic structure of
QDs. This short review does not mean to be complete in any sense: instead we
just mention some fundamental papers in the field, with emphasis on electronic
structure and transport properties in the low-magnetic-field regime. For complete-
ness, we also include recent references that appeared after the publication of our
own work.

1.4.1 Single Quantum Dot

True ab initio calculations for QDs, taking into account the detailed atomistic
structure as well as all many-body interactions, are at the moment very difficult,
because of the complexity of the system. It is a fact that almost all theoretical
works rely on the envelope function approximation (see Subsection 2.1.1) and as-
sume a simplified confining potential which is usually parabolic (see Subsection
2.1.4). Kumar et al.[41] solved a Schrödinger-Poisson Equation for a square QD
and found that in the low-energy excitation spectrum the single-particle confine-
ment potential is parabolic to a good approximation; Stopa[42] obtained similar
results and the evidence of a spin-degenerate shell structure corresponding to the
symmetries of the parabolic potential by means of Density Functional Theory
(DFT) [see Subsec. 2.1.4 for more details].

Exact Diagonalization

Because of the competion between kinetic energy, Coulomb interaction and Zee-
man energy, diagonalization of the exact many-body hamiltonian is the most desir-
able approach in many cases. Unfortunately, this is limited to very few electrons
(Ne  6), and frequently special constraints are imposed to reduce the compu-
24 Quantum Dots: a Survey

tational effort, e.g. the basis set is truncated to the first Landau level in strong
magnetic fields, some degrees of freedom are frozen, etc.
The first who stressed the importance of the electronic correlation was Bryant[43],
who performed numerical calculations for Ne = 2 electrons in a two-dimensional
(2D) rectangular box with infinite-potential walls at B = 0 magnetic field. He
investigated the interplay of the kinetic energy ( L;2 ) and the potential energy
( L;1 ) as a function of the the box size Lx ; Ly . He found the energy spectrum to
depend strongly on the ratio Lx =Ly . For sufficiently large L the potential energy
dominates and the possible precursor of a Wigner solid can be seen in both one-
(Lx  Ly ) and two-dimensional (Lx  Ly ) limits.
In the context of the fractional quantum Hall effect (FQHE), Laughlin[44]
studied the 2D system with Ne = 3 in a strong magnetic field. The effect of con-
finement on single-particle wavefunctions and energies was, however, neglected.
Laughlin explicitely constructed spin-polarized correlated states in the lowest Lan-
dau level (LLL) and showed that they well approximate exact eigenstates. The
ground state turned out to be incompressible over a range of applied pressure be-
cause only special values of the angular momentum M = 3m (m = 1; 2; 3) of
the ground state minimize Coulomb repulsion. The role of electron-electron in-
teractions including the effect of confinement on single-particle spectra has been
studied by Maksym and Chakraborty[45]. They calculated energy spectra for
Ne = 3; 4 spin-polarized electrons in strong magnetic fields and pointed out the
competition of kinetic and interaction energy. As a result of this competition,
the angular momentum of the ground state of the electron system changes with
increasing B through a series of “magic numbers”. These strongly correlated
states can be considered as precursors of FQHE ground states with different fill-
ing factors. Correlated electronic states, however, cannot be probed by infrared
spectroscopic techniques because far-infrared radiation couples to the center-of-
mass motion and hence it is insensitive to the interaction when the confinement is
parabolic[46]. This explains why subsequent works focused on alternative physi-
cal probes of correlation.
Maksym and Chakraborty[47], Wagner et al.[48] investigated the changes in
magnetization vs B for Ne = 2. Increasing B causes the ground-state angular mo-
mentum and spin to discontinuously jump. Pfannkuche and Gerhardts[49] consid-
1.4 Survey of the Theoretical Work 25

ered the effects of deviations from a parabolic confinement potential on infrared

spectroscopy (coupling of relative and center-of-mass motion) in the two-electron
system, Merkt et al.[50] studied the two-electron energy spectrum vs the dot size,
while Pfannkuche et al.[51] examined the role of correlation in the singlet ground
state.
Another exploited excitation channel was the radiative recombination of electrons
with valence band holes localized by acceptors. Hawrylak and Pfannkuche[52]
analyzed the magnetoluminescence spectrum for a Ne = 3, polarized and unpo-
larized, electron system. From the same system Hawrylak[53] deduced a spin-
and angular-momentum-resolved addition spectrum which he succesfully com-
pared with SECS data[27].
Eric Yang et al.[54] exactly diagonalized a system up to 6 electrons (over a LLL-
only basis) and obtained the addition spectrum in the strong B regime. In partic-
ular, the so-called “maximum-density-droplet” region was explored, and precur-
sors of FQHE droplets were found. With the same approximation later Wójs and
Hawrylak[55] computed one- and two-particle spectral functions by diagonaliza-
tion up to Ne = 10.
An interesting possibility we only mentioned in Subsec. 1.1.2 it is to probe ex-
cited correlated states by means of non-linear transport measurements. Pfannkuche
and Ulloa[56] found quasiselection rules as hallmark of a correlation effect[57],
prohibiting tunneling processes otherwise allowed by energy and spin conserva-
tion. The topic of spin blockade[58, 59] is intriguing on its own: Imamura et
al.[60] considered the possibility of realizing spin-blockade in single and double
QDs in a four-electron low-B system.
We finally mention exact diagonalization studies at low- or zero-field where
exchange effects induce spontaneous spin polarization. Palacios et al.[57] per-
formed exact diagonalizations up to Ne = 5 and unrestricted Hartree-Fock (H-F)
calculations up to 15 electrons. Noticeably the B -range considered was large.
Eto[61], under certain approximations (frozen occupancies of the lowest single-
particle levels), obtained exact results for Ne  8. Ezaki et al.[62] considered
how modifications in the fully three-dimensional QD geometry affect the open-
shell structure, with Ne  11. Finally we cite the exact diagonalization study
(Ne  6) of a self-assembled QD by Wójs and Hawrylak[63].
26 Quantum Dots: a Survey

Hartree, Hartree-Fock, Density Functional Theory

A discussion of Hartree and H-F method applied to QDs can be found in[51, 64].
Pfannkuche et al.[65] found new features evolving in the far-infrared B -dependent
spectra with an increasing number of electrons: the appearance of magnetoplas-
mon excitations was predicted by H-F calculations.
With regards to addition spectra at zero- or low-field, Oaknin et al.[66] performed
a Hartree calculation, Wang et al.[67] a restricted H-F computation, while Macucci
et al.[68] employed (spin-independent) density functional theory (DFT). All these
latter works were unable to resolve the spin-dependent structure of addition spec-
tra. Unrestricted H-F calculations were instead performed by Fujito et al.[69] and
by Tamura[70]. The first one (Ne  12) considered different three-dimensional
geometries (Ne  12) at B = 0, while the latter one investigated the B -dependent
additon spectra of single and coupled QDs.
Steffens et al.[71] made use of current-spin DFT (CSDFT)[72, 73] to study
evolution of Hund’s rules with B in addition spectra. They found that, at low B ,
one can still speak of a generalized Hund’s rule referred to single-particle levels
different than those at B = 0.

Spin and Charge Desity Waves, Wigner Crystallization, Edge States

Kramers and co-workers[74] have carried out a numerical calculation for Ne =

3; 4 in a rectangular box Lx  Ly using a “pocket-state” basis approach. This
approach exploits the potential-energy minima associated with the classical Ne -
electron configurations (see e.g. Ref. [75]) to introduce a finite set of approxi-
mate, localized basis functions for the Ne -electron system in configuration space:
the Hamiltonian is then diagonalized within this basis. For small Lx the single-
particle confinement energy dominates; the charge density of the ground state is
essentialy homogeneous. As Lx increases the potential energy begins to dominate
and the electrons form an inhomogeneous charge distribution resembling a blurred
version of the classical limit of equispaced point charges (Wigner molecule). The
idea that under certain circumstances the QD ground state is predicted to have
some order (whose form is determined by the equilibrium between the confine-
ment and the Coulomb interaction) has been exploited also to explain the origin
1.4 Survey of the Theoretical Work 27

of “magic numbers”[76, 77]. Wigner crystallization in QDs has also been studied
by means of H-F calculations[78], unrestricted spin-and-space H-F[79], Quantum
Monte Carlo simulations[80].
Another intriguing question is the breakdown of Hund’s rules at B = 0. CS-
DFT calculations[81] predicted spin-density wave excitations associated to “nor-
mal” ground state instabilities as far as the electron density increases. Spin-and-
space unrestricted H-F calculations[79] found also some evidence of charge den-
sity wave instabilities. Moreover, CSDFT[82] and partial diagonalization tech-
nique approach[83] studied edge reconstruction phenomena in QDs in the FQHE
regime, maybe connected with the so-called Chamon-Wen edge reconstruction[84].

Analytic Solutions

We mention just a few results. Johnson and Payne[85] exactly solved the prob-
lem of Ne electrons of a QD which repel each other via harmonic interaction.
Taut[86] solved exactly the two-body problem for a discrete set of harmonic os-
cillator energies. Dineykhan and Nazmitdinov[87] extended these results to a
three-dimensional oscillator with different in-plane and perpendicular oscillator
frequencies. Gonzales et al.[88] found Padé approximants for the ground state
energies of closed shells.

1.4.2 Coupled Quantum Dots

Until now, double layer two-dimensional electron systems (DL2DESs) have been
extensively studied[89, 90, 91]. These systems, which can be considered the lim-
iting case of a double quantum dot (DQD) when the oscillator confinement energy
goes to zero, exhibit the rich phenomenology of FQHE ground states.
Palacios and Hawrylak[92] investigated the phase diagram of DQDs at high
B in connection with the physics of DL2DESs, introducing an isospin quantum
number analogous to the spin degree of freedom. In the regimes we study in this
Thesis (namely B ' 0 and the overall range of the inter-dot coupling), however,
the analogy is not so striking: unlike the isospin, the spin is a good quantum
number for every value of the inter-dot coupling.
28 Quantum Dots: a Survey

Some studies at B ' 0 appear in the literature. Oh et al.[93] solved the

problem exactly for Ne =2. Tamura[70] treated the problem using a Hartree-Fock
approach. Tokura et al.[94] performed an exact diagonalization for Ne  5.
Asano[95] has studied the phase diagram for 13  Ne  24 by means of a many-
body hamiltonian with “core” electrons frozen in the lower shells. This “core”
approximation might fail when the coupling between dots is strong. Imamura et
al.[96] studied changes in spin and orbital angular momentum vs. B and inter-dot
coupling for N  4. They interestingly find that there is a crossover between two
regimes (inter-dot and intra-dot correlation, respectively), and that the crossover
critical point depends on B .
Hubbard-like hamiltonians for QDs were used —with different levels of approximations—
in Refs. [97, 98, 99], while Refs. [100, 101] are recent DFT studies. The DQD
was also analyzed from a classical point of view[102].
Chapter 2

Theory I: Single-Particle States

In this Chapter and in the next we present and discuss the theoretical frame-
work for the computation of correlated many-body electronic states in semi-
conductor vertical QDs. Our approach is general enough to be easily ex-
tended to QDs with different geometries and to different experimental set-
tings coupling single QDs between each other. Once electronic states are
known, it is straightforward to derive Addition Spectra and to compare them
with transport measurements. Applications of the theory and results will be
shown in Chapters 4, 5, and 6. Here we present some introductory theoret-
ical material. First we introduce the Hamiltonian describing the electronic
motion in QDs (Section 2.1), whitin the framework of the envelope function
approximation, where bulk material parameters as electron effective mass
m and static dielectric constant r are assumed. Then we focus on the
one-electron problem: we consider analytic solutions in Sec. 2.2, while in
Sec. 2.3 we think of one electron as moving in a self-consistent average po-
tential due to the presence of other electrons in the dot. The theory of the
true interacting many-electron system is left to the next Chapter.

2.1 Model

2.1.1 The Envelope Function Approximation

To start the study of electronic states in semiconductor QDs we note that the char-
acteristic size of QDs, like those we reviewed in the previous Chapter, is at least
one-two order of magnitude bigger than the characteristic length of the semicon-
ductor lattice (unit cell). Hence, the QD has a macroscopic size in comparison
to the unit cell, but it is small on all macroscopic scales. One often calls QDs
30 Theory I: Single-Particle States

mesoscopic structures. As a consequence, it is reasonable for mesoscopic struc-

tures to make the usual bulk-semiconductor ansatz for the spatial single-particle
r
wavefunctions ( )[35],
r r r
( ) = ( ) u( ) ; (2.1)
where r is the position of the electron, u(r) is the rapidly oscillating periodic part
of the Bloch function and (r) is the envelope function, which varies on the scale
of several unit cells[103] (see Fig. 2.1). Eq. (2.1) implies that we have a non

Figure 2.1: Schematic diagram of a QD single-electron wavefunction in real

space. In this figure u0 (r ) is the rapidly oscillating part of the Bloch function
k
at = 0, C (r) stands for the envelope function, and (r) for the total wavefunc-
tion: a is the distance between the lattice sites[104].

k
degenerate conduction band with edge at = 0 in the reciprocal space, as it is
the case in usual GaAs/GaAlAs heterostructures, and that the Bloch function u( ) r
k
refers to the state  0.
In the spirit of the ansatz (2.1), it seems sensible to assume that the energy
eigenvalues of the electron in the periodic lattice, i.e., the energy bands, are not
appreciabily modified by the quantum confinement. Besides, most experimen-
tal work has been carried out on QDs built from wide-band-gap semiconductors
where the electron energies are small compared to the band gap, hence non-
parabolicity effects (i.e. energy-dependent conduction-band effective mass and
band-edge mixing) can be neglected[16]. Of course, if QDs are so small that
the potential profile cannot be considered anymore slowly varying with respect
2.1 Model 31

to the periodicity of the crystalline potential, considerable shortcomings of the

envelope function approximation are expected[105]. It seems then reasonable to
use the envelope function approximation for all QDs but the self-assembled ones
(the smallest ones). Therefore, we use the envelope function and the effective
mass approximation to describe the free motion of electrons in QDs. This means
that the only effect of the periodic lattice is to renormalize the electronic mass,
otherwise the motion of electrons in the bulk crystal is that of a free electron gas.
Throughout this Thesis we will consider only electrons which would belong to the
conduction band if they were in the bulk, and we will assume that valence bands
are completely filled.

2.1.2 Hamiltonian
Within the envelope function approximation, we may write the exact Schrödinger
equation for Ne electrons in a QD or in a system of coupled QDs, given by

H =E ; (2.2)

with
= (r1 s1 ; r2 s2 ; : : : ; rNe sNe )
r
total envelope wavefunction of electrons at position i and with spin projection
along z -axis si = 1=2 (i = 1; : : : ; Ne ), and E total eigenvalue. The total Hamil-
tonian H is the sum of a part acting only on spatial coordinates Hspace and a term
Hspin acting on spin coordinates only:
H = Hspace + Hspin: (2.3)

We ignore the effect of spin-orbit coupling which can be shown to be small for a
single conduction band and for a small number of electrons[106].
P
The spatial part Hspace is the sum of a single particle term H0(i) and of the
two-body Coulomb interaction term:
Ne
Hspace =
X
H0 (ri) + 12
X e2
i=1 i6=j r jri ; rj j ; (2.4)
32 Theory I: Single-Particle States

with e < 0 electronic charge (we use Gauss units throughout this Thesis) and
r relative dielectric constant of the host semiconductor, which is assumed to be
experimentally known (r  10 in semiconductors). We have written the electron-
electron interaction as traslationally invariant. This is not a priori true due to the
presence of image charges in the surrounding dielectric materials and gates[16].
For a treatment of QDs surrounded by materials with a dielectric constant different
from that of the host material, see Ref. [107].
We will discuss the single particle term H0 in a moment. The spin part Hspin
is simply a Zeeman coupling between the total-spin magnetic moment and an
B
external magnetic field = B z^ which we possibly apply along the z -axis:

Hspin = gB B S~z ; (2.5)

where B is the Bohr magneton (B =5.7884 10;2 meV/T) and g  is the effective
g-factor (g  1). The total z-component of spin Sz is given by
Ne
X
Sz = ~2 zi ;
i=1
where z is the 2  2 Pauli matrix such that

zi(si) =  (si) ;

with  (s) single-particle spin eigenfunction, and ~ reduced Planck’s constant.
S
The total spin is a vector operator,

S =(Sx; Sy ; Sz ) ;
whose components do not commute with each other and whose quantum number
is S , as it is well known. Since typical single-particle energies computed from the
spatial part of the Hamiltonian H0 are of the order of meV, this Zeeman term is
much smaller and it is usually neglected in finding out electronic ground states,
while excited states are approximately considered doubly degenerate, at least in
not-too-high magnetic field regimes. In other words, the way the spin term Hspin
S
works is just to lift the (2S + 1)-fold degeneracy of the total spin . Hence, the
practical algorithm to find out the ground state electronic configuration we used
2.1 Model 33

S
in our calculations was first to compute electronic terms as if were conserved,
and then to choose the electronic term with maximum Sz [51]. Incidentally, we
observe that this modus operandi could be used in direct diagonalizations of Hspace
to reduce Hilbert-space sector dimensions. This could be achieved by labelling
subspaces with the additional quantum number S , in addition to Sz , even if is S
B
not a constant of motion when is present.
Now we examine the single-particle spatial Hamiltonian H0 . Its more general
form is:
H0( ) = 1  ; e ( ) + V ( ) ;
h i2
r 2m
p cA r r (2.6)

B
where we have introduced the external constant magnetic field = B z^ by means
Ar B Ar p
of the vector potential ( ) [ = r  ( )], and where is the canonical
momentum, p = ;i~r, and m is the effective electron mass (m  0.1m0
r
in semiconductors, m0 free electron mass). V ( ) is the single-particle confining
potential of the QD (or the system of coupled QDs) and c is the speed of light.
To summarize, parameters we need are the effective mass m , the static dielectric
constant r and the effective g -factor g . These quantities describe the effect of
the crystalline periodic potential and the screening of all the other electrons with
respect to the few electrons we look at in the dot.

2.1.3 Cylindrical Symmetry and Magnetic Field

r
Until now the Hamiltonian H0 ( ) is rather general and the choice of the z -axis
r
and of V ( ) is completely arbitrary, so it could describe any type of dot geometry
or confining potential. Now we specialize in QDs with a cylindrical symmetry
around the z -axis. This is the case of disk-shaped QDs built by depletion of a
two-dimensional electron gas by means of electrodes, or of the so called vertical
QDs, single or coupled. This symmetry means that the projection along z of
r
the orbital canonical angular momentum Lz and the confining potential V ( ) are
commuting operators:
[Lz ; V (r)] = 0; (2.7)

with Lz = xpy ; ypx and [A; B ] = AB ; BA. Eq. (2.7) implies that Lz is
conserved, so the orbital angular momentum along z is a good quantum number
34 Theory I: Single-Particle States

(in general this is false for the angular momentum vector L except for spherical
QDs at B = 0).
To prove the previous statement, i.e.

[H0 (r) ; Lz ] = 0; (2.8)

Ar
we need to specify a gauge for the vector potential ( ): we choose the “sym-
metric” one, which is especially advantageous for our purposes, namely

A(r) = 12 B  r: (2.9)

Note that the symmetric gauge is also a Coulomb gauge, i.e.

r
A(r) = 0; (2.10)

as it is easy to check, hence

[A(r) ; p] = 0: (2.11)

We will immediately use this property, after having spent some words about gauge
transformations.

Canonical vs “True” Orbital Angular Momentum

Ar
Of course one is free of choosing any vector potential ( ) whose curl gives the
B
same magnetic field , and all these different choices must be physically equiva-
Ar r
lent. Hovever, for different forms of ( ) the Hamiltonian H0 ( ) changes and so
the probability density current, the velocity and related quantities. In particular, if
one defines, according to Heisenberg’s equations of motion, the velocity operator
v r
as _ ,
r_ = ; ~i [r; H0(r)] ;
one obtains
mv = p ; ec A(r) ;
hence the “true” orbital angular momentum

Ltrue = r  mv
2.1 Model 35

is different from the canonical one L and has the form

Ltrue = L ; ec r  A(r) : (2.12)

Eq. (2.12) is valid in every Coulomb gauge: in the symmetric gauge in addition
we obtain the explicit expression

Ltrue = L ; 2ec r  [B  r] :
This difference is relevant when one looks at the electronic magnetization in the
dot and wants to derive the correct giromagnetic ratio[108].
Let’s now go back to prove Eq. (2.8). We just expand the square of operators
in the right member of Eq. (2.6) using the commutative property (2.11) and the
explicit expression (2.9):
1 h
p ; Ar p
e ( )i2 = 2 + e
(  ) + e2B 2 ;x2 + y2
: (2.13)
p r B
2m c 2m 2m c 8m c2
By means of the triple product rule A
B  C = A  B
C and defining the
cyclotron frequency !c = jej B=m c we eventually obtain

H0(r) = 2pm + V (r) + !2c Lz + m 8!c x2 + y2 :

2  2;

(2.14)

From Eq. (2.14), by inspection, keeping in mind Eq. (2.7) and the fact that 2 =
x2 + y2 is invariant under rotations around the z-axis, it turns out that Lz is con-
served. This is true also for the total angular momentum along z
Ne
X
Ltot
z = Lzi
i=1
for the many-electron system, because Coulomb interaction is invariant under any
rotation.

2.1.4 Dot Confining Potential

r
We now describe the confining potential V ( ) and the kind of dot we are going to
examine. First we assume, consistently with Eq. (2.7), that we can separate V ( )r
into the sum of two parts,

V (r) = V (x; y) + V (z) ;

36 Theory I: Single-Particle States

one for the motion of electrons in the plane xy perpendicular to the growth axis
V (x; y), the other referring to the motion along the z-axis V (z). Systems we think
of are: i) planar single QDs built by depleting a two-dimensional electron gas by
suitable electrodes, ii) disc-shaped vertical QDs, single or coupled, like those we
discussed in Chapter 1. In both cases: 1) the confinement along the z direction
is much stronger than the in-plane one, 2) the potential profile V (z ) can be well
described by a quantum well (QW), single or double, in the case of a single or a
double QD, respectively.
The in-plane confining potential V (x; y ) is more worth discussing. The lat-
eral potential of a QD differs significantly from the Coulomb potential binding
electrons in an atom. Depending on the method used to create the dot, the lateral
potential can be approximated by a different model potential. The potential of a
square etched dot with a considerable radius is fairly close to a rectangular well
with rounded edges. When a dot is small (i.e., when its radius is comparable to
the characteristic length L of the variation of the lateral potential near the edge), a
good approximation offers simple smooth potentials, such as a Gaussian well[20],

V () / ;e;2 =L2 :

In the cases where the scattering states can be neglected, the Gaussian well can
be replaced at the bottom with a parabolic well. Throughout this work, we will
always assume a parabolic form:

V (x; y) = 12 m!02 x2 + y2 = 21 m !022 ;

;

(2.15)

with !0 characteristic frequency, and  in-plane vector position. This approxima-

tion seems particularly fit for QDs of type i) or ii) we have mentioned above. A
r
schematic picture of the model potential V ( ) we use is drawn in Fig. 2.2.
Theoretical and experimental arguments lead to the assumption (2.15):

 The lateral confining potential has mainly an electrostatic origin and repre-
sents the static potential inside the dot at the equilibrium with all the electric
charge density inside and outside the dot. Charge neutrality is ensured by
considering the whole surrounding environment, electrodes included. Rea-
soning in a classical way, we can think that the electric field works against
2.1 Model 37

V(z)
V(x,y) a)
1
2
y b)
x z
in-plane along z
Figure 2.2: Schematic picture of the single-particle confining potential V ( ) = r
V (x; y) + V (z). a) (left panel): the lateral potential V (x; y) is a harmonic circular
oscillator (both for single and coupled QDs). b) (right panel): In the case of two
coupled QDs, V (z ) is a double well. Each well represents a different dot.

the motion of electrons perturbing the equilibrium position inside the dot.
In a first approximation, we can model the restoring force of the field as
linear in the displacement. Hence, the electrostatic confining potential must
be parabolic.

 Whatever model of circularly symmetric lateral potential we consider, it

will not introduce any substantial error if we are interested only in the very
first excited single-particle states.

 Full quantum mechanical calculations have been reported which stress the
validity of the harmonic approximation for a large variety of QDs and values
of parameters. These theoretical schemes take account, in a self-consistent
way, of the combined effect of the interaction of electrons in the dot with
external gates and/or image charges at the heterostructure interfaces and of
the electrostatic screening of the charge inside the dot.
38 Theory I: Single-Particle States

Kumar et al.[41] described the results of a numeric, self-consistent solution

of the Poisson and Schrödinger equations in the Hartree approximation for
a QD produced by a voltage applied to a metal electrode covering a square
GaAs layer with an area of 300300 nm and a thickness of 30 nm, cre-
ated on the surface of a GaAs/AlGaAs QW. A small number of electrons
(Ne  10) was considered. It follows from these calculations that despite
of the square shape of the electrode, the confining potential is to a good ap-
proximation circularly symmetric, with a diameter of  100 nm, which is
considerably smaller than the size of the electrode. The separation between
the energy levels is almost independent of Ne , and the magnetic field evo-
lution of energy levels is similar to that of levels of a parabolic well (see
Sec. 2.2).
Macucci et al.[68] reported similar calculations using a local density func-
tional approach. They found significant deviations from the harmonic con-
finement due to the self-consistent Coulomb interaction of electrons inside
the dot: as the number of electrons Ne is increased, the potential is gradu-
ally flatten out and raised.
Stopa[42] performed accurate density-functional calculations for Ne  100
electrons in a lateral square QD (500 nm  560 nm approximately) pat-
terned via surface gates on the two-dimensional electron gas formed at the
interface of a GaAs-Alx Ga1;x As heterosturcture. He found that the lateral
confining potential can be regarded as parabolic to lowest order with quartic
and higher order corrections whose influence increases near the perimeter.
A parabolic confining potential was also obtained as a result of calculations
regarding n-i-p-i doping superlattices[109], wires in Si[110] and GaAs[111].

 Maybe the strongest argument in favour of Eq. (2.15) is an experimental

one. Kohn’s theorem[46] states that the cyclotron frequency in a transla-
tionally invariant electron system is independent of the electron density and
of the form of the electron-electron interaction. The theorem follows from
the fact that the electric dipole of the radiation only couples to the cen-
tre of mass of the electrons, leaving the relative motion unchanged. This
result has been generalized to parabolic quantum wells[112] and quantum
2.2 Single-Particle States 39

dots where the confinement is parabolic[45, 113, 114]. Far-infrared opti-

cal measurements on artificially fabricated semiconductor QDs have indeed
found the absorption frequencies to be essentially independent of the num-
ber of electrons[115]; this implies that the bare confining potential is nearly
parabolic. Besides, this latter assumption is consistent with the behaviour
of absorption lines in presence of an external magnetic field.

2.2 Single-Particle States

In this Section we carefully inspect solutions of the single-particle Hamiltonian
r
H0( ) of Eq. (2.14) with the lateral parabolic confinement potential (2.15), which
was discussed in the previous Section. A complete understanding of the single-
particle energy spectrum and related degeneracies is the basis for a further inves-
tigation of the many-electron energy shell structure. In this regard, the logical
approach is fully analogous to the study of electronic states in Atomic and Molec-
ular Physics.
In Subsection 2.2.1 we look at the general structure of the single-particle wave-
function and at the motion along the growth direction, while in Subsection 2.2.2
we explicitely solve the in-plane electronic motion problem.

2.2.1 General Considerations

We solve the spatial single-particle Hamiltonian

p2 
H0(r) = 2m + 2 2 2 + V (z) + !2c Lz :
m (2.16)

Here
2 = !02 + !c2 =4
is an effective frequency: if B ! 0 then !c ! 0 and ! !0 , i.e. we recover
the zero-magnetic-field case, while if B ! 1 then ! !c=2 and (2.16) be-
comes the Hamiltonian of a free electron (in the plane) in a transverse magnetic
r
field. The spatial wavefunction solution ( ) of the Schrödinger equation associ-
ated with Eq. (2.16) is the product of the in-plane wavefunction (; ') times the
40 Theory I: Single-Particle States

wavefunction (z ) describing the motion along z :

(r) = (; ') (z) ; (2.17)

where (; ') is the in-plane position vector (x; y ) in polar coordinates.

Motion along the growth axis

Let’s focus on the motion along z . We will always assume a potential invariant
under reflection with respect to the plane at z = 0 perpendicular to the growth
direction, namely
V (z) = V (;z) : (2.18)
From general considerations it follows that (z ) must be even or odd under z !
;z reflection. In particular, if the ground state is bound, then it has to be even
without nodes.
In the case of a single QD, we take as V (z ) a symmetric quantum well:
 
V (z) = V0  jzj ; L2 : (2.19)

Here (x) is the Heaviside function, L is the well width and V0 is the well height.
We assume the same dielectric constant in both the well and the barrier, while the
effective mass can be different (mout in the barrier and mdot in the dot, respec-
tively). The solution is standard in elementary Quantum Mechanics, except that
the condition of continuity of derivatives on both side of one interface must be
replaced by the condition
1 @ 1 @
mout @z
=
mdot @z ; (2.20)

which derives from probability current density conservation[116]. We just sum-

marize well known results: The energy of a bound state z is given by

z = 2~m ;
2 2
(2.21)
dot
with  assuming discrete values obtained by the solution of the transcendental
equation  
 tan L = : (2.22)
2
2.2 Single-Particle States 41
p
Here 0 <  < =L, = mout =mdot , and  = (V0 ; z )2mout =~2 . The form of
the wavefunction (z ), up to a phase, is
8
< c0 C e
> z if z < ; L2 ,
(z) = > c0 cos (z) if ; L2 < z < L2 , (2.23)
:
c0C e;z if z > L2 ,

with normalization constants

 
C L
= e 2 cos  L2 ;
 ; 1
c0 = L + sin (L) + C 2 e;L 2
:
2 2 
As we have already mentioned in Sec. 2.1.4, the confinement of the motion along
z is much stronger than the lateral one: E.g., with typical GaAs parameters,
V0 = 200 meV, and L  10 nm, the separation between ground and first excited
state is about 100 meV, at least one order of magnitude bigger than characteristic
lateral confinement energies. Hence, for a single QD, we will always postulate
the adiabatic condition according to which the electron is in its ground state with
respect to the motion along z . While this condition has no effect on the single-
particle energy spectrum, which is entirely determined by the in-plane motion,
it can have important quantitative consequencies on the many-electron spectrum,
affecting two-particle Coulomb and exchange integrals, as we shall see.
The case of two coupled QDs is a straightforward generalization of the one
above. The potential V (z ) is a double QW:

if z < ;L ; d=2,
8
>
>
V0
if ;L ; d=2 < z < ;d=2,
>
<0
>
>
V (z) = > V0 if ;d=2 < d < d=2, (2.24)
>
>
>
> 0 if d=2 < z < L + d=2,
:
V0 if L + d=2 < z ,

where L is the width of both dots and d the inter-dot distance (see Fig. 2.3).
Although we could write down explicitely a transcendental equation more com-
plex than (2.22) to find eigenvalues and wavefunctions, we prefer to solve the
one-dimensional Schrödinger equation numerically. In Fig. 2.3 we show typical
42 Theory I: Single-Particle States

200
1 2
0.32
jsi

V(z) (meV)
) 0.00 0
−1/2

jai
Wavefunctions (nm
eigenstates
−0.32 of the double well

alternative
basis
p p
(jsi + jai)= 2 (jsi ; jai)= 2
0.32

0.00
−30 −20 −10 0 10 20 30
z (nm)
Figure 2.3: Confinement potential V (z ) along the growth direction z for a system
of two couple QDs. The lower energy wavefunctions (even ground state jsi and
odd first excited state jai) are also drawn.

wavefunctions together with a characteristic potential profile. From energy argu-

ments similar to those of the single QD case, we are now forced to consider not
only the even ground state jsi but also the odd first excited state jai. This has im-
portant qualitative implications for the energy spectrum of double QDs, of course.
Note that, in the limit d ! 1, the ground state jsi turns into the symmetric su-
perposition of ground states of single QWs localized on each dot, while the first
excited state jai is the antisymmetric linear combination, and the two eigenvalues
are degenerate. In the opposite limit, d ! 0, one regains the single QW pic-
ture and jsi and jai become the ground and first excited states of the single QD,
respectively.
We now discuss the in-plane motion. By inspection of Eq. (2.16), it is evident
r
that in the case B = 0 the Hamiltonian H0 ( ) is invariant under reflection in
a plane parallel to the z axis and which contains the origin. This explains why
r
the eigenfunctions of H0 ( ), which are also eigenfunctions of the orbital angular
2.2 Single-Particle States 43

momentum Lz with quantum number m, are doubly degenerate, with opposite

numbers m and ;m corresponding to the same energy, except the case m =
0. This degeneracy can also be associated to the time-reversal symmetry of the
Hamiltonian (2.16). The presence of a magnetic field B breaks the time-reversal
symmetry (or the reflection symmetry), hence states with opposite m are no more
degenerate, as we shall see in the next Subsection.

2.2.2 Fock-Darwin States

In this Subsection we solve analytically the in-plane motion problem. It is conve-
nient to look first at the case B = 0[117]. We already know that solutions (; ')
of the time-independent Schrödinger equation associated with the in-plane Hamil-
tonian   2 2  m 
~2 @ @
;  2 + 2 + !0  (; ') = " (; ')
2 2 (2.25)
2m @x @y 2
are simultaneously eigenfunctions of the z -component of the orbital angular mo-
mentum
@;
Lz = ~i @'
so we write (; ') as the product of a radial part v () by an angular part:
(; ') = v () e;im' : (2.26)

The angular part e;im' is an eigenfunction of Lz with integer quantum number m

(m = 0; 1; 2; : : :).
At this point, we note that unfortunately in the QD literature there are different
conventions about the sign of orbital and spin angular momentum. To be consis-
tent with previous works, from now on we choose to change sign in the definition
of angular momentum. Hence the angular wavefunction

p1 e;im' (2.27)
2
is eigenfunction of
@
Lz = ; ~i @' (2.28)

with eigenvalue ~m, and analogously the Zeeman spin term favours configurations
with maximum positive Sz , if B > 0.
44 Theory I: Single-Particle States

After the separation of variables of Eq. (2.26), we obtain a radial ordinary

differential equation from Eq. (2.25):
 2 
@ v() +
1 @v ()
; m2 v() + k2 ; 22  v() = 0: (2.29)
@2  @ 2
The first bracket is originated by the Laplacian. Here k2 is connected to the eigen-
value " which we will determine compatibly with boundary conditions,

" = ~2mk ;
2 2

and 
 = m~!0
is a characteristic oscillator quantity such that ;1 is the mean square radius of
the ground state, h2 ig:s: = 1=. Eq. (2.29), together with boundary conditions at
the frontier of the variable domain, constitutes a Stourm-Liouville problem to be
solved with the standard procedure of Wave Mechanics. By means of boundary
conditions we ask for a meaningful physical wavefunction, namely v () remains
finite as  ! 0 and v () ! 0 as  ! 1 (bound state).
If one looks at the differential equation (2.29)in the neighbourhood of   0
one retains, at the lowest order,
@ 2 v() + 1 @v() ; m2 v() = 0: (2.30)
@2  @ 2
Because v () must be finite around the origin, we can write down v () as a Taylor
expansion for   0, and the first term in the expansion has to be

v()  s ;
with s integer [a constant is not a solution of (2.30)]. From the compatibility
condition
s2 ; m2 = 0
we choose s = jmj to keep v () finite at the origin. By means of a similar
argument, we find the asymptotic form of v () as  ! 1:

v()  e;2 =2:

2.2 Single-Particle States 45

Now we combine the two results and postulate the form of the true wavefunction
as
v() = jmje;2 =2 F () ; (2.31)

where F () must tend to a non-zero constant value as  ! 0 and cannot diverge
faster than e =2 as  ! 1. Inserting (2.31) into Eq. (2.29) the differential
2

equation
 
d2 F () 2 jmj + 1 dF ()  2  F () = 0 (2.32)
d2
+
 ; 2  d
; 2 (j mj + 1) ; k

is obtained for F () which, by using, instead of , the dimensionless variable

x = 2
is transformed into the Kummer equation
 
x d dFx(2x) + [(jmj + 1) ; x] dFdx(x) ; 12 (jmj + 1) ; 2k F (x) = 0 (2.33)
2 2

whose solution regular at x = 0 is the Confluent Hypergeometric Series[118]

F (x) = M (a; jmj + 1; x)

where
a = 12 (jmj + 1) ; 4k :
2

For large values of x this function would diverge as ex , thus preventing normal-
ization. If, and only if
a = ;n (2.34)

with n = 0; 1; 2; : : : integer radial quantum number, the Hypergeometric Conflu-

ent Series becomes a polynomial and the wavefunction can be normalized. We
then have the solutions

jmj e;2 =2 M ;;n; jmj + 1; 2
e;im'

nm (; ') = Cnm  (2.35)

and
"nm = ~!0(2n + jmj + 1) : (2.36)
46 Theory I: Single-Particle States
degeneracy
... ... ...

5 (0,-4) (1,-2) (2,0) (1,2) (0,4)

4 (0,-3) (1,-1) (1,1) (0,3)

3 (0,-2) (1,0) (0,2)

2 (0,-1) (0,1)

1 (0,0)

Figure 2.4: Shell structure of the single-particle energy spectrum, and associ-
ated degeneracies. Each shell corresponds to the energy ~!0 (N + 1), where
N = 2n + jmj is fixed, and (n; m) are the radial and azimuthal quantum num-
bers, respectively. The degeneracy of each shell (not taking account of spin) is
N + 1.

Here Cnm are normalization factors, "nm is the eigenvalue depending on the cou-
ple of radial and azimuthal quantum numbers (n; m), and nm (; ') are called
Fock-Darwin states, after [119] and [120].
Let’s focus now on the structure of the single-particle energy spectrum. In
Fig. 2.4 we have schematically depicted its shell structure and the associated
degeneracies. Each shell corresponds to the energy ~!0 (N + 1), where N =
2n + jmj is fixed. The shell degeneracy (not taking account of spin) is then N + 1.
Even without analyzing the wawefunctions’ analytical structure, we can very
easily compute the mean square radius h2 inm over any orbital, because the start-
ing Hamiltonian is quadratic in coordinate operators. In such a fortunate case we
can write down the Virial Theorem for bound states[121] (analogous to the one of
Classical Mechanics) as
    
~2
; 2m @2 + @2 =
m !22 ;
@x2 @y2 2 0
where the symbol h: : :i stands for quantum mechanical average over any state.
2.2 Single-Particle States 47

0.8
(0,0)
ψnm(x,y=0) (λ units) 0.6 (0,1)
(0,2)
0.4 (1,0)

0.2

0.0

−0.2

−0.4
−4 −2 0 2 4
−1/2
x (λ units)
Figure 2.5: Plot of Fock-Darwin wavefunctions along the x-axis, at y = 0 (' =
0;  ). All nm ’s are real along this direction, and states corresponding to m are
the same. Functions corresponding to the three lowest energy shells are plotted.

Hence, one has for the state (n; m):

m !022 nm = h"nm inm = ~!0 (2n + jmj + 1) ; (2.37)

which we can recast as

1
 (2n + jmj + 1) :
2 nm = (2.38)
p
We see that h2 i scales as the square root of N + 1, and that it is the same for
each orbital of a given shell, even for different values of m. This considerable
spatial extension of probability density for high quantum numbers is consistent
with the “softness” of the parabolic potential. In a real QD, i.e. in a system with a
finite spatial extension, there are of course physical bounds to the accuracy of this
description.
Now we consider wavefunctions. The Hypergeometric Confluent Series, for
special values of parameters, reduces to simpler classes of Orthogonal Polynomi-
jmj
als, in this case the Generalized Laguerre Polynomials Ln (x). The connection
48 Theory I: Single-Particle States

(0,0)
0.8
(0,1)
(0,2)

units)
1/2 0.6 (1,0)
Pnm( ρ) (λ

0.4

0.2

0.0
0 1 2 3 4
−1/2
ρ (λ units)
Figure 2.6: Plot of Fock-Darwin radial charge density Pnm () =
2 j nm (; ')j . The quantity Pnm () d  is the amount of charge contained be-
2
tween  and  + d  associated to the state (n; m). Note that Pnm does not depend
R1
on the sign of m, and that the normalization is such that 0 d Pnm () = 1.
Functions corresponding to the three lowest energy shells are plotted.

formula is
jmj)! M (;n; jmj + 1; x) ;
Ljnmj (x) = (nn+! jm j! (2.39)

jmj
and an expression for Ln (x) is given by
n
X (n + jmj)!
Ljmj(x) = (;1)i
n (n ; i)!(jmj + i)!i!
xi: (2.40)
i=0
We write down explicitely the first few polynomials:

L00 (x) = 1;
L10 (x) = 1;
L20 (x) = 1; L01 (x) = ;x + 1;
L30 (x) = 1; L11 (x) = ;x + 2;
L40 (x) = 1; L21 (x) = ;x + 3; L02 (x) = 1 ; 2x + x2 =2;
2.2 Single-Particle States 49

L03 (x) = 1; L31 (x) = ;x + 4; L12(x) = 3 ; 3x + x2 =2;

:::
Besides, some useful relations are worth mentioning:
jmj)! ;
Ljnmj (0) = (nn+! jm L0n (x) = 1; Lj1mj(x) = ;x + jmj + 1:
j!
If m = 0, L0n (x) reduces to the Laguerre Polynomial Ln (x),

L0n(x) = Ln(x) :
The following orthogonality relations hold:
Z 1
(n + jmj)!
d x e;x xjmj Ljnmj (x) Ljnmj (x) = n;n
n! : (2.41)
0 0

0
By means of Eq. (2.39) and (2.41) we are now able to calculate normalization
factors Cnm , so the expression (2.35) for the properly normalized Fock-Darwin
states turns into (up to a phase)
s
(jmj+1)=2 n! ;

jmj e;2 =2 Ljmj 2 e;im' :
nm (; ') =  
(n + jmj)! n (2.42)

A few explicit formulae, covering the four lowest shells, are given below:
r
 e;2 =2 ;
00 (; ') =


01 (; ') = p e
;2 =2 ei' ;
 r
  2 e;2 =2ei2' ;
0;2 (; ') =
r
2
 ;1 ; 2
e;2 =2 ;
10 (; ') =

 2
03 (; ') = p  e
3 ;2 =2 ei3' ;
6
 ;

2 ; 2 e; =2 ei' :
11 (; ') =  2

2
In Fig. 2.5 we have plotted a few wavefunctions corresponding to the three
lowest energy shells. The plot is along the x-axis, at y = 0, where all wave-
functions are real, and depend only on the absolute value of m, while in general
50 Theory I: Single-Particle States

wavefunctions are complex, and the phase depends both on the value and sign of
m. One sees that the state (0; 1) changes sign under x ! ;x reflection (in gen-
eral, under a reflection with respect to a plane containing the origin and the z -axis),
while the other states are symmetric. Besides, states (0; 1) and (0; 2) have one
node, while (1; 0) has two nodes. It is interesting to plot not only the wavefunc-
tion itself, but also the radial charge density Pnm () = 2 j nm (; ')j2 . Fig. 2.6
shows this latter quantity corresponding to the same states of Fig. 2.5. The distri-
bution Pnm () represents the amount of probability density of the orbital (n; m)
contained between  and  + d . The normalization prefactor 2 ensures that
Z 1
Pnm() d  = 1:
0
One clearly sees that, at fixed n, more and more probability weight is moved
to larger values of  as long as m is increased. This is in agreement with the
expression (2.38) for the mean square radius. Besides, it is easy to check that
n ; 1 represents the number of nodes of the radial part of the wavefunction. In
this latter plot the fact that the outer maximum is more important than the inner
one is exaggerated as compared to the plot of the wavefunction.
We can get a more useful picture of the distribution of the Fock-Darwin or-
bitals in angle by showing polar diagrams. The functions

p1 e;im'
2
as they stand are not very easy to visualize, since they represent complex func-
tions. However, we can make simple real linear combinations of them. Thus, we
can take the sum of functions for a positive and an equal negative m and divide by
p p
2, or we can take the difference and divide by ;i 2. These functions will be
real and will be normalized and orthogonal, so that this transformation represents
a unitary transformation. This is done in Fig. 2.7, where we plot the square of
these latter linear combinations as a function of angle ', for m = 0; 1; 2; 3
(m = 0 does not depend on angle). Finally, Fig. 2.8 shows two-dimensional
contour plots of Fock-Darwin orbitals of the four lowest energy shells. Here the
quantity plotted is the square modulus of the wavefunction (gray scale). As the
shell number is increased, the probability density is split far apart, and the density
spatial pattern becomes more and more complex.
2.2 Single-Particle States 51

jm = 0i

p p
( jm = 1i + jm = ;1i)= 2 ( jm = 1i ; jm = ;1i)= 2

p p
( jm = 2i + jm = ;2i)= 2 ( jm = 2i ; jm = ;2i)= 2

p p
( jm = 3i + jm = ;3i)= 2 ( jm = 3i ; jm = ;3i)= 2

Figure 2.7: Dependence of Fock-Darwin wavefunctions on angle. Polar diagrams

of linear combinations of eigenfunctions of angular momentum Lz (corresponding
to a degenerate value of energy) are depicted. The square modulus of (e;im' 
p
eim' )= 4 is plotted as a function of azimuthal angle '.
52 Theory I: Single-Particle States
(0; 0)
(n; m)  (n; ;m) means
p
I [ nm (; ' )  n;m ( ; ' )] = 2
Shell

(0; 1) + (0; ;1) (0; 1) ; (0; ;1)

II
Shell

(0; 2) + (0; ;2) (1; 0) (0; 2) ; (0; ;2)

III
Shell

(0; 3) + (0; ;3) (1; 1) + (1; ;1) (1; 1) ; (1; ;1) (0; 3) ; (0; ;3)

IV
Shell

Figure 2.8: Two-dimensional contour plot of Fock-Darwin states of the four low-
est energy shells. The gray scale has the same normalization for all (n; m) orbitals,
with n radial and m angular quantum numbers, respectively. Each plot domain is a
square of 5.65.6 dimensionless length units, where the dimensionless real space
is defined by (x; y ) 1=2 , with  = m !0 =~. Within each shell, indipendent linear
combinations of degenerate wave functions with different values of m are plotted.
2.3 The Hartree-Fock Method 53

Fock-Darwin States in Transverse Magnetic Field

It is straightforward to extend all the results obtained until now with B = 0 to the
case B 6= 0. From the Hamiltonian (2.16) holding in the general case and from
the fact that the solutions (2.42) are eigenfunctions of the angular momentum Lz
we can immediately write down the new energy eigenvalues as

"nm = ~ (2n + jmj + 1) ; ~2!c m: (2.43)

The wavefunctions now have the same form of Fock-Darwin states (2.42) except
that the quantity  occurring in (2.42) must be replaced with

 = m~ : (2.44)

Fig. 2.9 is a plot of a few lowest eingenvalues "nm (in units of ~!0 ) vs the magnetic
field B (expressed as !c =!0 ). As B is increased, one sees that levels labeled by
the maximum value of m go first downwards and then slightly upwards crossing
all levels of lower shells but the ones corresponding to the maximum value of
m within one shell. It is worth to note that, in the limit B ! 1, these lowest
eigenvalues (i.e. those labeled by (0; m), with m > 0) tend to an asymptotic form
corresponding to the lowest Landau level. A second asymptote, with a steeper
slope, corresponding to the first excited Landau level, accumulates a second bunch
of Fock-Darwin states, as long as B rises, and so on. Landau levels are solutions
of the free in-plane electronic motion in the presence of an external static and
homogeneous magnetic field. As B ! 1, the parabolic confinement potential
becomes negligible with respect to the magnetic confinement and one regains the
free electron picture. In our approach, Landau levels are obtained as a special case
of Eq. (2.42) and (2.43) putting !0 = 0. Some care is required to take account of
the degeneracy, which turns into a continuum. For more details on this point, see
Ref. [122].

2.3 The Hartree-Fock Method

Until now we have considered solutions of the single-particle Hamiltonian (2.16).
This is only a starting point for the study of the strongly correlated system of
54 Theory I: Single-Particle States

4
2πεnm /hω0

0
0 1 2 3 4
ωc /ω0
Figure 2.9: Plot of a few lowest eigenvalues "nm (in units of ~!0 ) for a in-
plane single-particle parabolic confinement potential vs magnetic field (in units
of !c =!0 ).

Ne electrons, which we will face in Chapter 3. In particular, we will solve a

many-body model Hamiltonian, written on the basis of some suitable complete
and orthogonal set of single-particle wavefunctions. In this perspective, it is not
fundamental that this set actually represents solutions of the one-body Hamilto-
nian (2.16). Instead, this one-particle basis should embody the essential physics
of the system. In this regard, we can think that electrons move independently in
an average potential produced by all of the electrons. Our strategy then is to use
single-particle wavefunctions which are solutions of a suitable effective Hamilto-
nian describing many-body effects as a one-particle mean-field effective potential.
Hence, one has an effective Schrödinger equation where the motion of other elec-
trons is described by an average electrostatic potential (Hartree equation[123])
2.3 The Hartree-Fock Method 55

which has to be determined self-consistently, together with the wavefunction it-

self. If one, in addition, takes account of Pauli’s Exclusion Principle, then obtains
the Hartree-Fock (H-F) equation[124, 125]. In this Section we will briefly review
the main points of this method. To summarize, we look at H-F method because:

 One-particle wavefunction bases computed by means of H-F method can

constitute the optimal choice in writing down a many-body model Hamilto-
nian. This procedural scheme, borrowed by Quantum Chemistry, is an am-
bitious program and could be a natural development of the work reported in
this Thesis.

 The H-F method is a classical paradigm for a mean-field approach to the

many-body problem. Hence it is sensible to compare its results with those
obtained by means of other many-body techniques, as we will do in Chap-
ter 4.

To keep the discussion simple, in this Section we consider only H-F solutions of
the many-body Hamiltonian H  Hspace (2.4) [we neglect the Zeeman spin-term,
r
as discussed in subsection 2.1.2] with the single-particle Hamiltonian H0 ( ) of
Eq. (2.16) referred to a single QD, the generalization to the case of couple QDs
being straightforward.

2.3.1 The Variational Principle

To derive the H-F Equation, we have first to introduce the Variational Principle.
In this subsection we use Dirac’s notation of “bra” and “ket” for state vectors. We
first want to show that the exact many-body Schrödinger equation

Hj i = Ej i (2.45)

is equivalent to the variational equation

E [ ] = 0; (2.46)

with
E [ ] = h h j Hj j i i : (2.47)
56 Theory I: Single-Particle States

The variation (2.46) can be obtained from (2.47):

h j H ; E j i + h j H ; E j i = 0: (2.48)

Since j i is, in general, a complex function, we can carry out the variation over
the real and imaginary part independently, which is equivalent to carrying out
the variation over j i and h j independently. To see this we use the fact that
Eq. (2.48) is valid for arbitrary infinitesimal j i. We can replace j i by i j i
and get
;i h j H ; E j i + i h j H ; E j i : (2.49)
Together with Eq. (2.48), we find

h j H ; E j i = 0 (2.50)

and the complex conjugate equation. Since j i is arbitrary, Eq. (2.50) is equiva-
lent to the eigenvalue problem (2.45).
The approximation of such variational methods like H-F consists of the fact
that j i is usually restricted to a set of mathematically simple trial wave functions.
As soon as the true function is not in this set, the minimal solution is no longer the
exact eigenfunction, but only an approximation. The variational method is espe-
cially well suited for determining the ground state, since for any trial wavefunction
j i it can be shown[126] that
E [ ]  E0 ; (2.51)

and thus the true ground state energy E0 will always be the lower bound of a
variational calculation. In cases where the ground state energy is not degenerate,
the equality sign in (2.51) is valid, if and only if j i is proportional to the true
ground state j 0 i. If we are interested in the first excited state, we then have to
carry out the variation within the subspace entirely orthogonal to j 0 i. Within
this subspace the first excited state j 1 i has the minimal expectation value of
H. To find j 1i, we must carry out the variation with the subsidiary condition
h 1 j 0i = 0. In principle we can continue and calculate the whole spectrum
using this method.
In practice, however, we do not know j 0 i exactly. From a variation in a
restricted subset of the Hilbert space, we find only an approximation j0 i. For
2.3 The Hartree-Fock Method 57

the calculation of an approximation j1 i to the first excited state j 1 i, we have to

solve the variational equation (2.46) with the supplementary condition that j1 i
is orthogonal to j0 i:
h1 j 0i = 0: (2.52)

For the second excited state, we must have two supplementary conditions, namely:
h2 j 1 i = 0 and h2 j 0 i = 0. These suppplementary conditions are coupled to
the problem via Lagrange parameters. We thus see that for higher excited states
this method quickly gets rather complicated, therefore it has been applied mainly
for the calculation of the ground state. Sometimes, however, these conditions are
simply fulfilled because of symmetry properties, as, for example, is the case for
states with different angular momentum quantum numbers.

Hartree-Fock Equations

We shall assume now that there is an average single-particle potential (later to be

called the Hartree-Fock potential)
Ne
X
HHF = h(ri; si) (2.53)
i=1
whose eigenfunction having the lowest eigenvalue E0HF is an approximation to the
r r r
exact ground state function. This eigenfunction HF ( 1 ; s1 ; 2 ; s2 ; : : : ; Ne ; sNe )
is a Slater determinant
YNe
HF = cy i i j0i (2.54)
i=1
in which the Fermion operators (see Appendix A for Second Quantization formu-
lae and notations we need) cy  , c  correspond to the single-particle spin-orbitals
r
  ( ; s), which are themselves eigenfunctions of the single-particle Hamiltonian
r
h( ; s), namely:
h(ri; si)   (ri; si) = "HF   (ri; si) ; i = 1; : : : ; Ne: (2.55)

Here labels a set of single-particle quantum numbers. In the case of an isolated

r
QD, assuming that the one-electron Hamiltonian h( ; s) has axial symmetry,
stands for (n; m), with m usual azimuthal quantum number and n radial quantum
58 Theory I: Single-Particle States

number. In the case of a double QD, an index i = s; a is added, to label the

wavefunction for the motion along z . We prefer to keep the more general and
compact . We obtain the lowest eigenvalue of HHF if one occupies the Ne lowest
levels in the state HF . Note that, in general, spin-orbitals with the same set of
quantum numbers but with opposite spin  have a different functional form and
a different eigenvalue "  .
The Hartree-Fock method is now defined in the following way. We set up
the determinantal function (2.54), compute the average value of the Hamiltonian
H on this state, and apply the variational principle (2.46), demanding the spin-
orbitals to be chosen to make the average energy stationary. In this process, the
variations of the spin-orbitals must be such to keep them orthonormal. To save
space in notations, we introduce the symbols

xi = (ri; si) ; i = ( i; i ) :
Within this convention, we assume that the symbol of integration over the differen-
tial quantity d x implies a true integration over the space vector and a summation
over the spin variable: Z Z X
dx ! d r:
s=1=2
From the Second Quantization expression of the Hamiltonian H given in Ap-
pendix A is easy to compute the average energy HF H HF :
Ne Ne  
X 1X
HF H HF = "~ [iji] + 2 V [i; j jj; i] ; V [i; j ji; j ]
~ ~ (2.56)
i=1 i;j =1
where the single-particle diagonal element is
Z
"~ [iji] = d x i (x) H0(r) i (x) (2.57)

and
Z Z
V~ [i; j jk; l] = d x d x0 i (x) j (x0 )
e2  (x0 )  (x) :
jr ; r0j k l (2.58)

Because the integration over d x includes summation over spin, the exchange in-
tegral V~ [i; j ji; j ] is zero unless i and j are spin-orbitals associated with the
2.3 The Hartree-Fock Method 59

same spin. To derive the H-F equations, we now wish to vary the i ’s in Eq. (2.56)
mantaining the subsidiary conditions, namely the normalization of all i ’s, and
the orthogonality of any two i ’s. We shall handle these subsidiary conditions by
the method of undetermined multipliers:
" Ne Z #
X
 HF H HF + ij d x i (x) j (x) = 0: (2.59)
i;j =1
We choose to have ji = ij , which gives us the correct number of independent
multipliers ij , one for each subsidiary condition. We shall now vary a particular
i ; if HF H HF is really a mimimum, it will be a minimum as far as the
variation of each i is concerned. We then find that Eq. (2.59) equals
Z  Ne  Z
d x  (x) H0(r) i (x) +
X
d x0 j (x0 ) j (x0 )
e2  (x)
i
j =1 jr ; r0j i
Z
e2 
; d x0 j (x0 ) i (x0 )
jr ; r0j j (x) + ij j (x) = 0; (2.60)

where we have interchanged the names of the variables of integration in the two-
body integrals. In Eq. (2.60) we have the statement that the integral of a certain
function multiplied by i (x), where this quantity is arbitrary, must be zero. That
is, we must have the remaining factor of the integrand equal to zero, which leads
to the equation
Ne Z 
H0(r) i (x) +
X
d x0 j (x0 ) j (x0 )
e2
j =1 jr ; r0j i (x)
Ne Z  Ne
;
X
d x0 j (x0 ) i (x0 )
e2 X

j =1 jr ; r0j j (x) = ; j=1 ij j (x) : (2.61)

This equation is identical with the H-F equation, except for the occurence of the
nondiagonal terms, for j 6= i, on the right side. It is possible to introduce linear
combinations of the spin-orbitals i (x), determined by Eq. (2.61), by a unitary
transformation, making no change neither in the form of the Slater determinant
(up to a factor) nor in the form of the equations, except that the matrix ij is
transformed like the matrix of an ordinary operator under the action of a unitary
transformation. In particular, we can make such a unitary transformation that we
60 Theory I: Single-Particle States

diagonalize the matrix, so that we have only a term in i (x) on the right side of
Eq. (2.61)[127]. In this case we let the matrix element ii be called ;"HF
i , and we
obtain the HF equations:

Ne Z 
H0(r) i (x) +
X
d x0 j (x0 ) j (x0 )
e2
j =1 jr ; r0j i (x)
Ne Z 
;
X
d x0 j (x0 ) i (x0 )
e2 HF
j =1 jr ; r0j j (x) = "i i (x) : (2.62)

This is a set of Ne integro-differential equations: each of them constitutes an

eigenvalue problem, which is not linear, because the Hermitian operator acting on
i (x) depends on the solution i (x) itself. Hence Eqs. (2.62) are solved self-
consistently. The first sum (Hartree term) is made of direct or Coulomb integrals
and represents the electrostatic interaction with the electronic charge, the i-th elec-
tron included; the second sum (Fock term) is a non local operator and is made of
exchange terms. Note that the self interaction of the i-th electron on itself is not
contained in the H-F operator, because when i = j the direct and exchange terms
in the two sums are equal and cancel one each other. The interested reader can
find a discussion on the physical meaning of Eq. (2.62) in the reference cited in
note [127].
We shall now consider the relation between the “one-electron energies” "HF i ,
which do not have a true and precise physical interpretation in a many-body prob-
lem, and the quantity we are really interested in, i.e. the total energy of the system.
First we multiply (2.62) on the left by i (x) and integrate over d x to express "HF
i
in terms of Coulomb and exchange integrals, and then, using Eq. (2.56), we can
write:

Ne Ne ;
X 1X

HF H HF = i ;
"HF 2 i;j =1
Vi ;j ;j ;i ; Vi ;j ;i ;j : (2.63)
i=1

Here we have used the notation of Appendix A for the Coulomb matrix elements
V , which are computed with respect to the H-F orbitals i (x) determined from
Eq. (2.62).
2.3 The Hartree-Fock Method 61

2.3.2 Roothaan’s Equations

In Chapter 4 we will show H-F results for the ground state (and first excited state)
of a single vertical QD. In this Subsection we shall describe the algorithm we nu-
merically implemented. Instead of trying to solve directly the integro-differential
equations (2.62), it is much more practical to build up approximate spin-orbitals
i (x) as linear combinations of the single-particle solutions of H0( ). We can r
set up such linear combinations, with adjustable coefficients; introduce them into
the determinantal function; and vary the resulting orbitals to make the energy sta-
tionary. This variation procedure results in algebric equations for the coefficients,
rather than in differential equations as in (2.62). If we had enough atomic orbitals
so that linear combinations of them could represent the true orbitals with complete
accuracy, the resulting linear combinations would be exact solutions of Eq. (2.62).
In actual cases, however, we use a truncated basis set. This scheme was suggested
by Roothaan[128].
We start by assuming a finite number Nb of unperturbed orbitals  p ( ), eigen- r
r
functions of the single-particle Hamiltonian H0 ( ) of Eq. (2.16). In terms of them,
we expand the spin-orbitals of the H-F method according to the equation
Nb
X
  (r) = cp( )  p (r) : (2.64)
p=1
Note that here we consider only the spatial part of the spin-orbitals.  p ( ) does r
r
not depend on the spin, instead of   ( ). Remember that stands for a suitable
set of spatial quantum numbers. Now we substitute the expansion (2.64) into
the H-F equations (2.62) (after having performed the sum over spin variables),
r r
multiply by  q ( ) and integrate over d . Finally we obtain[129]
Nb
X  
cp( ) Fqp( ) ; q;p"HF = 0 q = 1; : : : ; Nb (2.65)
p=1
where
occupied
X X Nb h
Fqp( ) = q;p"~ q + cl ( 0) cl ( 0) V
0 q ; l0 0 ; l 0 ; p 
 0
l;l =1
0

i
;V q ; l  ; p; l
0
0 0 (2.66)
62 Theory I: Single-Particle States

and Z
"~ q = d r  q (r) H0 (r)  q (r) (2.67)

and the Coulomb matrix elements V are computed with respect to the basis func-
tions . Note that the exchange integrals V q ; l  ; p ; l  on the second line of
0
0 0

Eq. (2.66) are zero unless  = 0 .

The equations (2.65) form a set of Nb simultaneous linear homogeneous equa-
tions in the Nb unknowns cp (  ), p = 1; : : : ; Nb , which describe the spin-orbital
  (r) in Eq. (2.64). For a non trivial solution, we must have
 
det Fqp(  ) ; q;p"HF = 0: (2.68)

This is a secular equation whose Nb roots give the spin-orbital energies "HF  . We
number these in order of energy, from (  )1 to (  )Nb , and it is this index which
we have indicated as (  ) in Eq. (2.65). If Nb is greater than the number of occu-
pied states (  ), as it usually is, we must then make an assignement of electrons to
spin-orbitals, and when we are dealing with the ground state, we naturally assign
them to the spin-orbitals of lowest energy.
Equations (2.65) must be solved by an iterative process, since the Fqp (  ) ma-
trix depend on the spin-orbitals themselves, which in turn depend on the unknown
coefficients cp (  ). In our numerical calculations, we found good convergence
with Nb = 4. For the actual computation of the Coulomb integrals, which is done
once and for all before initializing the self-consistent procedure, see Appendix B.

2.3.3 Discussion
We do not mean here to discuss in a general way the H-F method: the subject is old
and well known. However, there are some points which are worth stressing in this
context, with relation to the study of QDs’ ground state electronic configurations
by means of any mean-field theory.

 Let’s focus on the case of a single vertical QD at zero or low magnetic

field. We anticipate that a shell model, analogous to the Periodic Table
of Elements of Atomic Physics, is presently accepted to explain the main
features of electronic structure, the strongest argument being the experi-
mental evidence[28]. For closed shells, it can be shown[127] that the H-F
2.3 The Hartree-Fock Method 63

potential is perfectly central. On the other hand, the phenomenon called

self-consistent symmetry is known to occur in the iterative procedure for
solving the H-F equations[126], namely the symmetry of the initial trial
wavefunction is preserved in all the successive improvements of the wave-
function during the recursive steps of the computation. Thus, if one chooses
as starting wavefunction an orbital solution of the “bare” potential which has
central symmetry, there are no inconsistencies in the theory.

 However, in the case of an open shell, where “valence” electrons do not oc-
cupy all possible degenerate spin-orbitals, the H-F potential in general has
not central symmetry[127]. To impose a central-field type self-consistent
symmetry is then a further approximation within the H-F method itself. The
aim is to build global electronic densities with the correct symmetry prop-
erties expected a priori from the solution of the true Hamiltonian H[130].

 Moreover, in these cases, a single Slater determinant is not an irreducible

representation of the symmetry group of the true Hamiltonian H. One is
forced to set up linear combinations of Slater determinants with the cor-
rect symmetry properties, according to the Theory of Multiplets of Atomic
Physics. Actually, this is not a big trouble, since it just corresponds to trans-
form the Slater determinant basis set into another one by a unitary transfor-
mation. At the end of this “restoring-symmetry” process, the energy con-
figuration is given by the average of the initial Hamiltonian H on a single
vector of the Hilbert space.

 As we have just seen, the H-F potential in general has not the same symme-
try of the true Hamiltonian H. On the basis of this argument, one could in-
troduce a symmetry-violating mean field approach to describe phase transi-
tions to a symmetry-violating state. This could be done, by example, relax-
ing the condition that the H-F potential must be of central-field type, which
is actually just an approximation in most cases. In the present context of fi-
nite systems, by spontaneous symmetry breaking we mean the formation of
ground states of lower symmetry than that of the confining potential[126].
This approach has already been employed in the nuclear many-body prob-
64 Theory I: Single-Particle States

lem, and there were recent claims of spontaneous symmetry breaking in

QDs at low B on the basis of mean-field calculations[78, 81, 79]. Caution
is needed, however, when considering the latter results, because:

– According to general principles of Quantum Mechanics, the ground

state of the system must be a representation of the symmetry group of
the true Hamiltonian H: one should try then to restore in some way
the symmetries broken in the mean-field approach.[78]
– The H-F method is based on a variational principle, and because of
the self-consistent symmetry of iterative solutions , if we start with
a certain symmetry, we will always stay within this symmetry, and
the minimum of energy can only be found among the wavefunctions
that have this symmetry. Indeed, there is no guarantee that one has
found the lowest energy configuration or that he has found the trial
wavefunction with the correct physical behaviour, which is even more
important.[131]
Chapter 3

Theory II: Many-Electron States

Continuing the exposition of the theoretical model, in this Chapter we face

the true many-body problem. In Section 3.1 we derive a model Hamilto-
nian which describes the interacting electronic system, and which we use to
compute Ne -dependent ground state energies and addition spectra. In partic-
ular, after a general introduction to the problem, in Subsection 3.1.1 we dis-
cuss the single-particle basis used, then we derive the Generalized Hubbard
Hamiltonian (Subsec. 3.1.2), and eventually we show how to diagonalize
the Hamiltonian exploiting the symmetries of the problem (Subsec. 3.1.3).
In view of applications in Chapters 4, 5, and 6, we then review (Sec. 3.2)
the Wigner-von Neumann theorem, which is a very general statement about
how crossing of electronic terms can occur, varying some parameters of the
system.

3.1 Generalized Hubbard Hamiltonian

Solving the problem of Ne electrons in QDs exactly is an impossible task, since
already with Ne = 3 the analogous problem in classical mechanics has only ap-
proximate solutions. One should find eigenvalues and eigenvectors of the total
many-body Hamiltonian H (see Appendix A)
X X X0
H = "0  n  + t0 ;  cy  c 
  ;
1 XXXX
+
2  
V ;  ;  ; cy  cy  c  c ;
0 0 0 0 (3.1)
 0
66 Theory II: Many-Electron States

z AlGaAs
dot 1
GaAs
AlGaAs
d
x y GaAs
dot 2
AlGaAs

Figure 3.1: Two vertically coupled quantum dots. Dots 1 and 2 correspond to
GaAs quantum wells confined by Alx Ga1;x As barriers. The z -axis is the growth
direction, and d is the width of the inter-dot barrier. Varying d means to tune
the coupling between the two dots. If the value of d is large, the coupling is just
of electrostatic nature, while if the inter-dot barrier is thin quantum-mechanical
tunneling effects occur.

r
where the basis set of arbitrary single-particle states f'  ( ; s)g  , over which
H is written, is infinite and complete. If the number of electrons is very small,
however, we could directly make H diagonal using only a reduced truncated basis
set. The accuracy of solutions is controlled by enlarging the set and checking if
the further corrections introduced are smaller than the error tolerated. Still, as the
number of electons Ne increases, matrix dimensions become rapidly so large that
the method of exact diagonalization can be implemented in QDs only for very few
electrons[45, 52].
We choose then to build a many-body model Hamiltonian, replacing a compu-
tational problem with a physical one. The obvious requirement is that this model
Hamiltonian should embody the essential physics of QDs. We are then forced to
accurately consider the specific electronic problem under study.
3.1 Generalized Hubbard Hamiltonian 67

As already stressed in Chap. 2, we consider vertical QDs like those experi-

mentally studied in Refs. [28, 34]. These devices have shown a very rich phe-
nomenology of correlated electronic states. As paradigmatic system we take the
pillar of two vertically coupled QDs depicted in Fig. 3.1, the single-dot system
being a special case. To describe the motion of correlated electrons in this sys-
tem, we can write down an approximate Hamiltonian exploiting the analogy of
QDs with natural molecules. If dots are far apart, the interaction between them is
purely electrostatic and electrons are localized on each isolated QD: a “molecu-
lar” wavefunction of Heitler-London type should be a very good approximation to
the true many-body state. On the other hand, if dots are very close, electrons can
tunnel into the inter-dot barrier and the whole system should behave as a coherent
entity in which electrons are completely delocalized. Intermediate regimes are
controlled by the competion between these two opposite effects, i.e. localization
vs delocalization: the approximate scheme better describing this balance is the
Hubbard model.
The Hubbard model was derived starting from a set of single particle states
(Wannier functions) localized on different sites of a lattice[132]. To do the same
with an array of QDs, we need a complete set of suitable single-particle orbitals
localized on each dot. This task is non-trivial at all.

3.1.1 The Choice of the Basis

We have already solved the single-particle problem for the double-dot system in
Sec. 2.2. The spatial part of the wavefunction, eigenvector of the one-body Hamil-
r
tonian H0 ( ) of Eq. (2.16), is

nml (r) = nm (; ') l (z ) ; (3.2)

where nm (; ') is a Fock-Darwin state and l (z ) is the wavefunction for the
motion along z . The index l assumes two values (l = s; a for symmetric and
antisymmetric states, respectively) for the double dot and only one (l = s) for the
r r
single dot. Even if nml ( ) is a solution of H0 ( ), it is not a suitable basis for our
purposes, since it represents an electron delocalized on both dots (see upper panel
68 Theory II: Many-Electron States

of Fig. 2.3). However, performing the unitary transformation

p
j1i = (jsi + jai) = 2;
p
j2i = (jsi ; jai) = 2; (3.3)
r
where jli stands for the orbital nml ( ), one obtains a new basis set nmi ( ) [with r
i = 1; 2], which is still complete, orthonormal, as it is easy to check, and, in addi-
tion, localized on one dot or the other. The lower panel of Fig. 2.3 shows orbitals
r r
nm1( ) and nm2( ) localized on dot 1 and 2, respectively. If we now write
Eq. (3.1) for the total Hamiltonian H in terms of the new localized basis nmi ( ), r
making the index = (n; m; i) explicit, we obtain that many parameters "0  ,
t0 ;  are zero, because of the cylindrical symmetry of the system [see Eqs. (A.13)
and (A.14), respectively]:
"0nmi = "nm + ("s + "a) =2;
t0nmi;n m i  = n;n m;m (1 ; i;i ) ("a ; "s) =2:
0 0 0 0 0 (3.4) 0

Here "nm is the energy of a Fock-Darwin state and "s, "a are the energies of sym-
metric and antisymmetric states along z , respectively. Thus, on this new localized
basis, the total Hamiltonian H becomes:
X X X0
H = ["nm + ("s + "a ) =2] nnmi ; t cynmi cnmi 
0

nmi nm i;i 0

1X X X X X
+ V
2  n1 m1 i1 n2 m2 i2 n3 m3 i3 n4 m4 i4 n1 m1 i1 ;n2 m2 i2  ;n3 m3 i3  ;n4 m4 i4 
0 0

 cyn m i  cyn m i  cn m i  cn m i  ;
1 1 1 2 2 2 0 3 3 3 0
4 4 4 (3.5)
where we have defined the hopping coefficient t as
t = ("a ; "s) =2;
and the prime on the sum means that i 6= i0 . Until now, there is no approximation
in (3.5).

3.1.2 Single and Coupled Vertical Quantum Dots

To obtain the model Hamiltonian we must simplify the two-body Coulomb term.
Let’s consider [see Eq. (A.15)]
Vn1m1 i1 ;n2 m2 i2 ;n3m3 i3  ;n4m4 i4  =
0 0
3.1 Generalized Hubbard Hamiltonian 69
ZZ
n1m1 i1 (r) n2m2 i2 (r0) n3m3 i3 (r0) n4m4 i4 (r)
e2 dr dr0 :
r jr ; r0j (3.6)

First we note that, because in a two-body scattering process the total orbital angu-
lar momentum is kept constant by Coulomb interaction, the only non-zero matrix
elements are those with
m1 + m2 = m3 + m4 :
Then, we focus on states localized all on the same dot: i.e.

i1 = i2 = i3 = i4 = i:
In this latter case the Coulomb matrix elements do not depend on the i index. Fur-
thermore, among all the other terms, we isolate the “semi-diagonal” ones, namely
those with

(n1 ; m1 ) = (n4 ; m4 ) and (n2 ; m2 ) = (n3 ; m3 ) ; (3.7)

which we adopt as Coulomb (or “direct”) integrals Un1 m1 ;n2 m2

Un1m1 ;n2m2 = Vn1m1 i;n2 m2 i ;n2m2 i ;n1m1 i ;

0 0

and those with

(n1 ; m1 ) = (n3 ; m3 ) and (n2 ; m2 ) = (n4 ; m4 ) ; (3.8)

which we call Exchange integrals Jn1 m1 ;n2 m2

Jn1m1 ;n2m2 = Vn1m1 i;n2 m2 i ;n1m1 i ;n2m2 i :

0 0

Note that “intra-dot” direct and exchange integrals do not depend on the dot where
electrons are localized. Following a similar procedure, we isolate also “inter-dot”
terms with

i1 = i4 and i2 = i3 ;
(n1 ; m1 ) = (n4 ; m4 ) and (n2 ; m2 ) = (n3 ; m3 ) ; (3.9)

which we call inter-dot Coulomb terms U~n1 m1 ;n2 m2 :

U~n1m1 ;n2m2 = Vn1m1 i1 ;n2m2 i2  ;n2m2 i2  ;n1m1 i1 :

0 0 (3.10)
70 Theory II: Many-Electron States

Also inter-dot Coulomb terms U~n1 m1 ;n2 m2 do not depend on dot-site. We do not
take into account inter-dot Exchange terms, which are usually very small. All
direct and exchange terms are positive definite quantities.
Now we are ready to write down the model Hamiltonian. We achieve this goal
separating the two-body part of H into a contribution where the four-operator
product cy1 cy2 c3 c4 is just given by the product of two number operators n1 n2
and into another one which contains all other terms:

H =
"s + "a X
nnmi +
X
"nmnnmi ; t
X
cynm1 cnm2 + h:c:
2 nmi nmi nm
1 X X
+ U n n
2 n1 m1 n2 m2 n1 m1 ;n2 m2 i n1 m1 i n2 m2 i;
1 X X
+ [Un1 m1 ;n2 m2 ; Jn1 m1 ;n2 m2 ] nn1 m1 i nn2 m2 i
2 n1 m1 n2 m2 i
X X
+ U~n1 m1 ;n2m2 nn1 m1 1 nn2 m2 2 0

n1 m1 n2 m2  0

1X
+ V
2 others n1 m1 i1 ;n2 m2 i2  ;n3 m3 i3  ;n4 m4 i4 
0 0

 cyn m i  cyn m i  cn m i  cn m i  :
1 1 1 2 2 2 0 3 3 3 0
4 4 4 (3.11)

The important point here is that the Coulomb matrix elements appearing in the
last sum of (3.11) are always smaller than the direct and exchange terms U , U ; J
and U~ appearing in the previous lines. Indeed, we checked that the biggest “off-
diagonal” terms are of the order of the exchange term J , while J is always signif-
icantly smaller (something less than one order of magnitude, on the average) than
the corresponding direct term. The reader can check this fact on his own directly
in Appendix B for the case of a single two-dimensional QD. The approximation
we choose consists in neglecting all these “off-diagonal” terms. We define then a
Generalized Hubbard Hamiltonian (GHH) HGHH such that

H  HGHH; (3.12)

where

HGHH =
"s + "a X
nnmi +
X
"nmnnmi ; t
X
cynm1 cnm2 + h:c:
2 nmi nmi nm
3.1 Generalized Hubbard Hamiltonian 71

1 X X
+
2 n1 m1 n2 m2
U n1 m1 ;n2 m2 nn1m1 i nn2 m2 i;
i
1 X X
+ [Un1 m1 ;n2 m2 ; Jn1 m1 ;n2 m2 ] nn1 m1 i nn2 m2 i
2 n1 m1 n2 m2 i
X X
+ U~n1 m1 ;n2m2 nn1 m1 1 nn2 m2 2 : 0 (3.13)
n1 m1 n2 m2  0

This is the Hamiltonian we actually diagonalize for a system of two coupled QDs.
The first two addenda are single-particle on-site terms, the third is the hopping
term, the fourth one accounts for the intra-dot Coulomb repulsion between elec-
trons with antiparallel spin, the fifth one refers to electrons with parallel spin (an
exchange contribution must be subtracted to the direct one, in this latter case),
while the last one is the inter-dot electrostatic interaction.
In the case of a single QD, we can suppress the site index i, and the GHH
Hamiltonian reduces to

"nmnnm + 12
X X X
HGHH = Un1 m1 ;n2m2 nn1 m1  nn2m2 ;
nm n1 m1 n2 m2 
1 X X
+ [Un1 m1 ;n2 m2 ; Jn1 m1 ;n2 m2 ] nn1 m1  nn2 m2  ; (3.14)
2 n1 m1 n2 m2 

where we have suppressed a Ne -dependent constant term. In the single QD case,

of course, there are no hopping term and inter-dot electrostatic coupling. Note
that the single-dot Hamiltonian (3.14) commutes with the number operator nnm ,
while the double-dot Hamiltonian (3.13) does not. This means that, while in the
first case single Slater determinants are eigenstates of HGHH , in the second case
we have to diagonalize the Hamiltonian matrix in order to find its eigenvalues.

3.1.3 Diagonalization and Addition Spectra

It is very convenient to exploit the symmetries of Hamiltonian (3.13), to reduce the
dimensions of subspaces over which HGHH must be diagonalized. In this regard,
it is evident by inspection of Eq. (3.13) that the number of electrons Ne , the total
orbital angular momentum (projection along the z -axis) Lz , and the projection of
the total spin along the z -axis Sz commute with the Hamiltonian (3.13).
72 Theory II: Many-Electron States

Thus, the practical algorithm we used to extract eigenvalues and eigenvectors

from HGHH is the following:

 For every set of external parameters, such as an homogeneous external static

magnetic field B or a given value t for the inter-dot coupling, we compute
direct and exchange integrals appearing in Eq. (3.13). While for a two-
dimensional disk these latter are analytically known (see Appendix B), in
general we are forced to compute them numerically.

 On each subspace labeled by a different value of Ne , Sz , and Lz , the Hamil-

tonian HGHH is diagonalized and the minimum energy state of that given
subspace is found: the true ground state of the system is the absolute mini-
mum over the entire set of quantum numbers allowed.

 From the knowledge of the Ne -dependent ground state of the system E0 (Ne )
one obtains in a straightforward way the addition energy A(Ne ), i.e. the
quantity to compare with experimental measures:

A(Ne) = E0(Ne) ; E0 (Ne ; 1) : (3.15)

Actually we considered QDs so weakly coupled to the leads that it is a very

good approximation to treat dots as isolated systems (as we implicitely did):
the addition energy A(Ne ) is then the resonance energy at which an electron
can tunnel between this “closed” system and the leads, idealized as electron
reservoirs [see Eq. (1.7)].

Double Dot Symmetries

Here we spend some words on symmetry notations. Ground state (or excited state)
configurations, frequently called “electron terms”, are labeled in the molecular
notation: , ,
, , ;, I correspond to the total orbital angular momentum
M = 0; : : : ; 5, and the left superscript is 2Sz + 1:
2Sz +1 M:

Actually, we forgot other two symmetry operations for the double dot: (i) inver-
r
sion with respect to the center of the molecule = 0, (ii) reflection with respect to
3.2 Symmetries and Wigner-von Neumann Theorem 73

the plane z = 0. Under both transformation (i) and (ii) the many-body states have
a definite parity. States are labeled with the right subscript g (even) or u (odd)
according to transformation (i), and by the right superscript + (even) or ; (odd)
according to (ii). To summarize the notation, we use the symbol
2Sz +1 M  :
g=u
It is worth mentioning that the above notation is different from the standard
molecular one because of the presence of the magnetic field. In fact, in the stan-
dard notation one has as left superscript 2S + 1 instead of 2Sz + 1, where S is the
total spin and 2S +1 is the molteplicity, and as right superscript an index  which
refers to the reflection with respect to a plane containing the symmetry axis of the
molecule instead of the plane orthogonal to it. If B = 0, the two reflection sym-
metries are not independent, but one can be obtained from the other through the
inversion symmetry g=u. Moreover, the total spin vector is conserved (in the total
Hamiltonian H, not in HGHH ), not only its projection along z , and the degeneracy
is actually 2S + 1. B removes the spin degeneracy, by means of the Zeeman cou-
pling term, and a reflection with respect to a plane containing the symmetry axis
of the molecule is no more a symmetry operation. In this regime, the superscript
2Sz + 1 does not mean any spin degeneracy.

3.2 Symmetries and Wigner-von Neumann Theorem

We mentioned that ground states configurations depend on parameters such as B
or t. The question which arises is whether we are allowed to observe transitions,
i.e. crossing of electron terms, as far as we vary such parameters. The relevance of
this issue is twofold: (i) The “phase space” of artificial molecules is much larger
than that of “natural” molecules. In particular, in natural molecules the inter-
nuclear distance is almost fixed, while we can tune as much as we like the inter-
dot coupling. Another example is the relevance of magnetic field on electronic
motion in QDs, which is much bigger than in the “natural case” (this is due to the
fact that, at the present time, maximum values of B reachable in laboratories are
comparable to typical QDs’ energy scales but are order of magnitude smaller than
typical chemical energies). (ii) These transitions can be experimentally observed.
74 Theory II: Many-Electron States

The answer to the question whether electron-term crossings are allowed is

positive, according to the so-called Wigner-von Neumann theorem (proved in Ap-
pendix C).

If electron terms depend on one parameter, only terms of different symmetry can
intersect, while the intersection of terms of like symmetry is impossible.

By symmetry we here understand all possible forms of symmetry: with respect to

rotations about an axis, reflections in planes, inversion, and also with respect to
interchanges of electrons. In coupled QDs this means that we may be dealing with
terms of different Lz , different Sz , different parity. We emphasise that this result
not only is true for the coupled QD system, but is a general theorem of Quantum
Mechanics; it holds for any case where the Hamiltonian contains some parameter
and its eigenvalues are consequently functions of that parameter. In particular, in
Chapter 6 we analyze electron terms of coupled dots and find that, as the inter-dot
distance varies, terms with different values of spin and angular momentum cross.
Chapter 4

Addition Spectra in Single Vertical

Quantum Dots

Our work was inspired by experimental findings of Tarucha and coworkers[28],

hence Figs. 1 and 2 of the paper which display our theoretical results for addition
spectra should be compared directly with data of Ref. [28]. For the convenience
of the reader, we have reproduced these data below.
76 Addition Spectra in Single Vertical Quantum Dots

Figure 4.1: (a) Coulomb oscillations in the current vs gate voltage at B = 0

T observed for a 0.5 m-diameter dot. (b) Addition energy variation (labeled
“addition energy” in the figure) vs electron number for two different dots with
diameter 0.5 m and 0.44 m, respectively. The inset shows a schematic diagram
of the device. The dot is located between the two heterostructure barriers. After
Ref. [28].

Figure 4.2: Measured evolution of the third, fourth, fifth, and sixth addition spec-
trum current peaks with B field from 0 to 2 T observed for the 0.5 m-diameter
dot of Fig. 4.1. After Ref. [28].
 77

APPLIED PHYSICS LETTERS VOLUME 72, NUMBER 8 23 FEBRUARY 1998

Addition energies in semiconductor quantum dots: Role

of electron–electron interaction
Massimo Rontani, Fausto Rossi,a) Franca Manghi, and Elisa Molinari
Istituto Nazionale per la Fisica della Materia (INFM), and Dipartimento di Fisica, Università di Modena,
via Campi 213/A, I-41100 Modena, Italy
共Received 18 November 1997; accepted for publication 24 December 1997兲
We show that the addition spectra of semiconductor quantum dots in the presence of magnetic field
can be studied through a theoretical scheme that allows an accurate and practical treatment of the
single-particle states and electron–electron interaction up to large numbers of electrons. The
calculated addition spectra exhibit the typical structures of Hund-like shell filling, and account for
recent experimental findings. A full three-dimensional description of Coulomb interaction is found
to be essential for predicting the conductance characteristics of few-electron semiconductor
structures. © 1998 American Institute of Physics. 关S0003-6951共98兲03608-0兴

In semiconductor quantum dots 共QDs兲 Coulomb- single-electron tunneling processes—i.e., between two suc-
correlation effects are expected to become more and more cessive maxima in the conductance—peaks at ‘‘magic’’ val-
pronounced as their spatial confinement is increased. This ues of N (N⫽2,6,12), consistent with the filling of complete
has been so far one of the reasons of interest for such sys- shells calculated8 for a dot of the same symmetry. Moreover,
tems: they display the rich shell structure typical of atomic the experimental analysis showed that unusually large values
physics, but in addition they offer the possibility to tailor the of ⌬A also occur for values of N corresponding to half-shell
confining potential and to vary the electron occupation by filling (N⫽4,9). The origin of these features, reminiscent of
adjusting external parameters,1 thus allowing direct investi- Hund’s rule in atomic physics,5,9,10 is intimately related to
gation of fundamental properties of charge correlation. electron–electron interaction; therefore their quantitative
At the same time, however, these results imply that evaluation is a challenge for any theoretical analysis of ad-
many-body effects cannot be neglected in the theoretical de- dition spectra in QDs.
scription of QDs, and may be very relevant for predictions Our description is based on an accurate treatment of the
on their possible applications, for example, in single-particle Hamiltonian and on the inclusion of Coulomb
semiconductor-based few-electron devices. While capaci- correlation according to first-order perturbation theory: as-
tance and tunneling spectroscopy experiments are becoming suming the many-particle ground state to be described by a
available for different dot structures,2–6 it is still an open and single Slater determinant, the total energy of the full inter-
difficult problem to devise theoretical approaches allowing to acting Hamiltonian is
include many-body effects in calculations for realistic sys-
1
tems. Exact calculations7 are necessarily limited to very few
electrons; state-of-the-art QD structures instead involve sev-
E共 N 兲⫽ 兺
␣␴
⑀ ␣ 具 n̂ ␣ ␴ 典 ⫹ 兺 关 U ␣␤ 具 n̂ ␤ ⫺ ␴ 典
2 ␣␤ ␴
eral electrons 共of the order of ten or hundred兲, therefore in ⫹ 共 U ␣␤ ⫺J ␣␤ 兲 具 n̂ ␤ ␴ 典 兴 具 n̂ ␣ ␴ 典 , 共1兲
general out of reach for these methods.
In this letter we propose an accurate and effective theo- where 具 n̂ ␣ ␴ 典 is the orbital occupation number, ␣ denoting the
retical scheme that includes electron–electron interaction set of radial and angular quantum numbers (n,m), and ␴ the
and can be applied to systems up to a large number of elec- spin value. According to Eq. 共1兲, the evaluation of the ener-
trons. This approach can treat arbitrary three-dimensional gies for the various many-electron states in the dot requires
共3D兲 confinement potentials, and hence deal with realistic only the knowledge of the Coulomb and exchange matrix
QD structures also in the presence of external magnetic field. elements

冕冕 ␾
We apply this scheme to structures that were investigated in
兩 ␣ 共 r兲 兩兩 ␾ ␤ 共 r⬘ 兲 兩 2
2
a recent experiment. The results are in good quantitative U ␣␤ ⫽e 2 drdr⬘ , 共2兲
agreement with the observed spectra,5 and provide a trans- ␬ 兩 r⫺r⬘ 兩

冕 冕 ␾*
parent interpretation of their physical origin.
* 共 r⬘ 兲 ␾ ␣ 共 r⬘ 兲 ␾ ␤ 共 r兲
␣ 共 r兲 ␾ ␤
A key quantity that characterizes transport into a QD is J ␣␤ ⫽e 2 drdr⬘ . 共3兲
the addition energy, i.e., the energy A(N) required in order ␬ 兩 r⫺r⬘ 兩
to place an extra electron into a dot that is initially occupied Here ␬ is the dielectric constant and ␾ ␣ are single-particle
by N⫺1 particles. Such quantity, analogous to electron af- real-space eigenstates of the dot in the presence of the ap-
finity in atomic physics, can be measured experimentally as a plied magnetic field.
function of N. A systematic experiment on disk-shaped dots5 The important feature of the present scheme is that U ␣␤ ,
has shown that the voltage increment ⌬A between successive J ␣␤ are calculated directly, contrary to other common ap-
proaches where Coulomb and exchange integrals are taken as
a兲
Electronic mail: rossi@unimo.it input parameters.11 Thus, many-body effects are taken into

0003-6951/98/72(8)/957/3/$15.00 957 © 1998 American Institute of Physics

78 Addition Spectra in Single Vertical Quantum Dots

958 Appl. Phys. Lett., Vol. 72, No. 8, 23 February 1998 Rontani et al.

FIG. 1. Calculated addition-energy increment ⌬A(N) vs electron number N

for different QD structures characterized by a parabolic potential in the xy
plane 共confining energy ប ␻ 0 兲 and by a finite-barrier quantum-well potential
along the z direction. FIG. 2. Addition energy A(N) vs magnetic field calculated for a realistic
共3D兲 QD structure with confinement energy ប ␻ 0 ⫽7.5 meV and for different
electron numbers. Ground-state configurations, varying with B, are also
shown.
account through 共1兲, and quantum-confinement effects
through the single-particle ingredients, energies ⑀ ␣ and wave
functions ␾ ␣ ; the latter enter only in the calculation of Cou- configuration: the single-particle term favors complete shell
lomb and exchange matrix elements. This has the advantage filling, while the repulsion among parallel-spin electrons,
that realistic confining potentials 共e.g., extracted from high- smaller than the repulsion among opposite-spin ones, makes
resolution transmission electron microscope 共TEM兲 micro- the configurations with maximum total spin energetically fa-
graphs兲 and an external magnetic field can be included quite vored. Hund’s rule is therefore already contained in Eq. 共1兲
easily by chosing the appropriate single-particle Hamil- and clearly explains the physical origin of the half-shell-
tonian, as is now commonly done for the calculation of op- filling structures. In fact, adding an electron to a half-filled
tical properties.12 shell forces the double occupancy of a level: consequently,
Note that previous approaches have modeled the QD ⌬A is raised by the dominant Coulomb repulsion U ␣␣ be-
confinement in terms of a purely two-dimensional 共2D兲 co- tween opposite-spin electrons on the same level.
ordinate space.7,9,10 As a matter of fact, in most state-of-the- Ground-state configurations and filling rules change
art QD structures the confinement is far from being 2D: for when a magnetic field is applied. It affects both single-
example, in the gated dots of Ref. 5 the typical confinement particle energies and U and J integrals through the induced
width in the growth direction z 共of the order of 10 nm兲 is changes in the wave function localization. For sufficiently
comparable with the typical extension of the carrier ground large values, the magnetic field energetically favors configu-
state in the lateral-confinement (xy) plane. Therefore, in our rations with higher total angular quantum number m. This is
calculations we fully retain the 3D nature of the problem and the physical origin of the wiggles in the A(N) vs B plot
mimic the dots of Ref. 5 by assuming a finite-barrier shown in Fig. 2 and observed in the experiments of Ref. 5.
quantum-well potential along z and a parabolic potential in Figure 3 shows the Coulomb and exchange integrals vs
(xy). Note that the assumption of parabolic potentials re- B for the first states, obtained for ប ␻ 0 ⫽7.5 meV. For com-
flects the experimental indications due to the specific sample parison, we also show the corresponding quantities calcu-
structure and is not required by our model. Within the usual lated within the simplified 2D model. We clearly see that U
envelope-function approximation, the only input parameters integrals describing the interaction between opposite-spin
are the electron effective masses 共m 쐓 ⫽0.065m 0 in the dot electrons are smaller by a few meV in the case of 3D con-
and m 쐓 ⫽0.079m 0 in the barrier兲, the dielectric constant in finement, while the differences in the interaction between
the dot ( ␬ ⫽12.98), and the quantum-well height and width parallel-spin electrons are much smaller. This affects dra-
共V 0 ⫽200 meV and L⫽12 nm兲. matically the energy balance which determines ground-state
Our results for the addition-energy variations, ⌬A(N) configurations, thus clearly showing the inadequacy of a pure
⫽A(N⫹1)⫺A(N), are displayed in Fig. 1 as a function of 2D description of state-of-the-art QD structures.
the electron number N for different dots, characterized by The proposed approach shares with the Hartree–Fock
different in-plane confinement energies ប ␻ 0 . Here, A(N) is 共HF兲 method the ansatz for total energy, expressed as the
obtained as E(N)⫺E(N⫺1), where E(N) is the ground- average of the exact Hamiltonian over a single Slater deter-
state energy in Eq. 共1兲. As we can see, ⌬A(N) exhibits peaks minant; the variational prescription—allowing the construc-
corresponding both to complete and half-shell filling, and is tion of optimal single-particle orbitals through self-
in excellent agreement with experiments in Ref. 5. consistency—is not contained in our approach. We notice,
The origin of this result is in the delicate interplay be- however, that in the present case the results of perturbation
tween single-particle contributions and electron–electron re- theory are already much closer to the exact results than in
pulsion, which according to Eq. 共1兲 defines the ground-state previous 2D calculations:13 this is due to the fact that Cou-
 79

Appl. Phys. Lett., Vol. 72, No. 8, 23 February 1998 Rontani et al. 959

suited for applications to dots with confinement potentials of

arbitrary shapes and symmetries. A full 3D description of
Coulomb interaction is found to be crucial in determining
single-electron conductance properties of realistic nanostruc-
tures.

The authors are grateful to C. Calandra, P. Hawrylak,

and D. Pfannkuche for useful discussions. This work was
supported in part by the EC through the TMR-Ultrafast and
HCM-Psik networks.

1
For a recent review, see L. P. Kouwenhoven, C. M. Marcus, P. L.
McEuen, S. Tarucha, R. M. Westervelt, and N. S. Wingreen, in Mesos-
copic Electron Transport, edited by L. L. Sohn, L. P. Kouwenhoven, and
G. Schön 共Kluwer, Dordrecht, 1997兲 共in press兲.
2
FIG. 3. Comparison between Coulomb and exchange integrals U ␣␤ and J ␣␤ N. B. Zhitenev, R. C. Ashoori, L. N. Pfeiffer, and K. W. West, Phys. Rev.
calculated assuming a simple two-dimensional parabolic model 共2D兲 and the Lett. 79, 2308 共1997兲.
3
corresponding three-dimensional model 共3D兲. ␣ and ␤ denote the sets of P. L. McEuen, E. B. Foxman, U. Meirav, M. A. Kastner, Ygal Meir, Ned
radial and angular quantum numbers (n,m) for the two single-particle states S. Wingreen, and S. J. Wind, Phys. Rev. Lett. 66, 1926 共1991兲.
4
involved in the interaction. T. Schmidt, M. Tewordt, R. H. Blick, R. J. Haung, D. Pfannkuche, K. v.
Klitzing, A. Förster, and H. Lüth, Phys. Rev. B 51, 5570 共1995兲.
5
S. Tarucha, D. G. Austing, T. Honda, R. J. van der Hage, and L. P.
lomb integrals are artificially enhanced in 2D with respect to Kouwenhoven, Phys. Rev. Lett. 77, 3613 共1996兲.
6
the realistic 3D description. Hence the role of self- M. Fricke, A. Lorke, J. P. Kotthaus, G. Medeiros-Ribeiro, and P. M.
consistency and the approximations of HF theory are much Petroff, Europhys. Lett. 36, 197 共1996兲.
7
See, e.g., P. A. Maksym and T. Chakraborty, Phys. Rev. Lett. 65, 108
less relevant in 3D. Finally, we point out that the present 共1990兲; U. Merkt, J. Huser, and M. Wagner, Phys. Rev. B 43, 7320
formalism can be reduced to a Hubbard model description: 共1991兲; P. Hawrylak, Phys. Rev. Lett. 71, 3347 共1993兲; D. Pfannkuche, V.
expression 共1兲 is in fact formally equivalent to the exact so- Gudmundsson, and P. A. Maksym, Phys. Rev. B 47, 2244 共1993兲, and
references therein.
lution of a single-site Hubbard Hamiltonian. This is impor- 8
M. Macucci, K. Hess, and G. J. Iafrate, Phys. Rev. B 55, R4879 共1997兲.
tant in view of a direct extension of this approach to coupled 9
L. Wang, J. K. Zhang, and A. R. Bishop, Phys. Rev. Lett. 73, 585 共1994兲.
dots. 10
A. Wojs and P. Hawrylak, Phys. Rev. B 53, 10841 共1996兲.
11
In summary, we have proposed an effective theoretical E.g. F. Manghi, C. Calandra, and S. Ossicini, Phys. Rev. Lett. 73, 3129
共1994兲.
approach for the analysis of addition spectra of quantum dots 12
F. Rossi and E. Molinari, Phys. Rev. Lett. 76, 3642 共1996兲; F. Rossi, G.
by combining a careful 3D description of electron–electron Goldoni, and E. Molinari, ibid. 78, 3527 共1997兲.
13
interaction with the realistic treatment of single-particle A direct comparison with exact results for a 3D vs 2D two-electron dot is
properties. By construction, the proposed scheme is ideally given in M. Rontani, F. Rossi, F. Manghi, and E. Molinari 共unpublished兲.
80 Addition Spectra in Single Vertical Quantum Dots
Chapter 5

The Importance of Electronic

Correlation
82 The Importance of Electronic Correlation
 83

PHYSICAL REVIEW B VOLUME 59, NUMBER 15 15 APRIL 1999-I

Coulomb correlation effects in semiconductor quantum dots: The role of dimensionality

Massimo Rontani, Fausto Rossi, Franca Manghi, and Elisa Molinari
Istituto Nazionale per la Fisica della Materia (INFM), and Dipartimento di Fisica, Università di Modena, via Campi 213/A,
I-41100 Modena, Italy
共Received 27 August 1998兲
We study the energy spectra of small three-dimensional 共3D兲 and two-dimensional 共2D兲 semiconductor
quantum dots through different theoretical approaches 共single-site Hubbard and Hartree-Fock Hamiltonians兲; in
the smallest dots we also compare with exact results. We find that purely 2D models often lead to an inad-
equate description of the Coulomb interaction existing in realistic structures, as a consequence of the overes-
timated carrier localization. We show that the dimensionality of the dots has a crucial impact on 共i兲 the
accuracy of the predicted addition spectra, and 共ii兲 the range of validity of approximate theoretical schemes.
When applied to realistic 3D geometries, the latter are found to be much more accurate than in the correspond-
ing 2D cases for a large class of quantum dots; the single-site Hubbard Hamiltonian is shown to provide a very
effective and accurate scheme to describe quantum dot spectra, leading to good agreement with experiments.
关S0163-1829共99兲10211-X兴

I. INTRODUCTION strength of the Coulomb interaction is also the key parameter

determining the accuracy and range of validity of the ap-
Adding an electron into a semiconductor quantum dot proximations which must be introduced for dots with many
共QD兲 produces a variation in the energy of the system that electrons.
depends on single-particle quantum confinement as well as In this paper we investigate theoretically the addition
on the Coulomb interaction between carriers.1 Understanding spectra of realistic QD structures, with special emphasis on
such addition-energy is a key step toward controlling the the effects of electron-electron repulsion and their depen-
physics of single-electron devices. At the same time, the ad- dence on the geometry and dimensionality of the confining
dition spectra of quantum dots offer a unique probe of few- potential. In Sec. II, we compare different approximate solu-
particle interactions in regimes that are not experimentally tions of the general Hamiltonian for N interacting electrons
accessible in atomic physics. The experimental effort in this confined in a QD structure; in particular we consider the
direction developed very rapidly after the recent fabrication single-site Hubbard 共SSH兲 scheme introduced in Ref. 5, and
of controlled small-QD devices based on gated vertical the standard Hartree-Fock 共HF兲 method.
heterostructures2 or self-assembled dots.3 The resulting addi- In Sec. III, we focus on the simplest case, i.e., a two-
tion spectra show a clear shell structure, corresponding to the electron system within a parabolic confining potential, and
symmetries of the confining potential, with a filling sequence calculate the exact energy eigenvalues and pair-correlation
analogous to Hund’s rule in atomic physics. functions for the 2D and 3D cases. As in Ref. 7, we use this
From the theoretical point of view, a general interpreta- prototypical system—called artificial or QD helium—as a
tion of these features was obtained by calculating the energy reference to evaluate the accuracy of the different approxi-
spectrum for a strictly two-dimensional 共2D兲 quantum dot, mation schemes: We find that both the importance of correc-
and using either exact methods 共for very few electrons兲, or tions beyond the HF scheme, and the differences between
approximate—usually Hartree-Fock—methods.4 The as- HF and SSH schemes, are drastically reduced for a realistic
sumption of a purely 2D model was initially motivated by 3D description of the dot with respect to its 2D modelization,
the typical disklike shape of the QD potential, whose exten- mainly as a consequence of the reduced Coulomb integrals.
sion along z is 共slightly兲 smaller than the lateral extension of This suggests the reliability of a fully 3D mean-field treat-
the carrier ground state in the xy plane. If one adopts a ment of semiconductor QD’s.
separable picture for the QD confining potential, V⫽V(z) Section IV is then devoted to the application of HF and
⫹V(x,y), the relevant 共i.e., lowest兲 single-electron states SSH methods to 3D and 2D quantum dots with a larger
can be all associated to the ground state of V(z). From the number of electrons. We compare both methods for QD
point of view of single-particle states the 2D assumption is structures of different geometries, and demonstrate that SSH
therefore justified. is an accurate and efficient scheme for realistic, i.e., 3D-like,
In view of the three-dimensional 共3D兲 nature of the Cou- dots. Finally, we discuss the implications of our results for
lomb interaction, however, the 2D model introduces addi- the interpretation of recent experimental data vs magnetic
tional approximations in the calculation of the Coulomb in- field in QD structures, and draw some conclusions.
tegrals, which are sensitive to the spatial extension—2D vs II. THEORETICAL APPROACH: EXACT FORMULATION
3D—of the single-particle wave functions.5,6 In turn, Cou- AND APPROXIMATION SCHEMES
lomb integrals control electron-electron correlation, and in-
fluence the quantitative determination of addition spectra and Our aim is to describe N electrons, confined in a QD
their dependence on magnetic field. At the same time, the structure 共with harmonic in-plane confining potential兲 and

0163-1829/99/59共15兲/10165共11兲/$15.00 PRB 59 10 165 ©1999 The American Physical Society

84 The Importance of Electronic Correlation

10 166 RONTANI, ROSSI, MANGHI, AND MOLINARI PRB 59

冕 冕 ␾*
interacting via Coulomb law, possibly in the presence of an * 共 r⬘兲 ␾ ␣ 共 r⬘兲 ␾ ␤ 共 r兲
␣ 共 r兲 ␾ ␤
external magnetic field perpendicular to the plane. The gen- J ␣␤ ⫽e 2 dr dr⬘. 共5兲
eral N-particle Hamiltonian is ␬ 兩 r⫺r⬘兩
N In this way, Eq. 共2兲 becomes
e2
Ĥ⫽ 兺 Ĥ 0 共 i 兲 ⫹ 21 兺 ␬ 兩 ri ⫺r j 兩
, 共1兲
i⫽1 i⫽ j Ĥ⫽ĤSSH⫹ 21 兺 ⬘ 兺 V ␣ ␴ , ␤ ␴ ⬘; ␥ ␴ ⬘, ␦ ␴ ĉ ␣† ␴ ĉ ␤† ␴ ⬘ĉ ␥ ␴ ⬘ĉ ␦ ␴ ;
␣␤␥ ␦ ␴␴ ⬘
where the single-particle Hamiltonian, within the effective- 共6兲
mass approximation, is
where the prime on the first summation is to omit the terms

冉 冊 2 with ␣ ⫽ ␦ , ␤ ⫽ ␥ and ␣ ⫽ ␥ , ␤ ⫽ ␦ and

1 e 1
Ĥ 0 共 i 兲 ⫽ p̂⫹ Â共 ri 兲 ⫹ m * ␻ 20 共 x 2i ⫹y 2i 兲 ⫹V 共 z i 兲 .
c 2
2m *
共2兲
ĤSSH⫽ 兺
␣␴
␧ ␣ n̂ ␣ ␴

Here  is the vector potential, ␬ and m * are the scalar di-

electric constant and the effective electron mass in the semi- ⫹ 12 兺
␣␤ ␴
关共 U ␣␤ ⫺J ␣␤ 兲 n̂ ␣ ␴ n̂ ␤ ␴ ⫹U ␣␤ n̂ ␣ ␴ n̂ ␤ ⫺ ␴ 兴 .
conductor, ␻ 0 is the characteristic oscillator frequency of the
in-plane confining potential, and V(z) is the confining poten- 共7兲
tial along z; V(z) can be chosen either as a harmonic poten- The relevance of this formal partition is twofold: 共i兲 it natu-
tial 关 V(z)⫽ 21 m * ␻ 20 z 2 兴 , a square well, or a zero-width infi- rally leads to a perturbation expansion in the off-diagonal
nite barrier to describe spherical, cylindrical, or disk-shaped interactions which are in general smaller than the semidiago-
QD structures, respectively. Here Zeeman coupling between nal ones; 共ii兲 moreover, the unperturbed term ĤSSH is one-
spin and magnetic field has been neglected. body-like, with single Slater determinants as exact eigen-
This general Hamiltonian can be written in second quan- states. The SSH approach defined in Ref. 5 consists of
tized form on the complete and orthonormalized basis of
assuming that Ĥ⯝ĤSSH, which amounts to neglecting the
single particle states
second- and higher-order contributions in the off-diagonal
interactions, the first-order one being exactly zero.
Ĥ⫽ 兺
␣␴
␧ ␣ ĉ ␣† ␴ ĉ ␣ ␴ The assumption that the off-diagonal V ␣ , ␤ ; ␥ , ␦ are negli-
gible with respect to the semidiagonal ones is implicit in all
the methods which describe electron correlation in terms of
⫹ 21 兺 兺 V ␣ ␴ , ␤ ␴ ⬘; ␥ ␴ ⬘, ␦ ␴ ĉ ␣† ␴ ĉ ␤† ␴ ⬘ĉ ␥ ␴ ⬘ĉ ␦ ␴ .
␣␤␥ ␦ ␴␴ ⬘
共3兲 the Hubbard model, either in its original form,8 including
only on-site interaction between opposite spin electrons, pro-
portional to U ␣␤ , or adding the interaction between parallel
Here ␧ ␣ are the eigenenergies of the one-particle Hamil- spin electrons as well, proportional to (U ␣␤ ⫺J ␣␤ ). The im-
tonian Ĥ 0 ;ĉ ␣† ␴ and ĉ ␣ ␴ the creation and destruction opera- portant point here is that when the Hubbard model is applied
tors for an electron with orbital index ␣ and spin ␴ ; and to an isolated QD, i.e., to a single site, the Hubbard Hamil-
V ␣ ␴ , ␤ ␴ ⬘ ; ␥ ␴ ⬘ , ␦ ␴ are the two-body matrix elements of the tonian turns out to be one-particle-like: this is so because the
electron-electron interaction intersite hopping of the traditional Hubbard Hamiltonian is
absent in this case and the commutator 关 ĤSSH,n̂ ␣ ␴ 兴 is zero.
V ␣␴,␤␴⬘;␥␴⬘,␦␴⫽ 兺
ss ⬘
冕 ␾* ␣ ␴ 共 r,s 兲 ␾ ␤ ␴ ⬘ 共 r⬘ ,s ⬘ 兲
* As a consequence, the Slater determinants, eigenstates of the
single-particle Hamiltonian Ĥ 0 , are exact eigenstates of
ĤSSH as well.
e2
⫻ ␾ ␥ ␴ ⬘ 共 r⬘ ,s ⬘ 兲 ␾ ␦ ␴ 共 r,s 兲 dr dr⬘ Within the SSH approach the total energy of N electrons
兩 r⫺r⬘兩 in a QD structure is given by
where ␾ ␣ ␴ (r,s)⫽ ␾ ␣ (r) ␹ ␴ (s) are the single-particle eigen- E SSH共 N 兲 ⫽ 具 ⌽ N 兩 ĤSSH兩 ⌽ N 典
functions.
It is useful to isolate, among the Coulomb matrix ele-
ments, the ‘‘semidiagonal’’ ones, namely,
⫽ 兺
␣␴
␧ ␣ 具 n̂ ␣ ␴ 典 ⫹ 兺 关 U ␣␤ 具 n̂ ␤ ⫺ ␴ 典
1
2
␣␤ ␴

V ␣ ␴ , ␤ ␴ ; ␤ ␴ , ␣ ␴ ⫽V ␣ ␴ , ␤ ⫺ ␴ ; ␤ ⫺ ␴ , ␣ ␴ ⬅U ␣␤ , ⫹ 共 U ␣␤ ⫺J ␣␤ 兲 具 n̂ ␤ ␴ 典 兴 具 n̂ ␣ ␴ 典 , 共8兲
where 兩 ⌽ 典 is a Slater determinant eigenvector of Ĥ 0 , and
N
V ␣ ␴ , ␤ ␴ ; ␣ ␴ , ␤ ␴ ⬅J ␣␤ .
具 典 denotes the average over the many-particle eigenstate,
These are the usual direct and exchange integrals which can which in our case simply reduces to the orbital occupation
be written more explicitly as number.
The proposed SSH approach shares in common with

冕冕 ␾
Hartree-Fock methods the form of the total energy, which in
兩 ␣ 共 r兲 兩
2
兩 ␾ ␤ 共 r⬘ 兲 兩 2
U ␣␤ ⫽e 2 dr dr⬘, 共4兲 both schemes is expressed as the average of the exact Hamil-
␬ 兩 r⫺r⬘兩 tonian over a single Slater determinant; the variational
 85

PRB 59 COULOMB CORRELATION EFFECTS IN . . . 10 167

prescription—allowing for the construction of optimal Solutions and notations for the 2D and 3D cases are summa-
single-particle orbitals through the self-consistent solution of rized in Appendix A for both Ĥ CM and Ĥ rm .
a single-particle eigenvalue problem—is not present in the By denoting the CM and rm quantum numbers with capi-
SSH approach. We notice, however, that the importance of tal and small letters, respectively, the eigenvalues for the
self-consistency is strongly related to the relative weight of two-particle system can be written as
Coulomb matrix elements: the HF potential entering the self-
consistent HF one-particle Hamiltonian is in fact related to E NM ,nm ⫽ប ␻ 共 2N⫹ 兩 M 兩 ⫹1 兲 ⫹ ⑀ nm 共13兲
the direct and exchange Coulomb integrals; similarly, the
in the 2D case, and
SSH approximation is exact—without any need of self-
consistency—whenever the higher-order contributions from
the off-diagonal Coulomb matrix elements are negligible.
For this reason we expect that a lower localization of the
冉
E NL,nl ⫽ប ␻ 2N⫹L⫹
3
2 冊
⫹ ⑀ nl 共14兲

confined single-particle states in three dimensions with re- in the 3D spherical case, the cylindrical 3D helium QD re-
spect to two dimensions, giving rise to smaller nondiagonal ducing to an effective 2D one 共see Appendix A兲. Here ⑀ nm
Coulomb integrals, will reduce the difference between HF and ⑀ nl are the rm eigenvalues in two and three dimensions,
and SSH results. To check this point in detail, we have ex- respectively. Note that degeneracy is strongly reduced by
plicitly performed HF calculations; we have used in particu- Coulomb interaction with respect to the noninteracting case.
lar the matrix form of the unrestricted HF equation.9 The corresponding two-particle total eigenfunctions are
Whenever possible, it is obviously useful to compare the
outcomes of different approximate schemes with exact re- ⌿ NM ,nm;SS z 共 r1 ,s 1 ;r2 ,s 2 兲 ⫽⌽ NM 共 R兲 ␸ nm 共 r兲 ␹ 共 S,S z 兲
sults. This is done in Sec. III, where we consider the exactly 共15兲
solvable two-electron QD 共artificial helium兲 in different con-
finement regimes; we will show that the differences between for 2D and 3D cylinders, and
HF and SSH results will be always comparable with those
⌿ NLM z ,nlm z ;SS z 共 r1 ,s 1 ;r2 ,s 2 兲 ⫽⌽ NLM z 共 R兲 ␸ nlm z 共 r兲 ␹ 共 S,S z 兲
between HF and exact results, and that they scale with the
dimensionality of the confining potential. 共16兲
for a 3D sphere. Here ⌽(R) and ␸ (r) are the spatial CM and
III. TWO-ELECTRON PROBLEM rm eigenfunctions, respectively, and ␹ (S,S z ) is the spin
function of a state with total spin ប 2 S(S⫹1) and z projection
In this section we will study the motion of two electrons S z . Note that the parity of the rm spatial eigenfunction is
within a QD structure in two and three dimensions. In this defined 共total orbital angular momentum and spin are con-
case, the exact Hamiltonian 共1兲 reduces to served兲 and connected with the value of total spin by the
antisymmetry of the two-particle total wave function
e2 ⌿(r1 ,s 1 ;r2 ,s 2 ). For both the disk and the cylinder, this im-
Ĥ⫽Ĥ 0 共 1 兲 ⫹Ĥ 0 共 2 兲 ⫹ . 共9兲
␬ 兩 r1 ⫺r2 兩 plies that if m is even, the state is a singlet (S⫽0), and, if m
is odd, the state is a triplet (S⫽1). Similarly for the sphere
Here ri is the position of the electron, ri ⬅(x i ,y i ) in two
case, if l is even, the state is a singlet (S⫽0), and if l is odd,
dimensions or ri ⬅(x i ,y i ,z i ) in three dimensions, and pi the
the state is a triplet (S⫽1).
corresponding momentum. In the above eigenvalues and eigenfunctions of the two-
To solve this equation, we perform the standard electron dot, the ingredients related to the CM Hamiltonian
transformation10 to center of mass 共CM兲 coordinates, R are known analytically 共see Appendix A兲, while the rm en-
⫽(r1 ⫹r2 )/2, P̂⫽p̂1 ⫹p̂2 , and relative-motion 共rm兲 coordi- ergies and wave functions must be determined numerically.
nates, r⫽r1 ⫺r2 , p̂⫽(p̂1 ⫺p̂2 )/2. The two-body Hamiltonian This is done by exact diagonalization of the rm eigenvalue
thus splits into CM and rm parts: problem 共Appendix A兲, thereby yielding the full 2D and 3D
spectrum of the QD helium.
Ĥ⫽Ĥ CM⫹Ĥ rm , 共10兲 Before comparing these exact results with the SSH ap-
proach, we point out that Hamiltonian 共9兲 can be translated
where into a second-quantized form; this is done in terms of the
same quantum numbers using CM and rm variables. The
P̂2 1 two-particle Hilbert space is the Kronecker product of the
Ĥ CM⫽ ⫹ M ␻ 2R 2, 共11兲 CM and rm single-particle spaces, generated, respectively,
2M 2
by the basis 兵 兩 N 典 其 N 共with eigenvalues E N and creation op-
p̂2 1 e2 erators â †N ) and 兵 兩 n 典 其 n 共with eigenvalues ⑀ n and creation
Ĥ rm⫽ ⫹ ␮ ␻ 2r 2⫹ , 共12兲 operators â †n ). Here, for simplicity, N and n label the whole
2␮ 2 ␬r
set of CM and rm quantum numbers, respectively. The
with M ⫽2m * , and ␮ ⫽m * /2. The CM Hamiltonian Ĥ CM second-quantized form of the two-particle Hamiltonian Ĥ, in
has the form of a simple harmonic oscillator. For the rm this variable, is then given by
Hamiltonian Ĥ rm , it is easy to separate variables and obtain
a radial differential equation, which gives solutions with the Ĥ⫽ 兺N E N â †N â N ⫹ 兺n ⑀ n â †n â n ⫹ 兺 V nn ⬘ â †n â n ⬘ . 共17兲
same set of quantum numbers as for the harmonic oscillator. nn ⬘
86 The Importance of Electronic Correlation

10 168 RONTANI, ROSSI, MANGHI, AND MOLINARI PRB 59

FIG. 2. 共a兲 Ground-state energy of the artificial He QD as a

function of the confinement energy ប ␻ 0 , calculated within different
FIG. 1. Ground-state spatial pair-correlation function g(x) for approaches 共exact, SSH, and HF兲. The range of ប ␻ 0 is 4.5–10
3D 共spherical兲 and 2D two-electron QD’s: exact and SSH results meV. The two panels correspond to 2D and 3D 共cylindrical兲 geom-
are reported. Here x⫽(2m * ␻ 0 r 2 /ប) 1/2 is the dimensionless relative etries. The ground-state configuration is always a spin singlet. 共b兲
radial coordinate and g(x) is normalized in such a way that Spin-singlet 共spin-triplet兲 energies vs confinement energies ប ␻ 0 .
兰 ⬁0 g(x)dx⫽1. The in-plane confinement energy is ប ␻ 0 ⫽5 meV. The range of ប ␻ 0 is 1–4.5 meV. The two panels are relative to 2D
and 3D 共cylindrical兲 geometries. The exact ground state is always a
This formulation allows us to obtain the result of the previ- singlet, while a singlet-triplet crossover occurs for both approxi-
ously discussed Hubbard model, by simply neglecting all mated schemes in the low-energy region.
off-diagonal matrix elements in Eq. 共17兲:
ences between exact and SSH results are significantly re-
duced assuming a 3D confining potential. This result is
ĤSSH⫽ 兺N E N â †N â N ⫹ 兺n 共 ⑀ n ⫹V nn 兲 â †n â n , 共18兲 coherent with what is found for other ground-state proper-
ties: Fig. 2共a兲 shows the ground-state energies calculated for
i.e., manifestly the noninteracting Hamiltonian ‘‘renormal- dots with different confinement energies, ប ␻ 0 , in the range
ized’’ by Coulomb interaction. between 4.5 and 10 meV. We compare the exact results with
In order to check the reliability of the approximations and the outcomes of HF and SSH calculations assuming 2D and
the role of dimensionality of the confining potential, we have 3D confinement potentials. Notice that the differences be-
calculated ground-state properties for QD’s with different tween HF and SSH are always smaller—by approximately
confinement energies, i.e., different values of ប ␻ 0 , assuming 50%—than the corresponding differences with respect to the
either a 2D or 3D confining potential. The quality of the exact results; moreover the 3D confinement reduces the over-
ground-state eigenfunctions can be probed by the spatial pair all deviation of both HF and SSH by about 60%.
correlation function f (r): Since the SSH scheme is exact at the first perturbative

冓兺 冔
order in the off-diagonal matrix elements of the e-e interac-
tion, it is interesting to check the importance of the next
f 共 r兲 ⫽K ␦ 共 r⫺ri ⫹r j 兲 . 共19兲 perturbative corrections. Details of how the perturbative ex-
i⫽ j
pansion is actually performed for the helium QD are reported
Because of the circular symmetry, f (r) depends only on the in Appendix B. Figure 3 reports exact and SSH ground-state
modulus of the relative distance r. Here, the factor K is cho- energies compared with the results of second-order perturba-
sen in such a way that, if we define the dimensionless rela- tion theory, showing that second-order corrections become
tive distance x⫽r 冑2m * ␻ 0 /ប, the quantity g(x)⫽x f (x) for much smaller if a 3D confinement is assumed.
the 2D and 3D cylinder cases, and g(x)⫽x 2 f (x) for a 3D The situation becomes more complicated when consider-
sphere is normalized: ing dots with smaller confinement energies: in this case the
HF and SSH differ from the exact result not only quantita-
冕 ⬁

0
g 共 x 兲 dx⫽1.
tively but also qualitatively, predicting the two-particle
ground state to be a triplet instead of a singlet, as it should
be. This is shown in Fig. 2共b兲, where again the exact HF and
We have calculated this quantity both exactly and according SSH results are shown for dots of different confinement en-
to the SSH scheme for an in-plane confining energy ប ␻ 0 ergies. The difference between triplet- and singlet-state ener-
⫽5 meV 共throughout the paper we use m * ⫽0.065m e inside gies decreases with increasing confinement energy both for
the dot and m * ⫽0.079m e outside; ␬ ⫽12.98, as in the QD of SSH and HF approximations until a crossover occurs; as-
Ref. 2; and m e is the electronic mass兲; the results are shown suming a 3D confining potential, the confinement energy of
in Fig. 1. The deviations between SSH and exact results this crossover is reduced, and this again is true both for SSH
clearly depend on the dimensionality of the confining poten- and HF approximations.
tial: in disk-shaped 2D QD’s the SSH approximation is We may summarize this analysis on helium QD by con-
found to overestimate the probability of finding the two elec- cluding that the assumed 3D confinement potential reduces
trons close together, in analogy with HF results7; the differ- the differences between approximate 共SSH and HF兲 solutions
 87

PRB 59 COULOMB CORRELATION EFFECTS IN . . . 10 169

FIG. 3. Ground-state energy of the artificial He QD as a func-

tion of the confinement energy ប ␻ 0 , as obtained via exact diago- FIG. 4. Calculated SSH addition-energy increment ⌬A as a
nalization, SSH approximation scheme, and Rayleigh-Schrödinger function of the total number N of electrons for two different QD
perturbation theory at the second order in the off-diagonal Coulomb structures, both characterized by a parabolic potential in the xy
matrix elements. Both 3D 共spherical兲 and 2D cases are shown. plane 共confining energy ប ␻ 0 ) and by a finite-barrier quantum-well
potential along the z direction 共3D cylindrical model兲.
with respect to the exact ones, both in terms of ground-state
eigenfunctions and eigenenergies. for N⫽16 we find a ground state with total spin S⫽0. Simi-
lar deviations from Hund’s rule have been found for large
IV. MANY-ELECTRON PROBLEM electron numbers (N⬎20) and associated with spin-density-
wave instabilities; for smaller numbers (N⫽16 and 18) the
The key quantity that characterizes single-electron trans- same S⫽0 spin-density-wave state has been found to be a
port into a QD is the addition energy, i.e., the energy A(N) low-energy ‘‘spin isomer,’’ slightly higher in energy than the
required to place an extra electron into a dot that is initially ground-state configuration.13
occupied by N⫺1 electrons. Such a quantity, analogous to From our calculations we may say that the S⫽0 configu-
electron affinity in atomic physics, can be measured experi- ration in dots with large N may be favored by the reduced
mentally as a function of N. It has been shown2 that the repulsion between electrons in high shells: in the fourth
measured voltage increment ⌬A between successive single- shell, for instance, the Coulomb integrals U ␣␤ relative to
electron tunneling processes—i.e., between two successive orbitals with higher values of the orbital momentum may be
maxima in the conductance—peaks at ‘‘magic’’ values of N smaller than the corresponding terms relating two levels with
corresponding to the filling of complete shells (N smaller angular momentum; the double occupation of an or-
⫽2, 6, and 12), as well as to half-shell filling 共e.g., N bital with high orbital momentum m 共i.e., the level with n
⫽4). The existence of these half-shell filling features is ⫽0, m⫽3; see Appendix A for the notation兲 with
reminiscent of Hund’s rule in atomic physics,2,11,12 and is antiparallel-spin electrons may therefore cost less than hav-
intimately related to electron-electron interaction. ing parallel-spin electrons on different degenerate orbitals,
The results of SSH theory for the addition-energy varia- but with smaller m 共i.e., the levels n⫽1 and m⫽1). The
tions, ⌬A(N)⫽A(N⫹1)⫺A(N), are displayed in Fig. 4 as a same interplay also explains the peaks in ⌬A(N) for N
function of the electron number N for two different 3D cy- ⫽14 and 18.14
lindrical quantum dots. Here A(N) is obtained as E SSH(N) We want to stress that also in the case of many electrons
⫺E SSH(N⫺1), where E SSH(N) is the ground-state energy in the reliability of the results of SSH approach is comparable
Eq. 共8兲. As we can see, ⌬A(N) exhibits peaks corresponding with HF ones. The explicit comparison between the addition
both to complete and half-shell filling, thus well reproducing energy variation calculated according to SSH and HF
the experimental evidence in Ref. 2. This behavior is the schemes and for 2D and 3D confinements is reported in Fig.
result of the interplay between single-particle contributions 5, showing that ⌬A always peaks at the same electron num-
and electron-electron repulsion: the single-particle term fa- bers, and that the agreement between SSH and HF results
vors complete shell filling, while the repulsion among improves on going from the 2D to the 3D confinement
parallel-spin electrons, smaller than the repulsion among model.
opposite-spin ones, makes the configurations with maximum Ground-state configurations and filling rules change when
total spin energetically favored 共Hund’s rule兲. This is the a magnetic field is applied. It affects both single-particle en-
physical origin of the half-shell-filling structure: indeed, add- ergies and Coulomb and exchange integrals through the in-
ing an electron to a half-filled shell forces the double occu- duced changes in the wave-function localization. Figure 6
pancy of a level; consequently, ⌬A is raised by the dominant shows the U and J integrals vs B for the first states, obtained
Coulomb repulsion U ␣␣ between opposite-spin electrons on for ប ␻ 0 ⫽7.5 meV. For comparison, we also show the cor-
the same level. responding quantities calculated within a strictly 2D confine-
For some nonclosed shell configurations the total spin ment model. We can see that U integrals describing the in-
turns out to be not determined by Hund’s rule: in particular, teraction between opposite-spin electrons are a few meV
88 The Importance of Electronic Correlation

10 170 RONTANI, ROSSI, MANGHI, AND MOLINARI PRB 59

FIG. 5. Comparison between SSH and HF addition-energy in-

crements ⌬A as a function of the total number N of electrons in the
dot. Here the upper panel corresponds to the 2D geometry, while FIG. 7. Total energy E SSH as a function of the applied magnetic
the lower one corresponds to the 3D cylindrical model. The in- field B corresponding to N electrons in a dot with confinement
plane confinement energy is ប ␻ 0 ⫽7.5 meV. energy ប ␻ 0 ⫽7.5 meV. For any given value of N, all the possible
configurations, denoted by the usual atomic physics terms 2S⫹1 L,
smaller in the case of 3D confinement, while the differences have been considered.
in the interaction between parallel-spin ones are much
smaller. This is going to affect dramatically the energy bal- Figure 7 shows the total energy E SSH as a function of the
ance which determines ground-state configurations, thus applied magnetic field B for different values of the electron
clearly showing the failure of a pure 2D description of state- number N in a dot with confinement energy ប ␻ 0
of-the-art QD structures. ⫽7.5 meV. It appears that for sufficiently large values of B
As already mentioned, according to the SSH approach the the Hamiltonian term linear in the magnetic field becomes
off-diagonal matrix elements of the electron-electron interac- dominant, making configurations with higher total angular
tion are assumed to be negligible. In Fig. 6 the values of two quantum number energetically favorable. This is also the
of them are reported as functions of the applied magnetic physical origin of the wiggles in the A(N) vs B plot shown in
field. As expected, we clearly see that for any B value they Fig. 8 and observed in the experiments reported in Ref. 2.
are negligible compared to all the other semidiagonal contri- Other authors have explicitly considered the question of
butions, and even more so in three dimensions with respect dimensionality in theoretical modelization of semiconductor
to the 2D case. QD’s. Kumar, Laux, and Stern15 self-consistently computed
the one-particle confining potential in a square QD. Accord-

FIG. 6. Coulomb (U ␣ ; ␤ ) and exchange (J ␣ ; ␤ ) integrals as well

as off-diagonal Coulomb matrix elements (V ␣ , ␤ ; ␥ , ␦ ), as functions FIG. 8. Addition energy A(N) as a function of the magnetic
of the magnetic field B for both 2D and 3D cases. Here ␣ and ␤ field B calculated for a realistic 共3D兲 QD structure with confinement
denote the sets of radial and angular quantum numbers (n,m) for energy ប ␻ 0 ⫽7.5 meV and for different values of N. The labels
the various single-particle states involved in the two-body interac- indicate the electronic terms for the ground-state configurations,
tion process. The in-plane confinement energy is ប ␻ 0 ⫽7.5 meV. that depend on B.
 89

PRB 59 COULOMB CORRELATION EFFECTS IN . . . 10 171

ing to their results, our assumption of an in-plane parabolic description of correlation effects in the macroatoms made
confining potential plus a well in the perpendicular direction available by present semiconductor technology.
is seen to be quite reliable and general, as well as the ansatz
of considering only the ground-state motion along z, at least ACKNOWLEDGMENTS
for few electron dots. Steinebach et al.16 pointed out the im-
portance of a full 3D model to treat spin-density excitations We are grateful to D. Pfannkuche and D. Vanossi for
共SDE’s兲 in semiconductor wires and dots. Specifically, they useful discussions. This work was supported in part by the
used the analogous of Eq. 共A4兲 as an effective 3D Coulomb EC through the TMR Network ‘‘Ultrafast quantum optoelec-
interaction, and they found that a 2D description artificially tronics,’’ and by MURST–Italy.
enhances the interaction strength and is unable to predict
experimental Raman spectra. The necessity of a 3D model- APPENDIX A: CM AND RM SOLUTIONS
ization is then seen to emerge not only in the description of FOR THE TWO-ELECTRON DOT
ground-state and single-particle processes, like addition
The present appendix is organized as follows: In Sec. A 1
spectra, but also in two-particle processes, like SDE’s.
we shall show how to reduce the 3D cylindrical helium prob-
lem to an effective two-dimensional one; in Sec. A 2 we shall
summarize the 2D and 3D solutions of the one-particle
V. SUMMARY AND CONCLUSIONS Schrödinger equations for the center-of-mass and the
relative-motion Hamiltonians, Ĥ CM and Ĥ rm , as defined in
We have presented a theoretical investigation of Eqs. 共11兲 and 共12兲.
Coulomb-correlation effects in semiconductor quantum dots.
In particular, we have performed a detailed analysis of the
1. 3D eigenvalue equation for the cylindrical QD
addition-spectrum problem for few-electron quantum-dot
structures 共macroatoms兲, pointing out possible analogies If only the lowest single-particle state ␾ 0 (z) of the quan-
with more conventional Coulomb-correlation effects in tum well is relevant to the two-electron motion, we can write
atomic physics. the spatial-part ⌿(r1 ;r2 ) of our helium wave function as
Our primary goal was to understand to which extent the
various approximation schemes, such as Hartree-Fock or ⌿ 共 r1 ;r2 兲 ⫽ ␺ 共 x 1 ,y 1 ;x 2 ,y 2 兲 ␾ 0 共 z 1 兲 ␾ 0 共 z 2 兲 . 共A1兲
Hubbard models, are able to properly describe Coulomb cor- This approximation is well justified for most cases of inter-
relation in realistic, state-of-the-art QD’s. To this end, we est. Indeed, for the typical QD structure used in the experi-
have first compared approximate results to the exact solution mental investigation of addition spectra2 共the quantum-well
for the prototypical case of a two-electron system, the so- width L⫽12 nm, the barrier height V 0 ⫽200 meV), and the
called quantum-dot helium; we have repeated such analysis energy separation between the ground and first-excited states
for different dimensionalities, considering 3D 共spherical and along z is 56 meV, about one order of magnitude larger than
cylindrical geometry兲 and pure 2D structures. The main re- typical in-plane single-particle confinement energies.
sult is that the degree of accuracy of any approximation Let us now consider the global Schrödinger equation cor-
scheme depends strongly on the dimensionality of the prob- responding to the exact helium Hamiltonian of Eq. 共9兲:
lem. More specifically, the pure 2D model—often used for a
description of quantum dots—is found to give approximate Ĥ⌿ 共 r1 ;r2 兲 ⫽E⌿ 共 r1 ;r2 兲 ; 共A2兲
results which differ significantly from the exact solution. We
have demonstrated that this is not a general failure of the by substituting Eq. 共A1兲, multiplying both sides by
approximation scheme, but that it rather reflects a pathologi- ␾*
0 (z 1 ) ␾ *
0 (z 2 ), and integrating over z 1 , and z 2 , we obtain

冋 册
cal behavior originating from the unphysical nature of the
2
pure 2D model. Indeed, for the case of a 3D cylindrical e2
model—which provides a much better description of realistic 2␧ z0 ⫹ 兺
i⫽1
Ĥ 0 共 i 兲 ⫹
␬
c 共 兩 r1 ⫺r2 兩 兲 ␺ 共 r1 ;r2 兲 ⫽E ␺ 共 r1 ;r2 兲 .
QD structures—the difference between an exact solution and 共A3兲
approximate results is found to be much smaller, thus con-
firming the validity of the various approximation schemes The eigenvalue equation is then reduced to a 2D one, since
considered. ri ⬅(x i ,y i ) and c(r)⫽c( 兩 r1 ⫺r2 兩 ) is an effective Coulomb
The same analysis has been then extended to many- potential, accounting for the geometry of the system:
electron systems for which addition-spectra measurements

冕 冕 兩␾*
0 共 z 1 兲兩 兩 ␾ *
0 共 z 2 兲兩
⫹⬁ ⫹⬁ 2 2
are available. Using different approximation schemes, we
c共 r 兲⫽ dz 1 dz 2 . 共A4兲
find that the deviations between the full 3D model and the ⫺⬁ ⫺⬁ 冑r 2 ⫹ 共 z 1 ⫺z 2 兲 2
simplified 2D quantum-dot model are very significant. The
full 3D model is found to reproduce the experimental data From now on we will drop the constant ground-state energy
for a large class of QD structures where simplified 2D mod- along z (␧ z0 ). As a first step, we evaluate c(r) by solving the
els fail. We conclude that this is due to the unphysical char- quantum well eigenvalue problem 共allowing for different
acter of the pure 2D confinement, for which the various ap- values of the effective mass in the well and in the barrier兲.
proximation schemes often yield unreliable results. A proper Then we numerically integrate Eq. 共A4兲. It is easy to show
description of the QD structure in terms of fully 3D single- analytically some important properties of c(r), namely, that
particle wave functions is therefore required; we have shown
that in this case approximate approaches can give an accurate 0⭐rc 共 r 兲 ⭐1, ᭙r, 共A5兲
90 The Importance of Electronic Correlation

10 172 RONTANI, ROSSI, MANGHI, AND MOLINARI PRB 59

lim rc 共 r 兲 ⫽0, 共A6兲

r→0

lim rc 共 r 兲 ⫽1. 共A7兲

r→⬁

These properties tell us that for large distances r c(r) tends

to the bare Coulomb potential, and that it is strongly reduced
in the neighborhood of the origin, i.e., the more relevant
space region in the computation of Coulomb and exchange
integrals. Figure 9 shows such an effective Coulomb poten-
tial C multiplied by the dimensionless variable x 共introduced
below兲 as a function of x for different values of the quantum-
well width: A monotonic behavior is apparent, going from
the bare Coulomb-potential value in the zero-width limit 共the
function is constant and equal to 1兲, into progressively FIG. 9. Plot of the effective Coulomb potential C(x) multiplied
smaller values, toward the infinite-width case. by the dimensionless coordinate x 关 ⫽x C(x) 兴 as a function of x for
different values of the quantum well width L and for a confinement
2. Exact solutions energy ប ␻ 0 ⫽5 meV. Notice that in the limit L→0 共2D case兲
C(x)→1/x and, therefore, x C(x)→1.
Let us first consider the CM equation, which has the form
of a standard harmonic oscillator and can thus be solved
analytically. For the 2D case 共3D cylindrical兲, its eigenvalues N⫽0,1,2, . . . , M ⫽0,⫾1,⫾2, . . . ,
are
and the corresponding orthonormalized eigenfunctions 共the
NM ⫽ប ␻ 0 共 2N⫹ 兩 M 兩 ⫹1 兲 ,
␧ 2D 共A8兲 so called ‘‘Fock-Darwin’’ states4,17兲 are

⌽ NM
2D
␴ 共 r,s 兲 ⫽ 具 s,r兩 NM ␴ 典 ⫽␭
共 兩 M 兩 ⫹1 兲 /2
冑 N!
␲ 共 N⫹ 兩 M 兩 兲 !
e ⫺iM ␸ r 兩 M 兩 e ⫺ 共 ␭r /2兲 L 兩NM 兩 共 ␭r 2 兲 ␹ ␴ 共 s 兲 .
2
共A9兲

In the 3D spherical case,18 the eigenvalues are

␧ NL
3D
冉
⫽ប ␻ 0 2N⫹L⫹
3
2 冊
, N⫽0,1,2, . . . , L⫽0,1,2, . . . , 共A10兲

and the orthonormalized eigenfunctions ⌽ NLM

3D
␴ (r,s) arez

⌽ NM
3D
L z ␴ 共 r,s 兲 ⫽ 具 s,r兩 NLM z ␴ 典 ⫽
冑冉 2␭ L⫹3/2N! L ⫺ 共 ␭r 2 /2兲 L⫹1/2

⌫ N⫹Ł⫹
3
2
r e
冊
LN 共 ␭r 2 兲 Y LM z 共 ␽ , ␸ 兲 ␹ ␴ 共 s 兲 . 共A11兲

Here, ␭⫽m * ␻ 0 /ប,L Np are generalized Laguerre polynomials,19 ⌫ is the usual gamma function, ␹ ␴ denotes the spin function,
and Y LM z are the spherical harmonics. We have used polar coordinates throughout: r⬅(r, ␸ ) in the 2D 共3D cylindrical兲 case
and r⬅(r, ␽ , ␸ ) in the 3D spherical case. For the 2D 共3D cylindrical兲 case the quantum numbers are (N,M , ␴ ): N is the radial
quantum number, M the angular momentum quantum number 共in this case the total angular momentum coincides with the
component along z, L z ⫽⫺បM ), and ␴ the spin component along z. In the 3D spherical case, on the other hand, the quantum
numbers are given by (N,L,M z , ␴ ): here L is the total angular momentum quantum number, and M z is the magnetic quantum
number, M z ⫽⫺L,⫺L⫹1, . . . ,L.
Let us now come to the single-particle Schrödinger equation for the rm Hamiltonian of Eq. 共12兲. In this equation the
variables are easily separable, and the problem is reduced to the solution of a radial differential equation. For the 2D 共3D
cylindrical兲 case, the rm eigenfunction in coordinate space is

e ⫺im ␸
␸ nm 共 r兲 ⫽R nm 共 r 兲 , 共A12兲
冑2 ␲
where R nm (r) is the solution of the radial Schrödinger equation
 91

PRB 59 COULOMB CORRELATION EFFECTS IN . . . 10 173

⳵ 2 R nm 共 r 兲
⳵r2
⫹
1 ⳵ R nm 共 r 兲
r ⳵r
⫹ k 2nm ⫺␭ 冋
˜ 2r 2⫺ ␣ c共 r 兲⫺
m2
r2
R nm 共 r 兲 ⫽0; 册 共A13兲

we have employed the notations ˜␭ ⫽ ␮ ␻ 0 /ប, ␣ ⫽2 ␮ e 2 / ␬ ប 2 , and k 2nm ⫽2 ␮⑀ nm /ប 2 , where ⑀ nm is the rm eigenvalue. The
effective Coulomb potential c(r) is simply 1/r in the 2D case, and it is defined in Sec. A 1 for the 3D cylindrical case.
For the 3D spherical case, the rm eigenfunction in coordinate space is

␸ nlm z 共 r兲 ⫽R nl 共 r 兲 Y lm z 共 ␽ , ␸ 兲 , 共A14兲

with R nl (r) satisfying the radial eigenvalue equation

⳵ 2 R nl 共 r 兲
⳵r 2
⫹
2 ⳵ R nl 共 r 兲
r ⳵r
⫹ k 2nl ⫺␭ 冋 ␣ l 共 l⫹1 兲
˜ 2r 2⫺ ⫺
r r2
R nl 共 r 兲 ⫽0; 册 共A15兲

where, again, we put k 2nl ⫽2 ␮⑀ nl /ប 2 , and ⑀ nl is the rm eigenvalue.

In order to obtain an exact solution for the rm eigenvalue problems, we rewrite Eqs. 共A13兲 and 共A15兲 in terms of the
dimensionless variable x⫽␭ ˜ 1/2r. For the 2D 共3D cylindrical兲 case, Eq. 共A13兲 becomes

d
dx
x冉dR̃ nm 共 x 兲
dx
⫹ ⫺
m2
x
冊冋
⫺ ˜␣ x C 共 x 兲 ⫹k̃ 2nm x⫺x 3 R̃ nm 共 x 兲 ⫽0, 册
R̃ nm 共 x 兲 ⫽R nm 共 r 兲 , 共A16兲

˜ ⫺1/2 c 共 ˜␭ ⫺1/2x 兲
C 共 x 兲 ⫽␭
关for the 2D case it is simply C(x)⫽1/x兴, while for the 3D case Eq. 共A15兲 transforms into

d 2˜␹ nl 共 x 兲
dx 2
⫹ ⫺ 冋 l 共 l⫹1 兲
x2
⫺
˜␣
x 册
⫹k̃ 2nl ⫺x 2 ˜␹ nl 共 x 兲 ⫽0,

共A17兲
R nl 共 r 兲
˜␹ nl 共 x 兲 ⫽ ␹ nl 共 r 兲 , ␹ nl 共 r 兲 ⫽ .
r

The dimensionless parameters are ˜␣ ⫽␭ ˜ ⫺1/2␣ ⫽2 冑R* /ប ␻ 0 and k̃ ␣2 ⫽k ␣2 /␭

˜ ⫽2 ⑀ ␣ /ប ␻ ;R* ⫽e 4 m * /2␬ 2 ប 2 is the effective
Rydberg energy. Actually, exact analytic solutions exist, but they are limited to 2D and 3D spherical cases only20,21; thus we
have chosen to solve Eqs. 共A16兲 and 共A17兲 by standard numerical methods. We stress that the numerical accuracy depends on
the accurate specification of the boundary conditions that we impose through analytical asymptotic formulas for eigenfunctions
near to the singular points 0 and ⫹⬁, following the general methods of Ref. 22. In this way the numerical solution is very
stable and efficient, thus overcoming possible difficulties related to the singlet ground state7; in our calculations energy values
are obtained with a nominal relative error of the order of 10⫺8 .

APPENDIX B: HELIUM PERTURBATION THEORY

We employ the standard Rayleigh-Schrödinger perturbation theory to correct the SSH eigenvalues in Eq. 共18兲 at the second
order in the off-diagonal Coulomb matrix elements entering the total Hamiltonian 共17兲. In the remaining part of this section we
shall consider the 2D and 3D spherical cases, by neglecting the center-of-mass motion.
For the 2D case, the rm SSH eigenvalues ⑀ SSH
nm are given by
10

nm ⫽ប ␻ 0 共 2n⫹ 兩 m 兩 ⫹1 兲 ⫹ 冑R* ប ␻ 0 S 共 n,m 兲 ,

⑀ SSH 共B1兲
2D

冉 冊
再 冎
1
⌫ 兩m兩⫹ n⫺1
2 n! 共 ⫺1 兲 s⫹1 关共 2s⫹1 兲 !! 兴 2 兩 m 兩 !
S 2D 共 n,m 兲 ⫽
兩m兩!
1⫹ 兺
s⫽0 共 n⫺s⫺1 兲 ! 2 2s⫹2 关共 s⫹1 兲 ! 兴 2 共 兩 m 兩 ⫹s⫹1 兲 !
, 共B2兲

while for the 3D case we have

⑀ SSH
nl ⫽ប ␻ 0 2n⫹l⫹ 冉 3
2 冊
⫹ 冑R* ប ␻ 0 S 3D 共 n,l 兲 , 共B3兲
92 The Importance of Electronic Correlation

10 174 RONTANI, ROSSI, MANGHI, AND MOLINARI PRB 59

冊再 冎
l! ⌫
1
2 冉冊
共 2l⫹1 兲 !! n⫺1
1
n! 共 ⫺1 兲 s⫹1 ⌫
2 冉冊
关共 2s⫹1 兲 !! 兴 2 共 2l⫹1 兲 !!
兺
冉 冉 冊
S 3D 共 n,l 兲 ⫽ 1⫹ . 共B4兲
3 s⫽0 5
2 l⫹1 ⌫ 2 l⫹ 2 s⫹l⫹3 共 n⫺s⫺1 兲 ! ⌫ s⫹l⫹ 关共 s⫹1 兲 ! 兴 2
2 2

The first-order correction due to nondiagonal Coulomb For the 3D case one obtains

冑
matrix elements is equal to zero. The second-order correction
⌬␧ (2)
0 to the ground-state energy is given by the well-known
expression
V n0 ⫽ 冑R* ប ␻ 0
冉 冊
⌫ 2 n⫹
1
2

冉 冊冉冊
,
3 3
兩 V 0n 兩 2 ␲ ⌫ 共 n⫹1 兲 ⌫ n⫹ ⌫
⌬␧ 共02 兲 ⫽ 兺n ␧ SSH⫺␧ SSH 共B5兲 2 2
0 n

关see the notation in Eq. 共17兲兴. The idea now is to look for 1 1
V n0 ⬇ 冑R* ប ␻ 0 共B7兲

冑 冉冊
analytic expressions for the off-diagonal integrals V 0n and , n→⬁.
then to perform a numerical summation. However, expres- 3 n 3/4
sions like those obtained in Eqs. 共B2兲–共B4兲 共Ref. 23兲 are not ␲⌫
useful, since each integral is given by an alternated-sign 2
summation, and numerical errors become rapidly critical as As already pointed out, now the generic terms 共B6兲 and 共B7兲
the quantum number n increases. In contrast, the solution can in the sum 共B5兲 have the same sign and the summation can
be obtained using an integration trick suggested in Ref. 24, be easily performed. The result for the 2D case is
so that all the terms in the summation are obtained with the
same sign. For the 2D case one obtains ⌬␧ 共02 兲 ⫽⫺R* 共 0.691兲 , 共B8兲

V n0 ⫽ 冑R* ប ␻ 0
1
冉 冊
⌫ n⫹
2
,
and for the 3D case it is

⌫ 共 n⫹1 兲 ⌬␧ 共02 兲 ⫽⫺R* 共 0.156兲 . 共B9兲

Note that the 3D term is significantly smaller than the corre-
1
V n0 ⬇ 冑R* ប ␻ 0 1/2
, n→⬁. 共B6兲 sponding 2D one, and that in the 3D case the series con-
n verges more quickly.

1
For recent reviews, see R. C. Ashoori, Nature 共London兲 379, 413 8
J. Hubbard, Proc. R. Soc. London, Ser. A 276, 238 共1963兲.
共1996兲; L. P. Kouwenhoven, C. M. Marcus, P. L. McEuen, S. 9
These are the so-called Roothaan equations: see, e.g., I. Levine,
Tarucha, R. M. Westervelt, and N. S. Wingreen, in Mesoscopic Quantum Chemistry 共Prentice-Hall, Englewood Cliffs, NJ,
Electron Transport, edited by L. L. Sohn, L. P. Kouwenhoven, 1991兲. For applications to 2D quantum dots, see Refs. 7 and 11.
and G. Schoen 共Kluwer, Dordrecht, 1997兲, p. 105. 10
U. Merkt, J. Huser, and M. Wagner, Phys. Rev. B 43, 7320
2
S. Tarucha, D. G. Austing, T. Honda, R. J. van der Hage, and L. 共1991兲.
P. Kouwenhoven, Phys. Rev. Lett. 77, 3613 共1996兲. 11
L. Wang, J. K. Zhang, and A. R. Bishop, Phys. Rev. Lett. 73, 585
3
M. Fricke, A. Lorke, J. P. Kotthaus, G. Medeiros-Ribeiro, and P. 共1994兲.
M. Petroff, Europhys. Lett. 36, 197 共1996兲. 12
A. Wójs and P. Hawrylak, Phys. Rev. B 53, 10 841 共1996兲.
4 13
For a recent review, see L. Jacak, P. Hawrylak, and A. Wójs, M. Koskinen, M. Manninen, and S. M. Reimann, Phys. Rev. Lett.
Quantum Dots 共Springer, Berlin, 1998兲; see also N. F. Johnson 79, 1389 共1997兲.
and M. Reina, J. Phys.: Condens. Matter 4, L623 共1992兲; J. J. 14
Since in these cases the energy balance defining the ground-state
Palacios, L. Martin-Moreno, G. Chiappe, E. Louis, and C. Teje- energy according to Eq. 共8兲 becomes very delicate, the depen-
dor, Phys. Rev. B 50, 5760 共1994兲, and references therein. dence of Coulomb and exchange integrals on the dot dimension-
5
M. Rontani, F. Rossi, F. Manghi, and E. Molinari, Appl. Phys. ality may give rise to different ground-state spin polarizations in
Lett. 72, 957 共1998兲. 2D and 3D QD’s.
6 15
A few examples of 3D calculations exist in the literature; see, A. Kumar, S. E. Laux, and F. Stern, Phys. Rev. B 42, 5166
e.g., Y. Tanaka and H. Akera, Phys. Rev. B 53, 3901 共1996兲; A. 共1990兲.
16
Wojs, P. Hawrylak, S. Fafard, and L. Jacak, ibid. 54, 5604 C. Steinebach, C. Schüller, G. Biese, D. Heitmann, and K. Eberl,
共1996兲; T. Ezaki, N. Mori, and C. Hamaguchi, ibid. 56, 6428 Phys. Rev. B 57, 1703 共1998兲.
共1997兲. 17
V. Fock, Z. Phys. 47, 446 共1928兲.
7
D. Pfannkuche, V. Gudmundsson, and P. A. Maksym, Phys. Rev. 18
S. Flügge, Practical Quantum Mechanics 共Springer-Verlag, Ber-
B 47, 2244 共1993兲. lin, 1971兲.
 93

PRB 59 COULOMB CORRELATION EFFECTS IN . . . 10 175

19
Handbook of Mathematical Functions, edited by M. Abramowitz 22
P. Moon and D. E. Spencer, Field Theory Handbook 共Springer-
and I. A. Stegun 共Dover, New York, 1972兲. Verlag, Berlin, 1961兲.
20
M. Taut, Phys. Rev. A 48, 3561 共1993兲.
23
A. Wójs and P. Hawrylak, Phys. Rev. B 51, 10 880 共1995兲; E.
21 Anisimovas and A. Matulis, J. Phys.: Condens. Matter 10, 601
M. Dineykhan and R. G. Nazmitdinov, Phys. Rev. B 55, 13 707
共1998兲.
共1997兲. This paper also considers different in-plane and orthogo- 24
M. Stone, H. W. Wyld, and R. L. Schult, Phys. Rev. B 45, 14 156
nal single-particle parabolic confinement potentials. 共1992兲.
94 The Importance of Electronic Correlation
Chapter 6

The Double-Dot Molecule

96 The Double-Dot Molecule
 97

PERGAMON Solid State Communications 112 (1999) 151–155

www.elsevier.com/locate/ssc

Multiple quantum phases in artificial double-dot molecules

M. Rontani a,b,*, F. Rossi a,b,c, F. Manghi a,b, E. Molinari a,b
a
Istituto Nazionale per la Fisica della Materia (INFM), I-41100 Modena, Italy
b
Dipartimento di Fisica, Università di Modena e Reggio Emilia, Via Campi 213/A, I-41100 Modena, Italy
c
Dipartimento di Fisica, Politecnico di Torino, Corso Duca degli Abruzzi 24, I-10129 Torino, Italy
Received 16 June 1999; accepted 18 June 1999 by M. Cardona

Abstract
We study coupled semiconductor quantum dots theoretically through a generalized Hubbard approach, where intra- and
inter-dot Coulomb correlation, as well as tunneling effects are described on the basis of realistic electron wavefunctions. We
find that the ground-state configuration of vertically coupled double dots undergoes non-trivial quantum transitions as a
function of the inter-dot distance d; at intermediate values of d we predict a new phase that should be observable in the
addition spectra and in the magnetization changes. 䉷 1999 Elsevier Science Ltd. All rights reserved.
Keywords: A. Nanostructures; D. Electron–electron interactions; D. Quantum localization

Semiconductor quantum dots (QDs) are nano- or meso- states of realistic double quantum dots (DQDs) using a
scopic structures that can be regarded as ‘artificial atoms’ theoretical scheme that fully takes into account intra-
because of the three-dimensional carrier confinement and and inter-dot many-body interactions. We focus on strongly
the resulting discrete energy spectrum. They are currently confined vertically coupled DQDs, and show that, for a
receiving great attention because they can be designed given number of electrons, N, the ground-state configura-
to study and exploit new physical phenomena: on the tion undergoes non-trivial quantum transitions as a func-
one hand, the nature and scale of electronic confinement tion of the inter-dot distance d; we identify specific ranges
allows the exploration of regimes that are not accessible of the DQD parameters characterizing a ‘coherent’ mol-
in conventional atomic physics; on the other, they lead to ecular phase, where tunneling effects dominate, and a
novel devices dominated by single- or few-electron effects phase where the inter-dot interaction is purely electro-
[1–3]. static. At intermediate values of d we predict a new
One of the important challenges at this point is to under- phase that should be observable by means of transport
stand the fundamental properties of coupled QDs, the experiments in the addition spectra and in the magnetization
simplest structures that display the interactions controlling changes.
potential quantum-computing devices. Here also the inter- From the theoretical point of view, a major difficulty is
dot coupling can be tuned through external parameters, far that we cannot make use of perturbative schemes [4,5] in the
out of the regimes known in ‘natural molecules’ where the calculation of the DQD many-body ground state, since we
ground-state interatomic distance is dictated by the nature of want to investigate all inter-dot coupling regimes. We thus
bonding. We expect that new phenomena will occur in these write the many-body hamiltonian H within a generalized
‘artificial molecules’ (AMs) when the relative importance of Hubbard (GHH) approach [6–11], 1 and choose a basis set
Coulomb interaction and single-particle tunneling is varied. formed by suitable single-particle wavefunctions localized
Through the study of such phenomena, coupled dots may on either dot (i ˆ 1; 2), and characterized by orbital
become a unique laboratory to explore electronic correla- quantum numbers, a (to be specified later), and by the
tions. spin quantum number, s . On this basis the many-body
In this paper we analyze ground and excited few-particle
1
Hubbard-like hamiltonians for QDs are also used—with differ-
* Corresponding author. ent levels of approximations—in Refs. [6–11].
0038-1098/99/$ - see front matter 䉷 1999 Elsevier Science Ltd. All rights reserved.
PII: S0038-109 8(99)00305-1
98 The Double-Dot Molecule

152 M. Rontani et al. / Solid State Communications 112 (1999) 151–155

hamiltonian is
X X † 1 X
H^ ˆ 1~ a n^ias ⫺ t c^ias c^jas ⫹ U n^ n^
ias as具ij典
2 iabs ab ias ib⫺s

1 X X
⫹ U ⫺ Jab †n^ias n^ibs ⫹ U~ ab n^ 1as n^2bs 0 :
2 iabs ab abss 0

The first two addenda are the single-particle on-site and

hopping term, respectively: 1~ a are the single-particle ener-
gies, t the tunneling parameter; n^ the occupation numbers
and c^ (c^† ) are the creation (destruction) operators. The third
and fourth terms account for intra-dot Coulomb interaction
between electrons with antiparallel and parallel spins,
respectively; U and J are the intra-dot Coulomb and
exchange integrals. Finally, the last term represents the
inter-dot Coulomb coupling, Ũ being the inter-dot Coulomb
integrals. These integrals are in turn expressed in terms of
Fig. 1. Parameters entering the many-body hamiltonian of a double single-particle states:
quantum dot with បv ˆ 10 meV, plotted as a function of the inter-
Z e2 兩f r†兩2 兩f r 0 †兩2
ia ib
dot distance d. The hopping coefficient t is shown together with two
Uab ˆ dr dr 0 ;
of the intra-dot and inter-dot Coulomb integrals. In the inset, the top kr 兩r ⫺ r 0 兩
panel shows the confinement potential V z† (the barrier height is
200 meV) and the corresponding symmetric and antisymmetric Z e2 兩f r†兩2 兩f r 0 †兩2
1a 2b
single-particle wavefunctions, 兩s典 and 兩a典; the bottom panel displays U~ ab ˆ dr dr 0 ;
the localized states, 兩1典 and 兩2典, obtained as combinations of 兩s典 and kr 兩r ⫺ r 0 兩
兩a典, that are used as basis set for our calculation.
Z e2 fⴱ r†fⴱ r 0 †f r 0 †f r†
1a ib ia ib
Jab ˆ dr dr 0 ;
kr 兩r ⫺ r 0 兩
with f ia (r) the full three-dimensional single-particle wave-
functions (obtained within the usual envelope-function
approximation), e the electronic charge and k r the relative
dielectric constant.
Here we shall consider a specific type of nanostructures,
namely vertically coupled cylindrical DQDs [12]; the ingre-
dients entering the hamiltonian can therefore be defined
explicitly. For simplicity, V(r) can be assumed to be separ-
able in the xy and z components; the profile is taken to be
parabolic in the xy-plane, with confinement energy បv , and
a symmetric double quantum well (QW) along z [12,13].
The eigenstates of the xy harmonic potential are the usual
Fock–Darwin states 兩a典 ˆ 兩 n; m†典 (n, m being the radial and
angular quantum numbers) [3]. Along z, the QW thickness is
such that only the lowest eigenstates (symmetric, 兩s典, and
antisymmetric 兩a典) are relevant for the low-energy spectrum.
From these, we construct a complete set of states that are
localized p p of Fig. 1): 兩1典 ˆ
on either dot (see inset
兩s典 ⫹ 兩a典†= 2 and 兩2典 ˆ 兩s典 ⫺ 兩a典†= 2. The basis we use is
therefore the direct product 兩ias典 ˆ 兩i典 丢 兩a典 丢 兩s典. The
Fig. 2. Energies of the ground state (thick line) and three lowest single-particle energies are 1~ a ˆ 1a ⫹ es ⫹ ea †=2, and the
excited states (thin lines) as a function of the inter-dot distance, d,
tunneling parameter is t ˆ ea ⫺ es †=2, with e s, e a double-
for a double QD occupied by N electrons. For N ˆ 4, the prominent
single particle configurations contributing to the many-body ground
well eigenenergies, and 1 a oscillator energies.
state are shown in the insets. Note that in the intermediate phase a Using the above expressions, the three-dimensional
significant contribution comes also from other Slater determinants Coulomb integrals and the tunneling parameter are
(see text). The p molecular states are doubly degenerate because of computed directly from the single-particle states for each
the two-fold degeneracy of the second shell in the single-dots sample. Fig. 1 shows the result for t, Ua b and U~ ab ‰a ˆ b ˆ
px ; py †: 0; 0†Š calculated for a In0.05Ga0.95As DQD (kr ˆ 12:98,
 99

M. Rontani et al. / Solid State Communications 112 (1999) 151–155 153

transition occurs, below which the new ground state is a

molecular-like state. For N ⬎ 3, two successive transitions
take place, at d ˆ db and d ˆ da and an intermediate non-
trivial phase is predicted to occur in the range d ⬍ da ⬍ db
Note that this phase is stable in a relatively large range of d
values, which depends on the number of electrons. An accu-
rate determination of da and db requires the correct inclusion
of all inter-dot coupling terms, including the inter-dot
Coulomb integrals. If the latter are neglected, all quantum
transitions occur for smaller values of the inter-dot distance,
and the d-range of the intermediate phase is underestimated
Fig. 3. Electronic pair correlation functions for a double QD with significantly; had also the other many-body terms been
N ˆ 6 electrons, calculated at three values of the inter-dot distance, neglected, the intermediate phase would disappear leaving
d, corresponding to the different quantum phases. The maps are a simple crossover from a molecular to an atomic-like
plotted as a function of the difference between the in-plane coordi- regime at d ˆ da ˆ db .
nates of the electrons in the pair x ˆ x 0 ⫺ x 00 and y ˆ y 0 ⫺ y 00 †; To understand the nature of the different phases it is
while their z coordinates are fixed either at the center of the same
useful to examine the many-body states in terms of the
dot [g#;# x; y; z1 ; z1 †; upper panels] or at the center of different dots
single Slater determinants that contribute to each of them.
[g#;# x; y; z1 ; z2 †; lower panels]. Here # represents the minority spins.
Here we discuss explicitly the 4-electron case with the help
of the insets in Fig. 2, but the same reasoning can be
effective mass 0.065me) with បv ˆ 10 meV, as a function of followed for the other cases. Both in the case of very
the inter-dot distance (barrier width) d. Note that already small and very large inter-dot distances the ground state
around d ˆ 5 nm the inter-dot Coulomb integral exceeds can be essentially described in terms of a single Slater deter-
the single-particle hopping parameter. minant: for large values of d (d ⬎ db ), the relevant config-
To obtain the many-body energies and eigenstates, the urations for the ground state have two electrons in the lowest
hamiltonian H^ is then diagonalized exactly for each value level of each isolated dot; the 兩s典 and 兩a典 extended ‘molecu-
of N (total number of electrons) on each configuration lar’ orbitals derived from the lowest ‘atomic’ states are of
subspace labeled by the quantum numbers S (z-component course almost degenerate and both filled with two electrons.
of the total spin) and M (z-component of the total orbital In the opposite limit (d ⬍ da ), by expanding the localized
angular momentum). atomic orbitals in terms of molecular orbitals we recognize
This approach has two main advantages: first, it allows us that the 兩s典 state derived from the lowest atomic state is filled
to solve the many-body problem consistently in the different with two electrons, while the corresponding 兩a典 molecular
coupling regimes, from the limit where t dominates over the state is empty. The two remaining electrons occupy the next
Coulomb integrals to the opposite limit where t is negligible. bonding molecular orbitals—derived from the higher px and
Second, it can provide quantitative predictions for given py levels—with parallel spin, in such a way that S is maxi-
DQD structures, since it contains no free parameters and mized. This is the manifestation of Coulomb interaction,
uses realistic ingredients t; Uab ; U~ ab ; Jab † calculated for which leads to Hund’s rule for molecules.
each nanostructure [14,15]. 2 In these two extreme phases the single particle picture is
Fig. 2 shows the calculated ground-state energies EN of essentially correct, provided that the appropriate basis set
correlated N-particle states as a function of the inter-dot (either localized or extended orbitals) is used. In the inter-
distance d. 3 The three lowest excited states are also shown mediate phases da ⬍ d ⬍ db , this is no longer true and the
for comparison. As expected, when d is large, the system ground state is a mixture of different Slater determinants in
behaves as two isolated QDs. With decreasing d, some of the any basis set [16]. In this sense again the intermediate phase
many-body excited states, favored by Coulomb interactions, exhibits an intrinsic many-body character. Coulomb direct
become lower in energy. For N ˆ 3 a single quantum phase and exchange terms, responsible for the selection of the
global quantum numbers, determine a new ground-state
configuration, where both S and M are maximized.
2
The same approach was introduced for the case of isolated QDs We obtain a clear evidence of the different electronic
giving addition spectra in good agreement with experiments distribution in the three quantum phases by calculating the
[14,15]. In that case, however, the Hubbard hamiltonian reduces spin-dependent electronic pair correlation function, defined
to an effective one-body hamiltonian since t and the inter-dot inte-
as
grals are zero.
3
Ground-state configurations are labeled in the molecular nota- Z
tion: S, P, D, F, G, I correspond to M ˆ 0; …; 5; the left superscript gs 0 ;s 00 r; z 0 ; z 00 † ˆ dR具C^ †s 0 r 0 †C^ †s 00 r 00 †C^ s 00 r 00 †C^ s 0 r 0 †典;
is 2S ⫹ 1; g and u specify the symmetry under inversion with
respect to the center of the molecule; ⫹ and ⫺ the symmetry where R ˆ r 0 ⫹ r 00 †=2 and r ˆ r 0 ⫺ r 00 †. Here r 0 ˆ
under the z ! ⫺z reflection. x 0 ; y 0 †; r 00 ˆ x 00 ; y 00 † are the in-plane spatial coordinates
100 The Double-Dot Molecule

154 M. Rontani et al. / Solid State Communications 112 (1999) 151–155

shown in the left, central, and right panels is representative

of the three phases. Secondly, the changes in the magnetiza-
tion induced by one electron addition—also accessible
experimentally [18]—are expected to follow a different
pattern in each phase (see the different sequence of quantum
numbers in Fig. 2).
A large experimental effort is presently devoted to trans-
port experiments in double QDs. In most cases, the dots are
obtained by gating a two-dimensional electron gas (lateral
confinement), and their coupling can be tuned through a gate
voltage [18–22]. Indeed, a set of experiments has recently
demonstrated a clear transition to a ‘coherent’ state with
increasing coupling between dots [20,22]. Outside this
strong coupling regime, however, experiments performed
in the lateral geometry have so far evidenced classical
inter-dot capacitance effects, probably owing to the size of
Fig. 4. Calculated addition spectra, A N† ˆ E N† ⫺ E N ⫺ 1†, as a dots. 4 On the other hand, transport experiments are now
function of magnetic field B for a double QD, calculated at three available on DQD structures with strong lateral confinement
values of the inter-dot distance, d, corresponding to the different fabricated by combined growth and etching techniques. 5
quantum phases. Labels indicate the ground-state configuration of The advantage is that the number of electrons in the struc-
the N-electron system. The energy zero is arbitrary. ture is limited, while an accurate control on the inter-dot
coupling is still possible by designing samples with appro-
of the electrons in the pair, and z 0 and z 00 are their coordi- priate barrier thickness. Both aspects are important to
nates along z, that will be kept fixed at the center of either enhance many-body effects and to explore intermediate
QD, i.e. in z1 or z2. r 0 ˆ r 0 ; z 0 †; r 00 ˆ r 00 ; z 00 †: s 0 ; s 00 are the coupling regimes. Recent experimental work on these struc-
spin variables and can assume the values " or # . In Fig. 3 tures has focused on the weak-coupling regimes [12]. We
we plot for example g#;# x; y; z 0 ; z 00 † for a double QD with hope that further investigations will be stimulated by the
N ˆ 6 electrons, at three values of the inter-dot distance present work, since the relevant transitions are now
corresponding to different quantum phases. Here # repre- predicted quantitatively and should occur in a range of para-
sents the minority spins. For d ⬍ da (left column), it is meters that is accessible to state-of-the-art experiments. We
indeed apparent that the pair correlation function is the expect that such studies will bring new insight into elec-
same when both electrons are in the same dot tron–electron interaction effects in coupled quantum nanos-
[z 0 ˆ z 00 ˆ z1 , panel (a)] or on different dots[z 0 ˆ z1 and tructures.
z 00 ˆ z2 , panel (b)]. In this sense, the system behaves ‘coher-
ently’. For d ⬎ db (right column), the maps indicate that the
probability of finding two # -electrons in the same dot is Acknowledgements
negligible, consistently with the picture of isolated dots. In
the intermediate phase da ⬍ d ⬍ db this is no longer the We acknowledge helpful discussions with C. Calandra
case: the electronic wavefunctions extend over both dots, and G. Goldoni. This work was supported in part by
and the g#;# pair correlation functions are very different INFM PRA99-SSQI, by the EC under the TMR Network
depending on the location of both electrons in the same or ‘Ultrafast Quantum Optoelectronics’, and by the MURST-
in different dots. Note that transitions between different 40% program ‘Physics of Nanostructures’.
electronic configurations vs. d were recently identified theo-
retically also for classical coupled dots [17]: we find that, for
the small values of N considered here, the number of distinct References
phases and the spatial distribution of electrons (as reflected
in their correlation functions) is drastically modified by [1] R.C. Ashoori, Nature 379 (1996) 413.
quantum effects. [2] L.P. Kouwenhoven et al., in: L. Sohn et al. (Eds.), Mesoscopic
Electron Transport, Kluwer Academic Publishers, Dordrecht,
The above findings are expected to be observable experi-
1997 and references therein.
mentally. First, the calculated magnetic-field dependent
addition spectra A N† present clear signatures of the phase 4
Interesting deviations from predictions of simple capacitance
transitions described above, as illustrated in Fig. 4. Here
models are however reported in Refs. [18,19].
A N† ˆ E N† ⫺ E N ⫺ 1† is obtained from the many-body 5
DQD with different geometries, obtained by cleaved-edge or
ground-state energies of the N- and (N ⫺ 1)-electron self-organized growth, have recently become available but were
systems, on the basis of single-particle states calculated in so far investigated mostly by optical experiments. See, e.g. Refs.
the presence of the external magnetic field B. The behavior [23–25].
 101

M. Rontani et al. / Solid State Communications 112 (1999) 151–155 155

[3] L. Jacak, P. Hawrylak, A. Wójs, Quantum Dots, Springer, [14] M. Rontani, F. Rossi, F. Manghi, E. Molinari, Appl. Phys.
Berlin, 1998. Lett. 72 (1998) 957.
[4] K.A. Matveev et al., Phys. Rev. B 53 (1996) 1034. [15] M. Rontani, F. Rossi, F. Manghi, E. Molinari, Phys. Rev. B 59
[5] J.M. Golden, B.I. Halperin, Phys. Rev. B 56 (1996) 4716. (1999) 10165.
[6] G.W. Bryant, Phys. Rev. B 48 (1993) 8024. [16] M. Eto, Solid State Electron. 42 (1998) 1373.
[7] G. Klimeck et al., Phys. Rev. B 50 (1994) 2316. [17] B. Partoens et al., Phys. Rev. Lett. 79 (1997) 3990.
[8] J.J. Palacios et al., Phys. Rev. B 51 (1995) 1769. [18] T.H. Oosterkamp et al., Phys. Rev. Lett. 80 (1998) 4951.
[9] R. Kotlyar, S. Das Sarma, Phys. Rev. B 56 (1997) 13235. [19] F.R. Waugh et al., Phys. Rev. Lett. 75 (1995) 705.
[10] Y. Asano, Phys. Rev. B 58 (1998) 1414. [20] C. Livermore et al., Science 274 (1996) 1332.
[11] Y. Tokura et al., in: D. Gershoni, et al. (Eds.), Proceedings of [21] T.H. Wang, S. Tarucha, Appl. Phys. Lett. 71 (1997) 2499.
the 24th International Conference on the Physics of Semicon- [22] R.H. Blick et al., Phys. Rev. Lett. 80 (1998) 4032.
ductors, World Scientific, Singapore, 1999, in press. [23] G. Schedelbeck et al., Science 278 (1997) 1792.
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102 The Double-Dot Molecule

The paper below appears in 1999 Spring Meeting MRS Symposium W Proceed-
ings: Semiconductor Quantum Dots, Mat. Res. Soc. Symp. Proc. Vol. 571, in
press. It clarifies the role of electronic correlation by comparing the results for
the full generalized Hubbard hamiltonian with those for the non-interacting case.
Moreover, it contains a physical discussion of the strongly correlated states of the
“intermediate phase” presented in the previous paper.
 103

THEORY OF ADDITION SPECTRA IN DOUBLE QUANTUM DOTS:

SINGLE-PARTICLE TUNNELING VS COULOMB INTERACTIONS
M. RONTANI , F. ROSSI  , F. MANGHI , E. MOLINARI

Istituto Nazionale per la Fisica della Materia and Dipartimento di Fisica, Universita degli
Studi di Modena e Reggio Emilia, Via Campi 213/a, 41100 Modena, Italy

present address: Dipartimento di Fisica, Politecnico di Torino, Corso Duca degli Abruzzi
24, 10129 Torino, Italy

ABSTRACT
We study coupled semiconductor quantum dots theoretically using a generalized Hub-
bard approach, where intra- and inter-dot Coulomb correlation, as well as tunneling e ects
are described on the basis of realistic electron wavefunctions. We nd that the ground-state
con guration of vertically coupled double dots undergoes non-trivial quantum transitions
as the inter-dot distance d changes; at intermediate values of d we predict a new phase
that should be observable in the addition spectra and in the magnetization changes.
INTRODUCTION
Semiconductor quantum dots (QDs) are nano- or mesoscopic structures that can be
regarded as `arti cial atoms' because of the three-dimensional carrier con nement and the
resulting discrete energy spectrum. They have currently received much attention because
they can be designed to study and exploit new physical phenomena: On the one hand, the
nature and scale of electronic con nement allows the exploration of regimes inaccessible in
conventional atomic physics; on the other hand, they lead to novel devices where single-
or few-electron e ects are important[1].
One of the important challenges at this point is to understand the fundamental prop-
erties of coupled quantum dots, the simplest structures that manifest the interactions
controlling potential quantum-computing devices. Here also the interdot coupling can be
tuned through external parameters, far from the regimes known in `natural molecules'
where the ground-state interatomic distance is dictated by the bonding. We expect to
see new phenomena in these `arti cial molecules' (AMs) when the relative importance of
Coulomb interaction and single-particle tunneling is varied. Through the study of such
phenomena, coupled dots may become a unique laboratory enabling one to understand the
role of correlations better.
In this paper we analyze ground and excited few-particle states of realistic double
quantum dots (DQDs) using a theoretical scheme that fully takes into account intra- and
inter-dot many-body interactions. We focus on strongly con ned vertically-coupled DQDs
in the zero- or low-magnetic eld regime; this subject is relatively unexplored[2]. We show
that, for a given number of electrons, N ( 6), the ground state con guration undergoes
non-trivial quantum transitions as the inter-dot distance d changes; we identify speci c
ranges of the DQD parameters characterizing a `coherent' molecular phase, where tunnel-
ing e ects dominate, and a phase where the inter-dot interaction is purely electrostatic.
At intermediate values of d we predict a new phase that should be observable by per-
forming transport experiments and observing changes in the addition spectra and in the
magnetization.
104 The Double-Dot Molecule

THEORY
In our calculations, we cannot make use of perturbative or single-particle schemes in
the calculation of the DQD many-body ground state, since we want to investigate all inter-
dot coupling regimes. We thus write the many-body hamiltonian H within a generalized
Hubbard (GHH) approach [3], and choose a basis set formed by suitable single-particle
wavefunctions localized on either dot (i = 1; 2), and characterized by orbital quantum
numbers, (to be speci ed below), and by the spin quantum number, . In this basis the
many-body hamiltonian is
H^ =
X "~ n^i  ; t
X X
c^yi  c^j  + 21 U n^i  n^i ; +
i 
X hij i

+ 1 (U ; J ) n^i  n^i  +
X i 

U~ n^1  n^2  : (1)

2i 
0

0


The rst two terms are the single-particle on-site and hopping term respectively: "~ are
the single-particle energies, t the tunneling parameter; n^ are the occupation numbers and c^
(c^y) the creation (destruction) operators. The third and fourth terms account for intra-dot
Coulomb interaction between electrons with antiparallel and parallel spins, respectively: U
and J are the intra-dot Coulomb and exchange integrals. Finally, the last term represents
the inter-dot Coulomb coupling, U~ being the inter-dot Coulomb integrals. These integrals
are in turn expressed in terms of single-particle states:
2 Z
U = e ji(rj)rj;jri0 j(r )j dr dr0;
2 0 2
(2)
r

U~
Z
= e j
2
(r)j2 j2 (r0 )j2 dr dr0;
1
(3)
r jr ; r0j
Z 2   0 0
J = e i (r) i j(rr ;) ri0j (r ) i (r) dr dr0; (4)
r
where i (r) are the full three-dimensional single-particle wavefunctions (obtained within
the usual envelope-function approximation), and r is the relative dielectric constant.
Here we shall consider a speci c type of nanostructure, namely vertically coupled cylin-
drical DQDs [4]; the contributions to the Hamiltonian can therefore be de ned explic-
itly. For simplicity, the single-particle con ning potential V (r) can be written in the form
V (r) = 1=2 m! (x2 + y2) + V0(z), where V0(z) is a symmetric double quantum well (QW)
and m is the e ective electronic mass[4]. We write the eigenstates of the two dimensional
harmonic oscillator in the usual Fock-Darwin form, j i = j(n; m)i where n, m are the
radial and angular quantum numbers[1]. Along z, the QW thickness is such that only the
lowest eigenstates (symmetric, jsi, and antisymmetric jai) are relevant for the low-energy
spectrum. From these, pwe construct a complete set p of states that are localized on either
dot: j1i = (jsi + jai) = 2 and j2i = (jsi ; jai) = 2. The basis we use is therefore the
direct product ji i = jii j i ji. The single-particle energies are "~ = " +(s + a)=2,
and the tunneling parameter is t = (a ; s )=2, with s, a double-well eigenenergies, and "
oscillator energies. Using the above expressions, the three-dimensional Coulomb integrals
and the tunneling parameter are computed directly from the single-particle states for each
sample.
 105

To obtain the many-body energies and eigenstates, the Hamiltonian H^ is then diagonal-
ized exactly for each value of N (total number of electrons) on each con guration subspace
labeled by the quantum numbers S (z-component of the total spin) and M (z-component
of the total angular momentum).
This approach has two main advantages: First, it allows us to solve the many-body
problem consistently in the di erent coupling regimes, from the limit where t is much
greater then the Coulomb integrals to the opposite limit where t is negligible. Second, it can
provide quantitative predictions for given DQD structures, since it contains no free param-
eters and uses realistic values of t, U , U~ , and J calculated for each nanostructure[5].
RESULTS AND DISCUSSION
Fig. 1(b) shows the calculated ground-state energies of correlated N -particle states as
a function of the inter-dot distance (barrier width) d. The three lowest excited states are
also shown for comparison. As expected, when d is large, the system behaves as two iso-
lated QDs. With decreasing d, some of the many-body excited states, favored by Coulomb
interactions, become lower in energy. For N  3 a single quantum phase transition occurs,
below which the new ground state is a molecular-like state. For N > 3, two successive
transitions take place, at d = db and d = da, and an intermediate non-trivial phase is
predicted to occur in the range da < d < db. Note that this phase is stable in a relatively
large range of d values, which depends on the number of electrons. An accurate determi-
nation of da and db requires the correct inclusion of all inter-dot coupling terms, including
the inter-dot Coulomb integrals. If the latter are neglected, all quantum transitions occur
for smaller values of the inter-dot distance, and the d-range of the intermediate phase is
underestimated signi cantly. If we completely neglect all the many-body terms in eq. (1),
we obtain the ground state con gurations shown in g. 1(a). Here the intermediate phase
disappears, and for 3  N  6 we have a simple crossover between single Slater determi-
nants, at d = da = db. This proves that the appearance of the intermediate phase is an
intrinsic correlation phenomenon.
To understand the nature of the di erent phases it is useful to examine the many-body
states in terms of the single Slater determinants that contribute to each of them. However,
one should remember that, even if a single con guration is a good approximation for the
ground state wavefunction when d is very small (LCAO-like) or large (Heitler-London-like),
this is not the case when d has an intermediate value[6]. Here we discuss explicitly the
4-electron case with the help of Fig. 2, but the same reasoning can be used for the other
cases. For large values of d (d > db), the relevant con gurations for the ground state have
two electrons in the lowest level of each isolated dot; the jsi and jai extended `molecular'
orbitals derived from the lowest `atomic' states are of course almost degenerate and both
lled with two electrons. In the opposite limit (d < da ), by expanding the localized atomic
orbitals in terms of molecular orbitals we recognize that the jsi state derived from the
lowest atomic state is lled with two electrons, while the corresponding jai molecular state
is empty. The two remaining electrons occupy the next bonding molecular orbitals |
derived from the higher px and py levels| with parallel spin, in such a way that S is
maximized. This is the manifestation of Coulomb interaction which leads to Hund's rule
for molecules. In the intermediate phase, da < d < db, the jai molecular state of the
lowest shell is nearly degenerate with the jsi molecular state of the second shell, so the
available states are di erent from the previous case. Coulomb direct and exchange terms,
106 The Double-Dot Molecule

761
656 N=6 (a) N=6 (b)
M=0 S=1 754 M=1 M=0 S=1
S=1
646 no correlation 747
M=0 S=0 M=0 S=0 full GHH
636 740
544 N=5 611 N=5
M=0 M=1
S=3/2 S=1/2
M=1 S=1/2
energies (meV)

534 603
M=1 S=1/2 M=1
S=1/2
524 595
N=4 N=4
431 472
M=1
S=1 M=0
M=0 S=0 S=0
423 466
M=0
M=0 S=1 S=1
415 460
N=3 N=3
322 342

M=0 S=1/2 M=0 S=1/2

314 336
ground state M=1 ground state
M=1 S=1/2
S=1/2 three lowest excited states three lowest excited states
306 330
5 6 7 8 9 10 5 6 7 8 9 10
inter-dot distance d (nm) inter-dot distance d (nm)

Figure 1: Energies of the ground state (thick line) and three lowest excited states (thin
lines) as a function of the inter-dot distance, d, for a double QD occupied by N electrons.
The total spin S and orbital angular momentum M are shown for every con guration.
The con nement energy h ! is 10 meV, the inter-dot barrier height is 200 meV (the width
of both wells is 4 nm), r = 12:98, and m = 0:065me. Panel (a): ground states of the
single-particle hamiltonian. Panel (b): ground states of the full GHH.

responsible for the selection of the global quantum numbers, therefore determine a new
ground state con guration characterized by a partial occupation of both these molecular
states, which maximizes S and M .
The above ndings are expected to be experimentally observable. First, the calculated
magnetic- eld dependent addition spectra present clear signatures of the phase transitions
described above, as it will be shown elsewhere. Secondly, the changes in the magnetization
brought about by the addition of one electron |also experimentally accessible [7]| are
expected to follow a di erent pattern in each phase (see the di erent sequence of quantum
numbers in Fig. 1(b)).
CONCLUSIONS
A large experimental e ort is presently devoted to transport experiments in double
QDs. In most cases, the dots are obtained by gating a two-dimensional electron gas
(lateral con nement), and their coupling can be tuned through a gate voltage [7, 8, 9,
10, 11]. Indeed, a set of experiments has recently shown that there is a clear transition to a
`coherent' state with increasing coupling between dots [9, 11]. Outside this strong coupling
 107

N =4
\coherent" intermediate isolated
molecular phase dots
state
πg πg πg
energy (a.u.)

πu t πu πu
σu σu σu
σg σg σg

d =5 nm d =7 nm d =9 nm
S=1 M =0 S=1 M =1 S=0 M =0

Figure 2: For N = 4, the prominent Slater determinants contributing to the many-body

ground state are shown, for di erent values of the inter-dot distance d. Molecular orbitals
are labeled according to the following notation: ,  stay for m = 0; 1, u; g subscripts
denote the symmetry under inversion (x; y; z) ! (;x; ;y; ;z). Note that the  molecular
states are doubly degenerate because of the two-fold degeneracy of the second shell in the
single-dots (px; py ).

regime, however, experiments performed in the lateral geometry have so far evidenced
classical interdot capacitance e ects, probably owing to the size of the dots[12]. On the
other hand, transport experiments are now available on DQD structures with strong lateral
con nement fabricated by combined growth and etching techniques [4, 13]. The advantage
is that the number of electrons in the structure is limited, while an accurate control on the
inter-dot coupling is still possible by designing samples with appropriate barrier thickness.
Both aspects are important for enhancing many-body e ects and for exploring intermediate
coupling regimes. Recent experimental work on these structures has focused on the weak-
or strong- coupling regimes [4]. We hope that the present work will stimulate further
investigations, since the precise locations of the relevant transitions are now predicted
quantitatively and such transitions should occur in a range of parameters that is accessible
to state-of-the-art experiments. We expect that such studies will bring new insight into
electron-electron interaction e ects in coupled quantum nanostructures.
ACKNOWLEDGMENTS
We acknowledge helpful discussions with C. Calandra and G. Goldoni. This work was
supported in part by the EC under the TMR Network \Ultrafast Quantum Optoelectron-
ics", and by the MURST-40% program \Physics of Nanostructures".
108 The Double-Dot Molecule

REFERENCES
1. L. Jacak, P. Hawrylak, and A. Wojs, Quantum Dots (Springer, Berlin, 1998).
2. In J.J. Palacios and P. Hawrylak, Phys. Rev. B 51, 1769 (1995) the high magnetic
eld regime is investigated; in Y. Asano, Phys. Rev. B 58, 1414 (1998) the con gu-
rations with N > 12 are studied within a `core' approximation that could fail when
the coupling between dots is strong; H. Tamura, Physica B 249-251 210 (1998) is
a Hartree-Fock study, and Y. Tokura et al., Proc. 24th Internat. Conference on the
Physics of Semiconductors, edited by D. Gershoni, World Scienti c (1999), to be pub-
lished, is an exact diagonalization study for N  5.
3. Hubbard-like hamiltonians for QDs are also used in G.W. Bryant, Phys. Rev. B 48,
8024 (1993); G. Klimeck, G. Chen, and S. Datta, Phys. Rev. B 50, 2316 (1994);
R. Kotlyar and S. Das Sarma, Phys. Rev. B 56, 13235 (1997).
4. D.G. Austing, T. Honda, and S. Tarucha, Jpn. J. Appl. Phys. 36, 1667 (1997);
D.G. Austing, T. Honda, K. Muraki, Y. Tokura, S. Tarucha, Physica B 249-251,
206 (1998).
5. The same approach was introduced for the case of isolated QDs giving addition spectra
in good agreement with experiments [M. Rontani, F. Rossi, F. Manghi, and E. Molinari,
Appl. Phys. Lett. 72, 957 (1998); Phys. Rev. B 59, 10165 (1999)]. In that case, however,
the Hubbard hamiltonian reduces to an e ective one-body hamiltonian since t and the
inter-dot integrals are zero.
6. M. Eto, Solid-State Electronics 42, 1373 (1998).
7. T.H. Oosterkamp, S.F. Godijn, M.J. Uilenreef, Y.V. Nazarov, N.C. van der Vaart,
L.P. Kouwenhoven, Phys. Rev. Lett. 80, 4951 (1998).
8. F.R. Waugh, M.J. Berry, D.J. Mar, R.M. Westervelt, K.L. Campman, A.C. Gossard,
Phys. Rev. Lett. 75, 705 (1995).
9. C. Livermore, C.H. Crouch, R.M. Westervelt, K.L. Campman, A.C. Gossard, Science
274, 1332 (1996).

10. T.H. Wang and S. Tarucha, Appl. Phys. Lett. 71, 2499 (1997).
11. R.H. Blick, D. Pfannkuche, R.J. Haug, K. von Klitzing, K. Eberl, Phys. Rev. Lett. 80,
4032 (1998).
12. Interesting deviations from predictions of simple capacitance models are however re-
ported in Refs. [7, 8].
13. DQDs with di erent geometries, obtained by cleaved-edge or self-organized growth,
have recently become available but were so far investigated mostly by optical exper-
iments. See e.g. G. Schedelbeck, W. Wegscheider, M. Bichler, G. Abstreiter, Science
278, 1792 (1997); N.N. Ledentsov et al., Phys. Rev. B 54, 8743 (1996); R. Cingolani
et al. (1999), unpublished.
Conclusions 109

We considered the electronic structure of semiconductor vertical quantum dots.

These state-of-the-art devices are a unique paradigm for a strongly correlated
system where practically all parameters can be varied in a controlled way, and
therefore display an exceptionally large phase diagram of different kinds of
ground states. We limited our investigation to regimes of low magnetic field
and spatial confinement strong enough to make the electronic atom-like shell
structure experimentally observable.
Our first result was the explanation of some very intriguing features of mea-
sured addition spectra like open-shell spontaneous spin polarization, exchange
effects, Hund’s rule, and electron term intersections in presence of an exter-
nal magnetic field. The Generalized Hubbard Hamiltonian allowed for a very
clear and physical picture of correlation effects, which are responsible for the
global behavior of the system.
We checked also very accurately the role of the device geometry on open-shell
effects. A related methodological issue which was investigated is the reliabil-
ity of different possible approaches with regards to the correct treatment of
correlation.
The double-dot system presents an even more rich phenomenology. We gave
theoretical predictions of how electron terms depend on the inter-dot coupling
and B . Non-trivial kinds of ground states were found with no analogue in
“natural” molecules, and changes in the spontaneous magnetization at zero
field were expected. Some preliminary experimental findings seem to confirm
our results.
What emerges from our work is the great variety of different manifestations
of the competition between confinement and correlation: if, on one hand, QDs
presents many similarities with natural systems, on the other they can real-
ize completely new physical states. In relation to this, the potential for new
technological applications is enormous.
Maybe the most exciting aspect of this Thesis is the huge work still to be done
in this field, both experimental and theoretical. Some extensions are obvious
(more electrons, higher values of B ), some are not. The phase space still to
explore is truly vast.
110 Conclusions
Appendix A

Second Quantization

In this Appendix we introduce the Second Quantization formalism and ac-

cording to this we write down a generic many-body Hamiltonian H.

We assume a quite general expression for the Hamiltonian H of electrons in QDs:

H = H (1) + V (2); (A.1)

where
Ne
X
H (1) = h(1) (ri; si) ; (A.2)
i=1
and
V (2) =
1 X e 2
:
2 i6=j r jri ; rj j
(A.3)

r
The operator h(1) ( i ; si ) is a general one-particle Hamiltonian, acting on both
space and spin coordinates. The meaning of all other symbols is the same that
in Chapter 2. Our goal is to change the representation of the Hermitian operator
H, from the coordinate representation of Eqs. (A.2) and (A.3), to a new represen-
tation in the so called Fock space. In this new space the Hamiltonian is given by
products of Fermionic operators and the Hilbert space is built up by successive
applications of creation operators on the vacuum (occupation number representa-
tion).
112 Second Quantization

To start we introduce a Fermi Field operator (r; s):

X
(r; s) = '  (r; s) c  : (A.4)

r
Here f'  ( ; s)g  is a complete and orthonormal set of single-particle states,
i.e. with the property
X Z
' (r; s) '  (r; s) dr =  ; ; ;
0 0 (A.5)
s=1=2
and c  (cy  ) is a destruction (creation) Fermi operator associated with the single
particle orbital  , obeying Fermi anticommutation relations:

c  cy  + cy  c
0 0  =  ; ; ; 0

c c  + c  c
0 0
 = 0: (A.6)

r
It is important to stress that single particle states '  ( ; s) do not need to be a so-
lution of a particular eigenvalue problem. The only thing which matters is that the
set is complete and Eqs. (A.5) and (A.6) hold, hence in general the '  ( ; s)’s are r
r
not eigenfunctions of the single-particle Hamiltonian h(1) ( ; s). The Fermionic
operators act on a vacuum j0i defined by:

c  j0i = 0 8 ; : (A.7)

From Eqs. (A.6) and from the definition (A.4) anticommutation relations for the
Fermi fields follow:

(r; s) y(r0 ; s0 ) + y(r0 ; s0 ) (r; s) =  (r ; r0 ) s;s 0

(r; s) (r0 ; s0 ) + (r0 ; s0 ) (r; s) = 0: (A.8)

r
These latter relations allow us to interpret the Fermi field y ( ; s) as the operator
which creates an electron with spin up and one with spin down at the position . r
r r
( ; 0) is the Dirac’s delta.
Now we follow Ref. [133] to obtain the Second Quantization form of H in
terms of Fermi fields and y. The one- and two-body terms of the Hamiltonian
H are, respectively:
X Z
H (1) = y(r; s) h(1) (r; s) (r; s) dr (A.9)
s=1=2
 113

and
ZZ
1 X X y(r; s) y(r0 ; s0 ) e2
r jr ; r0j (r ; s ) (r; s) dr dr :
V (2) = 0 0 0
2 s=1=2 s =1=2
0

(A.10)
If we substitute expression (A.4) for into into (A.9) and (A.10) we obtain:
X X X0
H (1) = "0  n  + t0 ;  cy  c  ; (A.11)
  ;
where we have separated the diagonal matrix elements "  from those non-diagonal
t0 ;  , and
V (2) = 12
XXXX
V y y
;  ;  ; c  c  c  c :
0 0 0 0 (A.12)
  0


Here n  = cy  c  is the number occupation operator, and the meaning of the

parameters entering Eqs. (A.11) and (A.12) is the following:
X Z
"0 = ' (r; s) h(1)(r; s) '  (r; s) dr (A.13)
s1=2
is an average single-particle energy,
X Z
t0 ;  = ' (r; s) h(1) (r; s) '  (r; s) dr (A.14)
s=1=2
is an hopping term, and

V
X
e2
ZZ
'  (r; s) '   (r0; s0) '  (r0; s0) ' (r; s) dr dr0
;  ;  ; =
0 0

r jr ; r0j
0 0

s;s =1=2
0

(A.15)
is a Coulomb Matrix element.
114 Second Quantization
Appendix B

Coulomb Matrix Elements

In this Appendix we derive an analytic expression for the generic Coulomb

matrix element in the case of a single two-dimensional QD[134, 135, 136].

We start with the expression (A.15) of the Coulomb matrix element V ;  ;  ; 0 0

written with respect to generic single-particle orbitals '  ( ; s): r

V
X
e2
ZZ
' (r; s) '   (r0; s0) '  (r0; s0) ' (r; s) dr dr0:
;  ;  ; =
0 0

r jr ; r0j
0 0

s;s =1=2
0

We shall now compute this quantity in the case in which the '  ( ; s)’s are the r
eigenfunctions of the purely two-dimensional Hamiltonian H0 ( ) of Eq. (2.16), r
whose expression (spatial part) is given by Eq. (2.42):
s
(jmj+1)=2 n! ;

jmj e;2 =2 Ljmj 2 e;im' :
nm (; ') =  
(n + jmj)! n

Because the spatial part of the eigenfunction does not depend on the spin, we
can suppress the spin index in the Coulomb matrix element. Moreover, Coulomb
interaction preserves the total angular momentum Lz in the scattering of two elec-
trons. Hence, if (n1 ; m1 ), (n2 ; m2 ), (n3 ; m3 ), and (n4 ; m4 ) are the quantum num-
bers of incident and scattered electrons, respectively, we a priori know that the
only non-zero matrix elements are those with

m1 + m2 = M = m3 + m4 : (B.1)
116 Coulomb Matrix Elements

Now we substitute Eq. (2.42) for '  ( r; s) into Eq. (A.15), working with dimen-
sionless coordinates [(x; y ) = 1=2 ]: r
p
Vn1m1 ;n2m2 ;n3m3 ;n4m4 = e   12
2

s r

 (n + jm j)! (n + jnm1 !nj)!2 !n(n3 !n+4! jm j)! (n + jm j)!

1 1 2 2 3 3 4 4
Z Z Z Z jm1 j jm2 j jm3 j jm4 j
 d x1 d y1 d x2 d y2 q 1 2 2 2 1 2
(x1 ; x2 ) + (y1 ; y2 )
;
;
;
;

 Ljnm1 1 j 21 Ljnm2 2 j 22 Ljnm3 3 j 22 Ljnm4 4 j 21
 e;(21 +22 )eim1 '1 eim2 '2 e;im3 '2 e;im4 '1 : (B.2)

Note that in Eq. (B.2) the only dimensional parameter is the prefactor
p s
e2  = e4 m (~ ) = p2R(~ ); (B.3)
r 2r ~2
where R = e4 m =(2~2 2r ) is the effective Rydberg constant of the host material.
We carry on our derivation recovering the expansion (2.40) of the Generalized
Laguerre Polynomial
n  
j j ; 2
X j n + jmj 2j
Ln  = (;1) n ; j j !
m
j =0
and substituting it for its compact expression in (B.2):
p " 4 #1=2
Vn1 m1 ;n2m2 ;n3m3 ;n4m4 =  2 e 2  1 Y ni !
r i=1 (ni + jmi j)!
n 4  Z Z Z Z
X (;1)j1 +j2 +j3 +j4 Y nl + jml j
 j1 !j2 !j3 !j4 ! l=1 nl ; jl d x1 d y1 d x2 d y2
(4)j =0
e;(1 +2 ) ei(m1 ;m4 )'1 ei(m2 ;m3 )'2 jm1 j+jm4 j+2j1 +2j4 jm2 j+jm3 j+2j2 +2j3
2 2

 q 1 2 ;
(x1 ; x2 )2 + (y1 ; y2 )2
(B.4)

with n n1 X
n2 X
n3 X
n4
X X
 :
(4)j =0 j1 =0 j2 =0 j3 =0 j4 =0
 117

At this point, introducing the definitions

1 = j1 + j4 + (jm1j + m1 ) =2 + (jm4 j ; m4 ) =2;

2 = j2 + j3 + (jm2j + m2 ) =2 + (jm3 j ; m3 ) =2;
3 = j2 + j3 + (jm2j ; m2 ) =2 + (jm3j + m3 ) =2;
4 = j1 + j4 + (jm1j ; m1 ) =2 + (jm4j + m4 ) =2; (B.5)

we may write (B.4) as

p "
4 #1=2
Vn1m1 ;n2m2 ;n3m3 ;n4m4 =  2 e2  1 Y ni !
r i=1 (ni + jmi j)!
n 4  Z Z Z Z
X (;1)j1 +j2 +j3 +j4 Y nl + jml j
 j ! j !j !j ! n ; j d x1 d y1 d x2 d y2
(4)j =0 1 2 3 4 l=1 l l

e;(1 +2 )
2 2
;
1;
2;
3;

q 1ei'1 2 ei'2 2e;i'2 1 e;i'1 4
:
(x1 ; x2 )2 + (y1 ; y2 )2
(B.6)

It is convenient to define the multiple integral I :

Z Z Z Z
e;(1 +2 )
2 2

I = d x1 d y1 d x2 d y2 q
(x1 ; x2 )2 + (y1 ; y2 )2
;
;
;
;

 1 ei'1 1 2 ei'2 2 2 e;i'2 3 1e;i'1 4 : (B.7)

We now separate integration variables into center of mass R and relative motion
 coordinates
R = (r1 + r2) =2;  = r1 ; r2; (B.8)
identifying the two-dimensional real space with the complex plane, namely

(x1 ; y1)  1 ei'1 = z1 = Z + z=2; (x2 ; y2 )  2 ei'2 = z2 = Z ; z=2;

Z = (z1 + z2 ) =2; z = z1 ; z2 :
Eq. (B.7) turns into
Z Z
I = d Z e;2jZ j d z jz j;1 e;jzj =2 (Z + z=2) 1
2 2

 (Z ; z=2) (Z  ; z =2) (Z  + z =2) :

2 3 4
(B.9)
118 Coulomb Matrix Elements

Making use of the binomial theorem

n  
n
(a + b) =
X n ai bn;i (B.10)
i=0 i
Eq. (B.9) is reduced to
X  1  2  3  4  Z Z
I = d Z e;2jZ j d z jz j;1 e;jzj =2
2 2

(4)`=0
`1 `2 `3 `4
Z `1 +`2 (Z )`3+`4 (z=2) 1 ;`1 (;z=2) 2 ;`2 (;z =2) 3 ;`3 (z =2) 4 ;`4 ;
(B.11)

or
4  
X Y Z Z
I = i
(;1) 2 + 3 ;`2 ;`3 2;G d Z e;2jZ j
2
d z jz j;1 e;jzj =2
2

(4)`=0 i=1 i
`
 jzjG; exp [i'rm( 1 + 2 ; 3 ; 4 ; `1 ; `2 + `3 + `4 )]
 jZ j exp [i'cm(`1 + `2 ; `3 ; `4 )]; (B.12)

with the definitions

G = 1 + 2 + 3 + 4;  = `1 + ` 2 + ` 3 + `4 : (B.13)

Performing the integration over azimuthal angles we obtain the two constraints
`1 + `2 = `3 + `4 and 1 + 2 ; 3 ; 4 = 0. This latter condition is equivalent
to angular momentum conservation (B.1), as it is easy to verify from definitions
(B.5). Eq. (B.12) becomes:
4  
X Y
I = m1 +m2 ;m3+m4 4 2 `1 +`2;`3+`4 i
(;1) 2 + 3 ;`2 ;`3 2;G
(4)`=0 i=1 i`
Z Z
 d jZ j jZ j+1 e;2jZ j2 d jzj jzjG; e;jzj2 =2: (B.14)

After some manipulation, using the definition of Gamma function ;(x) (note that
G  ), we obtain
X 4  
Y
I = m1 +m2 ;m3 +m4 22;G=2;1=2 `1+`2 ;`3+`4 i
(;1) 2 + 3 ;`2 ;`3
(4)`=0 i=1 `i
 ;(=2 + 1) ;([G ;  + 1] =2) (B.15)
 119

and finally
p "Y #1=2
Vn1m1 ;n2m2 ;n3m3 ;n4m4 = m1 +m2 ;m3 +m4 e  4
2 ni !
r i=1 (ni + jmi j)!
n 4  
X (;1)j1 +j2 +j3 +j4 Y nl + jml j
 j1 !j2 !j3 !j4 ! l=1 nl ; jl
(4)j =0
X 4  
Y
 2;G=2;1=2 `1 +`2;`3+`4 (;1) 2 + 3 ;`2 ;`3
t
(4)`=0 t=1 t `
 ;(=2 + 1) ;([G ;  + 1] =2) : (B.16)
120 Coulomb Matrix Elements
Appendix C

Wigner-von Neumann Theorem

In this appendix we derive the Wigner-von Neumann theorem presented in

Sec. 3.2[133].

Theorem C.1 (E. Wigner and J. von Neumann 1929) If electron terms depend
on one parameter, only terms of different symmetry can intersect, while the inter-
section of terms of like symmetry is impossible.

Let’s take as parameter on which electron terms depend the inter-dot coupling
t. They can be represented graphically by plotting the energy as a function of t.Let
U1 (t), U2(t) be two different electronic terms. If they intersect at some point, then
the functions U1 and U2 will have neighboring values near this point. To decide
whether such an intersection can occurr, it is convenient to put the problem as
follows. Let us consider a point t0 where the functions U1 (t), U2 (t) have very
close but not equal values (which we denote by E1 , E2 ), and examine whether
or not we can make U1 and U2 equal by displacing the point a short distance t.
The energies E1 and E2 are eigenvalues of the Hamiltonian HGHH of the dots
with a coupling strenght t0 . If we add to the hopping coefficient t0 an increment
t, the Hamiltonian becomes HGHH + V , where V = t (@ HGHH =@t) is a small
correction; the values of the functions U1 , U2 at the point t0 + t can be regarded
as eigenvalues of the new Hamiltonian. This enables us to determine the values
of the terms U1 (t), U2 (t) at the point t0 + t by means of perturbation theory, V
being regarded as a perturbation to the operator HGHH .
122 Wigner-von Neumann Theorem

The ordinary method of perturbation theory is here inapplicable, however,

since the eigenvalues E1 , E2 of the energy in the unperturbed problem are very
close to each other, and their difference is in general small compared with the
magnitude of the perturbation. Since, in the limit where the difference E2 ; E1
tends to zero, we have the case of degenerate eigenvalues, it is natural to attempt
to apply to the case of close eigenvalues the degenerate perturbation theory.
Let j 1 i, j 2 i the eigenstates of the unperturbed operator HGHH which cor-
respond to the energies E1 , E2 . As an initial zero-order approximation we take,
instead of j 1 i and j 2 i themselves, linear combinations of them of the form

j i = c1 j 1 i + c2 j 2 i : (C.1)

Substituting this expression in the perturbed equation

; GHH

H +V j i = E j i; (C.2)

we obtain

c1 (E1 + V ; E ) j 1 i + c2 (E2 + V ; E ) j 2i = 0: (C.3)

Multiplying this equation on the left by h 1 j and h 2 j in turn, we have two alge-
braic equations:

c1 (E1 + V11 ; E ) + c2V12 = 0;

c1 V21 + c2 (E2 + V22 ; E ) = 0; (C.4)

where Vik = h i jV j k i. since the operator V is Hermitian, the quantities V11 and
V22 are real while V12 = V21 . The compatibility conditions for these equation is
E1 + V11 ; E V12
= 0;
E2 + V22 ; E
(C.5)
V21
whence we obtain after some calculation
q
E = (E1 + E2 + V11 + V22 ) =2  (E1 ; E2 + V11 ; V22)2 + jV12j2=2: (C.6)

This formula gives the required eigenvalues of the energy in the first approxima-
tion.
 123

If the energy values of the two terms become equal at the point t0 + t (i.e. the
terms intersect), this means that the two values of E given by formula (C.6) are the
same. For this to happen, the expression under the radical in (C.6) must vanish.
Since it is the sum of two squares, we obtain, as the condition for there to be points
of intersection of the terms, the equations

E1 ; E2 + V11 ; V22 = 0; V12 = 0: (C.7)

However, we have at our disposal only one arbitrary parameter giving the pertur-
bation V , namely the magnitude t of the displacement. Hence the two equations
(C.7) cannot in general be simultaneously satisfied (we suppose that the functions
j 1 i, j 2 i are chosen to be real, so that V12 also is real).
It may happen, however, that the matrix element V12 vanishes identically; there
then remains only one equation (C.7), which can be satisfied by a suitable choice
of t. This happens in all cases where the two terms considered are of different
symmetry. This statement holds because the operator V (like the Hamiltonian
HGHH) commutes with all the symmetry operators for the system. Q.E.D.
If, as a result of some approximate calculation, we obtain two intersecting
terms of the same symmetry, they are found to move apart on calculating the next
approximation, as shown by the continuous lines in Fig. C.1.
124 Wigner-von Neumann Theorem

U(t)

t
Figure C.1: Diagram of electron terms U (t) vs the hopping coefficient t. If, as
a result of some approximate calculation, we obtain two intersecting terms of the
same symmetry, they are found to move apart on calculating the next approxima-
tion, as shown by the continuous lines.
Acknowledgements 125

I want to thank my supervisors, Franca and Elisa, for all the support, encour-
agement and stimulation they always gave me. It was very nice to work with them.
It was a pleasure also to work with Prof. Fausto Rossi, who is now in Torino. I
am in debt with Professor Sham at UCSD with whom I worked for one year. It
was a very exciting experience, and I think I learned a lot about Physics. Thanks
also to Prof. S. G. Louie and M. L. Cohen at UCB for their very kind hospital-
ity in Berkeley. I acknowledge very useful discussions about quantum dots with
Prof. Daniela Pfannkuche, Prof. Pawel Hawrylak, Dr. Axel Lorke, Dr. J. J. Pala-
cios, Dr. Davide Vanossi, and last but not least, Dr. Guido Goldoni. Thanks for
technical support to Gianpaolo Prampolini, Cristina Murari, and Roberta Canta-
roni of Computer Center at University of Modena, and to G. Casalini for his kind
help in nasty bureaucracy matters.
It is really an impossible task to thank all friends and colleagues in Modena
and around the world with whom I worked and had fun: I would not have re-
sisted without them. Let me just say thank to my family: babbo, mamma, zia and
fratellino. Last word is for Emanuela.
126 Acknowledgements
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