Академический Документы
Профессиональный Документы
Культура Документы
L. P. Kouwenhoven
Kavli Institute of Nanoscience, Delft University of Technology, P.O. Box 5046, 2600 GA
Delft, The Netherlands
J. R. Petta
Department of Physics, Princeton University, Princeton, New Jersey 08544, USA
and Department of Physics, Harvard University, Cambridge, Massachusetts 02138, USA
S. Tarucha
Department of Applied Physics and ICORP-JST, The University of Tokyo, Hongo, Bunkyo-
ku, Tokyo 113-8656, Japan
L. M. K. Vandersypen
Kavli Institute of NanoScience, Delft University of Technology, P.O. Box 5046, 2600 GA
Delft, The Netherlands
共Published 1 October 2007; publisher error corrected 4 October 2007兲
The canonical example of a quantum-mechanical two-level system is spin. The simplest picture of spin
is a magnetic moment pointing up or down. The full quantum properties of spin become apparent in
phenomena such as superpositions of spin states, entanglement among spins, and quantum
measurements. Many of these phenomena have been observed in experiments performed on
ensembles of particles with spin. Only in recent years have systems been realized in which individual
electrons can be trapped and their quantum properties can be studied, thus avoiding unnecessary
ensemble averaging. This review describes experiments performed with quantum dots, which are
nanometer-scale boxes defined in a semiconductor host material. Quantum dots can hold a precise but
tunable number of electron spins starting with 0, 1, 2, etc. Electrical contacts can be made for charge
transport measurements and electrostatic gates can be used for controlling the dot potential. This
system provides virtually full control over individual electrons. This new, enabling technology is
stimulating research on individual spins. This review describes the physics of spins in quantum dots
containing one or two electrons, from an experimentalist’s viewpoint. Various methods for extracting
spin properties from experiment are presented, restricted exclusively to electrical measurements.
Furthermore, experimental techniques are discussed that allow for 共1兲 the rotation of an electron spin
into a superposition of up and down, 共2兲 the measurement of the quantum state of an individual spin,
and 共3兲 the control of the interaction between two neighboring spins by the Heisenberg exchange
interaction. Finally, the physics of the relevant relaxation and dephasing mechanisms is reviewed and
experimental results are compared with theories for spin-orbit and hyperfine interactions. All these
subjects are directly relevant for the fields of quantum information processing and spintronics with
single spins 共i.e., single spintronics兲.
A. Spin-to-charge conversion 1231 ticle. The magnetic moment corresponding to spin is re-
B. Single-shot spin readout using a difference in energy 1231 ally very small and in most practical cases it can be ig-
C. Single-shot spin readout using a difference in tunnel nored. For instance, the most sensitive force sensor to
rate 1233 date has only recently been able to detect some effect
VII. Spin Interaction with the Environment 1234 from the magnetic moment of a single-electron spin
A. Spin-orbit interaction 1235 共Rugar et al., 2004兲. In solids, spin can apparently lead to
1. Origin 1235 strong effects, given the existence of permanent mag-
2. Spin-orbit interaction in bulk and two nets. Curiously, this has little to do with the strength of
dimensions 1235 the magnetic moment. Instead, the fact that spin is asso-
3. Spin-orbit interaction in quantum dots 1236 ciated with its own quantum number, combined with
4. Relaxation via the phonon bath 1237 Pauli’s exclusion principle that quantum states can at
5. Phase randomization due to the spin-orbit most be occupied with one fermion, leads to the phe-
interaction 1239 nomenon of exchange interaction. Because the exchange
B. Hyperfine interaction 1240 interaction is a correction term to the strong Coulomb
1. Origin 1240 interaction, it can be of much larger strength in solids
2. Effect of the Overhauser field on the than the dipolar interaction between two spin magnetic
electron-spin time evolution 1241 moments at an atomic distance of a few angstroms. It is
3. Mechanisms and time scales of nuclear field the exchange interaction that forces the electron spins in
fluctuations 1242 a collective alignment, together yielding a macroscopic
4. Electron-spin decoherence in a fluctuating magnetization 共Ashcroft and Mermin, 1974兲. It remains
nuclear field 1243 striking that an abstract concept as 共anti兲symmetrization
C. Summary of mechanisms and time scales 1244 in the end gives rise to magnets.
VIII. Spin States in Double Quantum Dots 1244 The magnetic state of solids has found important ap-
A. Electronic properties of electrons in double dots 1244 plications in electronics, in particular for memory de-
1. Charge stability diagram 1244 vices. An important field has emerged in the last two
2. High bias regime: Bias triangles 1246 decades known as spintronics. Phenomena like giant
B. Spin states in two-electron double dots 1248 magnetoresistance or tunneling magnetoresistance form
C. Pauli spin blockade 1249 the basis for magnetic heads for reading out the mag-
D. Hyperfine interaction in a double dot: netic state of a memory cell. Logic gates have been re-
Singlet-triplet mixing 1251 alized based on magnetoresistance effects as well 共Wolf
IX. Coherent Spin Manipulation 1254 et al., 2001; Zutic et al., 2004兲. In addition to applications,
A. Single-spin manipulation: ESR 1254 important scientific discoveries have been made in the
B. Manipulation of coupled electron spins 1256 field of spintronics 共Awschalom and Flatte, 2007兲, in-
X. Perspectives 1260 cluding magnetic semiconductors 共Ohno, 1998兲 and the
Acknowledgments 1261 spin Hall effect 共Sih et al., 2005兲. It is important to note
Appendix: Sign of the Ground-State Spin and the Nuclear that all spintronics phenomena consider macroscopic
Fields in GaAs 1261 numbers of spins. Together these spins form things like
1. Sign of the spin ground states 1261 spin densities or a collective magnetization. Although
2. Sign and magnitude of the thermal nuclear field 1261 the origin of spin densities and magnetization is quan-
3. Sign of the dynamic nuclear field 1261 tum mechanical, these collective, macroscopic variables
References 1261 behave entirely classically. For instance, the magnetiza-
tion of a micron-cubed piece of cobalt is a classical vec-
tor. The quantum state of this vector dephases so rapidly
I. INTRODUCTION
that quantum superpositions or entanglement between
The spin of an electron remains a somewhat mysteri- vectors is never observed. One has to go to systems with
ous property. The first derivations in 1925 of the spin a small number of spins, for instance in magnetic mol-
magnetic moment, based on a rotating charge distribu- ecules, in order to find quantum effects in the behavior
tion of finite size, are in conflict with special relativity of the collective magnetization 关for an overview, see,
theory. Pauli advised the young Ralph Kronig not to e.g., Gunther and Barbara 共1994兲兴.
publish his theory since “it has nothing to do with real- The technological drive to make electronic devices
ity.” More fortunate were Samuel Goudsmit and George continuously smaller has some interesting scientific con-
Uhlenbeck, who were supervised by Ehrenfest: “Pub- sequences. For instance, it is now routinely possible to
lish, you are both young enough to be able to afford a make small electron boxes in solid-state devices that
stupidity!”1 It requires Dirac’s equation to find that the contain an integer number of conduction electrons. Such
spin eigenvalues correspond to one-half times Planck’s devices are usually operated as transistors 共via field-
constant ប while considering the electron as a point par- effect gates兲 and are therefore named single-electron
transistors. In semiconductor boxes the number of
trapped electrons can be reduced to 0, or 1, 2, etc. Such
1 semiconductor single-electron transistors are called
See URL: http://www.lorentz.leidenuniv.nl/history/spin/
goudsmit.html quantum dots 共Kouwenhoven et al., 2001兲. Electrons are
trapped in a quantum dot by repelling electric fields im- view demonstrate that the five DiVincenzo criteria for
posed from all sides. The final region in which a small universal quantum computation using single-electron
number of electrons can still exist is typically at the scale spins have been fulfilled to a large extent 共DiVincenzo,
of tens of nanometers. The eigenenergies in such boxes 2000兲: initialization, one- and two-qubit operations, long
are discrete. Filling these states with electrons follows coherence times, and readout. Currently, the state of the
the rules from atomic physics, including Hund’s rule, art is at the level of single and double quantum dots and
shell filling, etc. much work is required to build larger systems.
Studies with quantum dots have been performed dur- In this review the system of choice is quantum dots in
ing the 1990s. By now it has become standard technol- GaAs semiconductors, simply because this has been
ogy to confine single-electron charges. Electrons can be most successful. Nevertheless, the physics is entirely
trapped as long as one desires. Changes in charge when general and can be fully applied to new material systems
one electron tunnels out of the quantum dot can be such as silicon-based transistors, carbon nanotubes,
measured on a microsecond time scale. Compared to semiconductor nanowires, graphene devices, etc. These
this control of charge, it is very difficult to control indi- other host materials may have advantageous spin prop-
vidual spins and measure the spin of an individual elec- erties. For instance, carbon-based devices can be puri-
tron. Such techniques have been developed only over fied with the isotope 12C in which the nuclear spin is
the past few years. zero, thus entirely suppressing spin dephasing by hyper-
In this review we describe experiments in which indi- fine interaction. This kind of hardware solution to engi-
vidual spins are controlled and measured. This is mostly neer a long-lived quantum system will be discussed at
an experimental review with explanations of the under- the end of this review. Also, we here restrict ourselves
lying physics. This review is limited to experiments that exclusively to electron-transport measurements of quan-
involve one or two electrons strongly confined to single tum dots, leaving out optical spectroscopy of quantum
or double quantum dot devices. The experiments show dots, which is a very active field in its own.3 Again, much
that one or two electrons can be trapped in a quantum of the physics discussed in this review also applies to
dot; that the spin of an individual electron can be put in optically measured quantum dots.
a superposition of up and down states; that two spins can Section II starts with an introduction on quantum dots
be made to interact and form an entangled state such as including the basic model of Coulomb blockade to de-
a spin singlet or triplet state; and that the result of such scribe the relevant energies. These energies can be visu-
manipulation can be measured on individual spins. alized in transport experiments and the relation between
These abilities of almost full control over the spin of experimental spectroscopic lines and underlying ener-
individual electrons enable the investigation of a new gies are explained in Sec. III. This spectroscopy is spe-
regime: single spin dynamics in a solid-state environ- cifically applied to spin states in single quantum dots in
ment. The dynamics are fully quantum mechanical and Sec. IV. Section V introduces a charge-sensing technique
thus quantum coherence can be studied on an individual that is used in Sec. VI to read out the spin state of indi-
electron spin. The exchange interaction is now also con- vidual electrons. Section VII provides a description of
trolled on the level of two particular spins that are spin-orbit and hyperfine interactions. In Sec. VIII, spin
brought into contact simply by varying some voltage states in double quantum dots are introduced and the
knob. concept of Pauli spin blockade is discussed. Quantum
In a solid the electron spins are not completely decou- coherent manipulations of spins in double dots are dis-
pled from other degrees of freedom. First of all, spins cussed in Sec. IX. Finally, a perspective is outlined in
and orbits are coupled by the spin-orbit interaction. Sec- Sec. X.
ond, the electron spins have an interaction with the spins
of the atomic nuclei, i.e., the hyperfine interaction. Both
interactions cause the lifetime of a quantum superposi- II. BASICS OF QUANTUM DOTS
tion of spin states to be finite. We therefore also describe
A. Introduction to quantum dots
experiments that probe spin-orbit and hyperfine interac-
tions by measuring the dynamics of individual spins. A quantum dot is an artificially structured system that
The study of individual spins is motivated by an inter- can be filled with electrons 共or holes兲. The dot can be
est in fundamental physics, but also by possible applica- coupled via tunnel barriers to reservoirs, with which
tions. First of all, miniaturized spintronics is developing electrons can be exchanged 共see Fig. 1兲. By attaching
towards single spins. In this context, this field can be current and voltage probes to these reservoirs, we can
denoted as single spintronics2 in analogy to single elec- measure the electronic properties. The dot is also
tronics. A second area of applications is quantum infor- coupled capacitively to one or more gate electrodes,
mation science. Here the spin states form the qubits. which can be used to tune the electrostatic potential of
The original proposal by Loss and DiVincenzo 共1998兲 the dot with respect to the reservoirs.
has been the guide in this field. In the context of quan-
tum information, the experiments described in this re-
3
See, e.g., Atature et al. 共2006兲, Berezovsky et al. 共2006兲,
Greilich, Oulton, et al. 共2006兲, Krenner et al. 共2006兲, and refer-
2
Name coined by Wolf 共2005兲. ences therein.
resistance 共Ohmic兲 contacts are made to the 2DEG res- The potential of charge sensing was first demonstrated
ervoirs. To access the quantum phenomena in GaAs by Ashoori et al. 共1992兲 and Field et al. 共1993兲. But
gated quantum dots, they have to be cooled down to whereas current measurements were already used exten-
well below 1 K. All experiments that are discussed in sively in the first experiments on quantum dots 共Kou-
this review are performed in dilution refrigerators with wenhoven et al., 1997兲, charge sensing has only recently
typical base temperatures of 20 mK. been fully developed as a spectroscopic tool 共Elzerman,
In so-called vertical quantum dots, control over the Hanson, Willems van Beveren, Vandersypen, et al., 2004;
number of electrons down to zero was already achieved Johnson, Marcus, et al., 2005兲. Several implementations
in the 1990s 共Kouwenhoven et al., 2001兲. In lateral gated of electrometers coupled to a quantum dot have been
dots this proved to be more difficult, since reducing the demonstrated: a single-electron transistor fabricated on
electron number by driving the gate voltage to more top of the heterostructure 共Ashoori et al., 1992; Lu et al.,
negative values tends to decrease the tunnel coupling to 2003兲, a second electrostatically defined quantum dot
the leads. The resulting current through the dot can then 共Hofmann et al., 1995; Fujisawa et al., 2004兲, and a quan-
become unmeasurably small before the few-electron re- tum point contact 共QPC兲 共Field et al., 1993; Sprinzak et
gime is reached. However, by proper design of the sur- al., 2002兲. The QPC is the most widely used because of
face gate geometry the decrease of the tunnel coupling its ease of fabrication and experimental operation. We
can be compensated for. discuss the QPC operation and charge sensing tech-
In 2000, Ciorga et al. reported measurements on the niques in more detail in Sec. V.
first lateral few-electron quantum dot 共Ciorga et al., We briefly compare charge sensing to electron-
2000兲. Their device, shown in Fig. 2共b兲, makes use of two transport measurements. The smallest currents that can
types of gates specifically designed to have different be resolved in optimized setups and devices are roughly
functionalities. The gates of one type are big and largely 10 fA, which sets a lower bound of order 10 fA/ e
enclose the quantum dot. The voltages on these gates ⬇ 100 kHz on the tunnel rate to the reservoir ⌫ for
mainly determine the dot potential. The other type of which transport experiments are possible 关see, e.g.,
gate is thin and just reaches up to the barrier region. The Vandersypen et al. 共2004兲 for a discussion on noise
voltage on this gate has a very small effect on the dot sources兴. For ⌫ ⬍ 100 kHz the charge detection tech-
potential but it can be used to set the tunnel barrier. The nique can be used to resolve electron tunneling in real
combination of the two gate types allows the dot poten- time. Because the coupling to the leads is a source of
tial 共and thereby electron number兲 to be changed over a decoherence and relaxation 共most notably via cotunnel-
wide range while keeping the tunnel rates high enough ing兲, charge detection is preferred for quantum informa-
for measuring electron transport through the dot. tion purposes since it still functions for very small cou-
Applying the same gate design principle to a double plings to a 共single兲 reservoir.
quantum dot, Elzerman et al. demonstrated control over Measurements using either technique are conve-
the electron number in both dots while maintaining tun- niently understood with the constant interaction model.
able tunnel coupling to the reservoir 共Elzerman et al., In the next section we use this model to describe the
2003兲. Their design is shown in Fig. 2共c兲 关for more details physics of single dots and show how relevant spin pa-
on design considerations and related versions of this rameters can be extracted from measurements.
gate design, see Hanson 共2005兲兴. In addition to the
coupled dots, two quantum point contacts 共QPCs兲 are
incorporated in this device to serve as charge sensors.
The QPCs are placed close to the dots, thus ensuring a D. The constant interaction model
good charge sensitivity. This design has become the stan-
dard for lateral coupled quantum dots and is used with We briefly outline the main ingredients of the constant
minor adaptions by several research groups 共Petta et al., interaction model; for more extensive discussions, see
2004; Pioro-Ladrière et al., 2005兲; one noticeable im- van Houten et al. 共1992兲 and Kouwenhoven et al. 共1997,
provement has been the electrical isolation of the charge 2001兲. The model is based on two assumptions. First, the
sensing part of the circuit from the reservoirs that con- Coulomb interactions among electrons in the dot, and
nect to the dot 共Hanson et al., 2005兲. between electrons in the dot and those in the environ-
ment, are parametrized by a single, constant capacitance
C. This capacitance is the sum of the capacitances be-
C. Measurement techniques tween the dot and the source CS, the drain CD, and the
gate CG: C = CS + CD + CG. 共In general, capacitances to
In this review, two all-electrical measurement tech- multiple gates and other parts of the 2DEG will also
niques are discussed: 共i兲 measurement of the current due play a role; they can simply be added to C.兲 The second
to transport of electrons through the dot, and 共ii兲 detec- assumption is that the single-particle energy-level spec-
tion of changes in the number of electrons on the dot trum is independent of these interactions and therefore
with a nearby electrometer, so-called charge sensing. of the number of electrons. Under these assumptions,
With the latter technique, the dot can be probed nonin- the total energy U共N兲 of a dot with N electrons in the
vasively in the sense that no current needs to be sent ground state, with voltages VS, VD, and VG applied to
through the dot. the source, drain, and gate, respectively, is given by
关− 兩e兩共N − N0兲 + CSVS + CDVD + CGVG兴2 Eadd共N兲 = 共N + 1兲 − 共N兲 = EC + ⌬E. 共4兲
U共N兲 =
2C The addition energy consists of a purely electrostatic
N part, the charging energy EC, plus the energy spacing
+ 兺 En共B兲, 共1兲 between two discrete quantum levels ⌬E. Note that ⌬E
n=1 can be zero, when two consecutive electrons are added
to the same spin-degenerate level.
where −兩e兩 is the electron charge, N0 兩 e兩 is the charge in Electron tunneling through the dot critically depends
the dot compensating the positive background charge on the alignment of electrochemical potentials in the dot
originating from the donors in the heterostructure, and with respect to those of the source S and the drain D.
B is the applied magnetic field. The terms CSVS, CDVD, The application of a bias voltage VSD = VS − VD between
and CGVG can be changed continuously and represent the source and drain reservoir opens up an energy win-
an effective induced charge that changes the electro- dow between S and D of S − D = −兩e 兩 VSD. This en-
static potential on the dot. The last term of Eq. 共1兲 is a ergy window is called the bias window. For energies
sum over the occupied single-particle energy levels within the bias window, the electron states in one reser-
En共B兲 which depend on the characteristics of the con- voir are filled whereas states in the other reservoir are
finement potential. empty. Therefore if there is an appropriate electro-
The electrochemical potential 共N兲 of the dot is de- chemical potential level within the bias window, elec-
fined as trons can tunnel from one reservoir onto the dot and off
to the empty states in the other reservoir. Here appro-
共N兲 ⬅ U共N兲 − U共N − 1兲 priate means that the electrochemical potential corre-
冉 冊
sponds to a transition that involves the current state of
1 the quantum dot.
= N − N0 − EC
2 In the following, we assume the temperature to be
negligible compared to the energy-level spacing ⌬E 共for
EC
− 共CSVS + CDVD + CGVG兲 + EN , 共2兲 GaAs dots this roughly means T ⬍ 0.5 K兲. The size of the
兩e兩 bias window then separates two regimes: the low-bias
regime where at most one dot level is within the bias
where EC = e2 / C is the charging energy. The electro- window 共−兩e兩VSD ⬍ ⌬E , Eadd兲, and the high-bias regime
chemical potential contains an electrostatic part 共first where multiple dot levels can be in the bias window
two terms兲 and a chemical part 共last term兲. Here 共N兲 共−兩e兩VSD 艌 ⌬E and/or −兩e兩VSD 艌 Eadd兲.
denotes the transition between the N-electron ground
state, GS共N兲, and the 共N − 1兲-electron ground state, E. Low-bias regime
GS共N − 1兲. When excited states also play a role, we have
to use a more explicit notation to avoid confusion: the For a quantum dot system in equilibrium, electron
electrochemical potential for the transition between the transport is only possible when a level corresponding to
共N − 1兲-electron state 兩a典 and the N-electron state 兩b典 is transport between successive ground states is in the bias
then denoted as a↔b, and is defined as the difference in window, i.e., S 艌 共N兲 艌 D for at least one value of N.
total energy between state 兩b典, Ub共N兲, and state 兩a典, If this condition is not met, the number of electrons on
Ua共N − 1兲: the dot remains fixed and no current flows through the
dot. This is known as Coulomb blockade. An example of
a↔b ⬅ Ub共N兲 − Ua共N − 1兲. 共3兲 such a level alignment is shown in Fig. 3共a兲.
Coulomb blockade can be lifted by changing the volt-
Note that the electrochemical potential depends lin- age applied to the gate electrode, as can be seen from
early on the gate voltage, whereas the energy has a qua- Eq. 共2兲. When 共N兲 is in the bias window one extra elec-
dratic dependence. In fact, the dependence is the same tron can tunnel onto the dot from the source 关see Fig.
for all N and the whole “ladder” of electrochemical po- 3共b兲兴, so that the number of electrons increases from N
tentials can be moved up or down while the distance − 1 to N. After it has tunneled to the drain, another
between levels remains constant.4 It is this property that electron can tunnel onto the dot from the source. This
makes the electrochemical potential the most conve- cycle is known as single-electron tunneling.
nient quantity for describing electron tunneling. By sweeping the gate voltage and measuring the cur-
The electrochemical potentials of the transitions be-
rent through the dot IDOT a trace is obtained as shown in
tween successive ground states are spaced by the so-
Fig. 3共c兲. At the positions of the peaks in IDOT, an elec-
called addition energy:
trochemical potential level corresponding to transport
between successive ground states is aligned between the
4
Deviations from this model are sometimes observed in sys- source and drain electrochemical potentials and a single-
tems where the source-drain voltage and gate voltage are var- electron tunneling current flows. In the valleys between
ied over a very wide range, one notable example being single peaks, the number of electrons on the dot is fixed due to
molecules trapped between closely spaced electrodes, where Coulomb blockade. By tuning the gate voltage from one
capacitances can depend on the electron state. valley to the next one, the number of electrons on the
FIG. 3. Quantum dot in the regime of low bias. 共a兲, 共b兲 Sche-
trochemical potentials of all relevant transitions are first
matic diagrams of the electrochemical potential levels of a
calculated by applying Eq. 共3兲. For example, consider
quantum dot in the low-bias regime. 共a兲 If no level in the dot
falls within the bias window set by S and D, the electron
two successive ground states GS共N兲 and GS共N + 1兲 and
number is fixed at N − 1 due to Coulomb blockade. 共b兲 The the excited states ES共N兲 and ES共N + 1兲, which are sepa-
共N兲 level is in the bias window, so the number of electrons rated from the GSs by ⌬E共N兲 and ⌬E共N + 1兲, respec-
can alternate between N − 1 and N, resulting in a single- tively 关see Fig. 5共a兲兴. The resulting electrochemical po-
electron tunneling current. The magnitude of the current de- tential ladder is shown in Fig. 5共b兲 共we omit the
pends on the tunnel rate between the dot and the reservoir on transition between the two ESs兲. Note that the electro-
the left ⌫S and on the right ⌫D 关see Kouwenhoven et al. 共1997兲 chemical potential of the transition ES共N兲 ↔ GS共N + 1兲 is
for details兴. 共c兲 Schematic plot of the current IDOT through the lower than that of the transition between the two ground
dot as a function of gate voltage VG. The gate voltages where states.
the level alignments of 共a兲 and 共b兲 occur are indicated. The electrochemical potential ladder is used to define
the gate voltage axis of the 共−兩e兩VSD , VG兲 plot, as in Fig.
dot can be precisely controlled. The distance between 5共c兲. Here each transition indicates the gate voltage at
peaks corresponds to Eadd 关see Eq. 共4兲兴, and therefore which its electrochemical potential is aligned with S
provides insight into the energy spectrum of the dot. and D at VSD = 0. Analogous to Figs. 3共c兲 and 3共d兲,
sweeping the gate voltage at low bias will show electron
tunneling only at the gate voltage indicated by
F. High-bias regime GS共N兲 ↔ GS共N + 1兲. For all other gate voltages the dot is
in Coulomb blockade.
We now look at the regime where the source-drain Then for each transition a V-shaped region is outlined
bias is so high that multiple dot levels can participate in
in the 共−兩e兩VSD , VG兲 plane, where its electrochemical po-
electron tunneling. Typically the electrochemical poten-
tential is within the bias window. This yields a plot like
tial of only one of the reservoirs is changed in experi-
Fig. 5共c兲. The slopes of the two edges of the V shape
ments, and the other one is kept fixed. Here we take the
depend on the capacitances; for VD = 0, the two slopes
drain reservoir to be at ground, i.e., D = 0. When a
d共−兩e兩VSD兲 / dVG are −CG / 共C − CS兲 and +CG / CS. The
negative voltage is applied between the source and the
transition between the N-electron GS and the
drain, S increases 共since S = −兩e兩VSD兲. The levels of the
共N + 1兲-electron GS 共dark solid line兲 defines the regions
dot also increase, due to the capacitive coupling between
of Coulomb blockade 共outside the V shape兲 and tunnel-
the source and the dot 关see Eq. 共2兲兴. Again, a current can
ing 共within the V shape兲. The other solid lines indicate
flow only when a level corresponding to a transition be-
where the current changes due to the onset of transitions
tween ground states falls within the bias window. When
involving excited states.
VSD is increased further such that also a transition in-
The set of solid lines indicates all values in the param-
volving an excited state falls within the bias window,
eter space spanned by VSD and VG where the current
there are two paths available for electrons tunneling
IDOT changes. Typically, the differential conductance
through the dot 关see Fig. 4共a兲兴. In general, this will lead
to a change in current, enabling us to perform energy dIDOT / dVSD is plotted, which has a nonzero value only
spectroscopy of the excited states. How exactly the cur- at the solid lines.5
rent changes depends on the tunnel coupling of the two A general rule of thumb for positions of the lines in-
dicating finite differential conductance is this: if a line
levels involved. Increasing VSD even more eventually
leads to a situation where the bias window is larger than
the addition energy 关see Fig. 4共b兲兴. Here the electron 5
In practice, a tunnel coupling dependence on VG and VSD
number can alternate between N − 1, N, and N + 1, lead- may result in a nonzero value of dIDOT / dVSD where current
ing to a double-electron tunneling current. flows. Since this background of nonzero dIDOT / dVSD is more
We now show how the current spectrum as a function uniform and much smaller than peaks in dIDOT / dVSD at the
of bias and gate voltage can be mapped out. The elec- solid lines, the two are easily distinguished in experiments.
FIG. 5. 共Color online兲 Schematic of a high-bias measurement. 共a兲 Energies for N electrons U共N兲 and for N + 1 electrons U共N
+ 1兲. Possible transitions are indicated by arrows. 共b兲 The electrochemical potential ladder for the transitions depicted in 共a兲. 共c兲
Schematic plot of the differential conductance dIDOT / dVSD as a function of −兩e兩VSD and VG. At several positions the level
alignment is indicated with schematic diagrams.
terminates at the N-electron Coulomb blockade region, tween different levels 共Fujisawa et al., 2002b兲.
the transition necessarily involves an N-electron excited If the voltage is swept across multiple electron
state. This is true for any N. As a consequence, no lines transitions and for both signs of the bias voltage, the
terminate at the Coulomb blockade region where N = 0, Coulomb blockade regions appear as diamond shapes
as there exists no excited state for N = 0.6 For a transition in the 共−兩e兩VSD , VG兲 plane. These are the well-known
between two excited states, say ES共N兲 and ES共N + 1兲, the Coulomb diamonds.
position of the line depends on the energy-level spacing:
for ⌬E共N + 1兲 ⬎ ⌬E共N兲, the line terminates at the 共N III. SPIN SPECTROSCOPY METHODS
+ 1兲-electron Coulomb blockade region, and vice versa.
A measurement as shown in Fig. 5共c兲 is very useful for In this section, we discuss various methods for getting
finding the energies of the excited states. Where a line of information on the spin state of electrons on a quantum
a transition involving one excited state touches the Cou- dot. These methods make use of various spin-dependent
lomb blockade region, the bias window exactly equals energy terms. Each electron spin is first influenced di-
the energy-level spacing. Figure 5共c兲 shows the level rectly by an external magnetic field via the Zeeman en-
diagrams at these special positions for both ergy EZ = SzgBB, where Sz is the spin z component.
ES共N兲 ↔ GS共N + 1兲 and GS共N兲 ↔ ES共N + 1兲. Here the Moreover, the Pauli exclusion principle forbids two elec-
level spacings can be read off directly on the −兩e兩VSD trons with equal spin orientation to occupy the same
axis. orbital, thus forcing one electron into a different orbital.
We discuss the transition ES共N兲 ↔ ES共N + 1兲 that was This generally leads to a state with a different energy.
neglected in the discussion thus far. The visibility of such Finally, the Coulomb interaction leads to an energy dif-
a transition depends on the relative magnitudes of the ference 共the exchange energy兲 between states with sym-
tunnel rates and the relaxation rates. When the relax- metric and antisymmetric orbital wave functions. Since
ation is much faster than the tunnel rates, the dot will the total wave function of the electrons is antisymmetric,
effectively be in its ground state all the time and the the symmetry of the orbital part is linked to that of the
transition ES共N兲 ↔ ES共N + 1兲 can therefore never occur. spin.
In the opposite limit where the relaxation is much
slower than the tunneling, the transition ES共N兲 ↔ ES共N A. Spin filling derived from magnetospectroscopy
+ 1兲 participates in the electron transport and will be
visible in a plot like Fig. 5共c兲. Thus the visibility of tran- The spin filling of a quantum dot can be derived from
sitions can give information on the relaxation rates be- the Zeeman energy shift of the Coulomb peaks in a
magnetic-field. 共An in-plane magnetic-field orientation
6
is favored to ensure minimum disturbance of the orbital
Note that energy absorption from the environment can lead levels.兲 On adding the Nth electron, the z component Sz
to exceptions: photon-or phonon-assisted tunneling can give
rise to lines ending in the N = 0 Coulomb blockade region.
of the spin on the dot is either increased by 1 / 2 共if a
However, many experiments are performed at very low tem- spin-up electron is added兲 or decreased by 1 / 2 共if a spin-
peratures where the number of photons and phonons in ther- down electron is added兲. This change in spin is reflected
mal equilibrium is small. Therefore these processes are usually in the magnetic-field dependence of the electrochemical
negligible. potential 共N兲 via the Zeeman term
Eadd共N兲
=0 :↑,↑ or ↓,↓
B
= + gB :↑,↓ FIG. 6. Spin filling deduced from high-bias excited-state spec-
= − gB :↓,↑, troscopy. Schematic diagrams of dIDOT / dVSD in the 共VSD , VG兲
plane. 共a兲 Ground-state filling is spin up: a line corresponding
where the first 共second兲 arrow depicts the spin added in to an 共N + 1兲-electron ES, separated from GS共N + 1兲 by ⌬EZ,
the N − 2 → N − 1 共N − 1 → N兲 electron transition. Spin fill- terminates at the edge of the 共N + 1兲-electron Coulomb block-
ing of both vertical 共Sasaki et al., 1998兲 and lateral GaAs ade region 共point P兲. 共b兲 Ground-state filling is spin down: a
quantum dots 共Duncan et al., 2000; Lindemann et al., line corresponding to an N-electron ES, separated from GS共N兲
2002; Potok et al., 2003兲 has been determined using this by ⌬EZ, terminates at the N-electron Coulomb blockade re-
method, showing clear deviations from a simple Pauli gion 共point Q兲.
filling 共Sz alternating between 0 and 21 兲. Note that tran-
sitions where Sz of the ground state changes by more As we show below, these scenarios always correspond to
than 21 , which can occur due to many-body interactions ground-state filling with spin up and spin down, respec-
in the dot, can lead to a spin blockade of the current tively.
共Weinmann et al., 1995; Korkusiński et al., 2004兲. Consider an electron entering an empty orbital with
In circularly symmetric few-electron vertical dots, spin well-resolved spin splitting 关see Fig. 6共a兲兴. Here addition
states have been determined from the evolution of or- of a spin-up electron corresponds to the transition
bital states in a magnetic field perpendicular to the plane GS共N兲 ↔ GS共N + 1兲. In contrast, addition of a spin-down
of the dots. This indirect determination of the spin state electron takes the dot from GS共N兲 to ES共N + 1兲, which is
has allowed observation of a two-electron singlet-to- ⌬EZ higher in energy than GS共N + 1兲. Thus we expect a
triplet ground-state transition and a four-electron spin high-bias spectrum as in Fig. 6共a兲.
filling following Hund’s rule. For a review on these ex- Now consider the case where the 共N + 1兲th electron
periments, see Kouwenhoven et al. 共2001兲. Similar tech- moves into an orbital that already contains one electron
niques were also used in experiments on few-electron 关see Fig. 6共b兲兴. The two electrons need to have antipar-
lateral dots in both weak and strong magnetic fields allel spins, in order to satisfy the Pauli exclusion prin-
共Ciorga et al., 2000; Kyriakidis et al., 2002兲. ciple. If the dot is in the ground state, the electron al-
ready present in this orbital has spin up. Therefore the
electron added in the transition from GS共N兲 to GS共N
B. Spin filling derived from excited-state spectroscopy + 1兲 must have spin down. A spin-up electron can only
be added if the first electron has spin down, i.e., when
Spin filling can also be deduced from excited-state the dot starts from ES共N兲, ⌬EZ higher in energy than
spectroscopy without changing the magnetic field 共Cob- GS共N兲. The high-bias spectrum that follows is shown
den et al., 1998兲, provided the Zeeman energy splitting schematically in Fig. 6共b兲.
⌬EZ = 2兩EZ兩 = gBB between spin-up and spin-down elec- Comparing the two scenarios, we see that spin filling
trons can be resolved. This powerful method is based on has a one-to-one correspondence with the excited-state
the simple fact that any single-particle orbital can be spectrum: if the spin ES line terminates at the
occupied by at most two electrons due to Pauli’s exclu- 共N + 1兲-electron Coulomb blockade region 关as point P in
sion principle. Therefore as we add one electron to a dot Fig. 6共a兲兴, a spin-up electron is added to the GS; if, how-
containing N electrons, there are only two scenarios pos- ever, the spin ES line terminates at the N-electron Cou-
sible: either the electron moves into an empty orbital, or lomb blockade region 关as point Q in Fig. 6共b兲兴, a spin-
it moves into an orbital that already holds one electron. down electron is added to the GS.
The method is valid regardless of the spin of the 共Cronenwett et al., 1998; Goldhaber-Gordon et al., 1988兲.
ground states involved, as long as the addition of one If a magnetic field B drives the onset of these currents to
electron changes the spin z component of the ground values of VSD = ± gBB / 兩e兩, it follows that the ground
state by 兩⌬Sz兩 = 1 / 2. If 兩⌬Sz兩 ⬎ 1 / 2, the 共N + 1兲-electron state has nonzero spin. Since the processes in these cur-
GS cannot be reached from the N-electron GS by addi- rents can change the spin z component by at most 1, the
tion of a single electron. This would cause a spin block- absolute value of the spin cannot be deduced with this
ade of electron transport through the dot 共Weinmann et method, unless the spin is zero.
al., 1995兲. We end this section with some remarks on spin filling.
The parity of the electron number cannot be inferred
from spin filling unless the sequence of spin filling is
C. Other methods exactly known. For example, consider the case where
the electron added in the GS共N兲 → GS共N + 1兲 transition
If the tunnel rates for spin up and spin down are not has spin down. Then, if the dot follows an alternating
equal, the amplitude of the current can be used to de- 共Pauli兲 spin-filling scheme, N is odd. However, if there is
termine the spin filling. This method has been termed a deviation from this scheme such that GS共N兲 is a spin
spin-blockade spectroscopy. This name is slightly mis- triplet state 共total spin S = 1兲, then N is even.
leading as the current is not actually blocked, but rather Second, spin-filling measurements do not yield the ab-
assumes a finite value that depends on the spin orienta- solute spin of the ground states, but only the change in
tion of transported electrons. This method has been ground-state spin. However, by starting from zero elec-
demonstrated and utilized in the quantum Hall regime, trons 共and thus zero spin兲 and tracking the change in
where the spatial separation of spin-split edge channels spin at subsequent electron transitions, the total spin of
induces a large difference in the tunnel rates of spin-up the ground state can be determined 共Willems van Bev-
and spin-down electrons 共Ciorga et al., 2000, 2002; Kupi- eren et al., 2005兲.
dura et al., 2006兲. Spin-polarized leads can also be ob-
tained in moderate magnetic fields by changing the elec-
tron density near the dot with a gate. This concept was IV. SPIN STATES IN A SINGLE DOT
used to perform spin spectroscopy on a quantum dot
connected to gate-tunable quasi-one-dimensional chan- A. One-electron spin states
nels 共Hitachi et al., 2006兲.
Care must be taken when inferring spin filling from The simplest spin system is that of a single electron,
the amplitude of the current as other factors, such as the which can have one of only two orientations: spin up or
orbital spread of the wave function, can have a large, spin down. Let E↑,0 and E↓,0 共E↑,1 and E↓,1兲 denote the
even dominating influence on the current amplitude. A one-electron energies for the two spin states in the low-
prime example is the difference in tunnel rate between est 共first excited兲 orbital. With a suitable choice of the
the two-electron spin singlet and triplet states due to the zero of energy we arrive at the following electrochemi-
different orbital wave functions of these states. In fact, cal potentials:
this difference is large enough to allow single-shot read-
0↔↑,0 = E↑,0 , 共7兲
out of the two-electron spin state, as discussed in Sec.
VI.C.
0↔↓,0 = E↓,0 = E↑,0 + ⌬EZ , 共8兲
In zero magnetic field, a state with total spin S is 共2S
+ 1兲-fold degenerate. This degeneracy is reflected in the
0↔↑,1 = E↑,1 = E↑,0 + ⌬Eorb , 共9兲
current if the dot has strongly asymmetric barriers. As
an example, in the transition from a one-electron S
0↔↓,1 = E↓,1 = E↑,0 + ⌬Eorb + ⌬EZ , 共10兲
= 1 / 2 state to a two-electron S = 0 state, only a spin-up
electron can tunnel onto the dot if the electron that is where ⌬Eorb is the orbital level spacing.
already on the dot is spin down, and vice versa. How- Figures 7共a兲–7共f兲 show excited-state spectroscopy
ever, in the reverse transition 共S = 0 to S = 1 / 2兲, both elec- measurements on two devices A and B via electron
trons on the dot can tunnel off. Therefore the rate for transport at the N = 0 ↔ 1 transition, at different mag-
tunneling off the dot is twice the rate for tunneling onto netic fields B储 applied in the plane of the 2DEG. A clear
the dot. In general, the ratio of the currents in opposite splitting of both the orbital ground and first excited state
bias directions at the GS共N兲 ↔ GS共N + 1兲 transition is, is observed, which increases with increasing magnetic
for spin-independent tunnel rates and for strongly asym- field 共Hanson et al., 2003; Potok et al., 2003; Könemann
metric barriers, given by 关2S共N + 1兲 + 1兴 / 关2S共N兲 + 1兴 共Ak- et al., 2005; Willems van Beveren et al., 2005兲. The or-
era, 1999兲. Here S共N兲 and S共N + 1兲 denote the total spin bital level spacing ⌬Eorb in device A is about 1.1 meV.
of GS共N兲 and GS共N + 1兲, respectively. This relation can Comparison with Fig. 6 shows that a spin-up electron is
be used in experiments to determine the ground-state added to the empty dot to form the one-electron ground
total spin 共Cobden et al., 1998; Hayashi et al., 2003兲. state, as expected.
Information on the spin of the ground state can also In Fig. 7共g兲 the Zeeman splitting ⌬EZ is plotted as
be found from 共inelastic兲 cotunneling currents 共Kogan et function of B储 for the same two devices A and B which
al., 2004兲 or the current due to a Kondo resonance are made on different heterostructures. These measure-
FIG. 7. Measurement of the one-electron spin states. 共a兲–共f兲 Excited-state spectroscopy on two devices: device A is fabricated on
a heterostructure with the 2DEG at 90 nm below the surface and device B with the 2DEG at 60 nm below the surface. Differential
conductance dIDOT / dVSD is plotted as a function of VSD and gate voltage near the 0 ↔ 1 electron transition, for in-plane magnetic
fields 共as indicated in top-right corners兲. Darker corresponds to larger dIDOT / dVSD. Data on device A show spin splitting in both
the orbital ground and first excited state; data on device B only display the orbital ground state. 共g兲 Zeeman splitting ⌬EZ as a
function of B extracted from 共a兲 to 共f兲 and similar measurements. Gray solid lines are fits to the data. Dashed line shows ⌬EZ
expected for the bulk GaAs g factor of −0.44. Data adapted from Hanson et al., 2003, and Willems van Beveren et al., 2005.
ments allow a straightforward determination of the elec- 兩T0典 = 共兩 ↑ ↓ 典 + 兩 ↓ ↑ 典兲 / 冑2, and Sz = −1 for 兩T−典 = 兩 ↓ ↓ 典.
tron g factor. The measured g factor can be affected by Using the constant interaction model, the energies of
共i兲 extension of the electron wave function into the the states can be expressed in terms of the single-particle
Al0.3Ga0.7As region, where g = + 0.4 共Snelling et al., 1991; energies of the two electrons plus a charging energy EC
Salis et al., 2001兲; 共ii兲 thermal nuclear polarization, which which accounts for the Coulomb interactions:
decreases the effective magnetic field through the hyper-
fine interaction 共Meier and Zakharchenya, 1984兲; 共iii兲 US = E↑,0 + E↓,0 + EC = 2E↑,0 + ⌬EZ + EC ,
dynamic nuclear polarization due to electron-nuclear
flip-flop processes in the dot, which enhances the effec- UT+ = E↑,0 + E↑,1 − EK + EC
tive magnetic field 共Meier and Zakharchenya, 1984兲; 共iv兲
the nonparabolicity of the GaAs conduction band 共Snel- = 2E↑,0 + ⌬Eorb − EK + EC
ling et al., 1991兲; 共v兲 the spin-orbit coupling 共Falko et al., = 2E↑,0 + EST + EC ,
2005兲; and 共vi兲 the confinement potential 共Hermann and
Weisbuch, 1977; Björk et al., 2005兲. The effect of the
UT0 = E↑,0 + E↓,0 + EST + EC
nuclear field on the measured g factor is discussed in the
Appendix. More experiments are needed to separate = 2E↑,0 + ⌬Eorb − EK + ⌬EZ + EC
these effects, e.g., by measuring the dependence of the g
factor on the orientation of the in-plane magnetic field = 2E↑,0 + EST + ⌬EZ + EC ,
with respect to the crystal axis 共Falko et al., 2005兲.
UT− = 2E↓,0 + EST + EC
= 2E↑,0 + ⌬Eorb − EK + 2⌬EZ + EC
B. Two-electron spin states
= 2E↑,0 + EST + 2⌬EZ + EC ,
The ground state of a two-electron dot in zero mag-
netic field is always a spin singlet 共total spin quantum with EST denoting the singlet-triplet energy difference in
number S = 0兲 共Ashcroft and Mermin, 1974兲, formed by the absence of the Zeeman splitting ⌬EZ: EST = ⌬Eorb
the two electrons occupying the lowest orbital with their − E K.
spins antiparallel: 兩S典 = 共兩 ↑ ↓ 典 − 兩 ↓ ↑ 典兲 / 冑2. The first excited We first consider the case of an in-plane magnetic field
states are the spin triplets 共S = 1兲, where the antisymme- B储. Here EST is almost independent of B储 and the ground
try of the total two-electron wave function requires one state remains a spin singlet for all fields attainable in the
electron to occupy a higher orbital. Both the antisymme- lab. The case of a magnetic field perpendicular to the
try of the orbital part of the wave function and the oc- plane of the 2DEG will be treated below.
cupation of different orbitals reduce the Coulomb en- Figure 8共a兲 shows the possible transitions between the
ergy of the triplet states with respect to the singlet with one-electron spin-split orbital ground state and the two-
two electrons in the same orbital 共Kouwenhoven et al., electron states. The transitions ↑ ↔ T− and ↓ ↔ T+ are
2001兲. We include this change in Coulomb energy by the omitted, since these require a change in the spin z com-
energy term EK. The three triplet states are degenerate ponent of more than 21 and are thus spin blocked 共Wein-
at zero magnetic field, but acquire different Zeeman en- mann et al., 1995兲. From the energy diagram the follow-
ergy shifts EZ in finite magnetic fields because their spin ing electrochemical potentials can be deduced 关see Fig.
z components differ: Sz = + 1 for 兩T+典 = 兩 ↑ ↑ 典, Sz = 0 for 8共b兲兴:
FIG. 8. 共Color online兲 Measurement of the two-electron spin states. 共a兲 Energy diagram schematically showing the energy levels
of the one- and two-electron states. The allowed transitions between these levels are indicated by arrows. 共b兲 Electrochemical
potential ladder corresponding to the transitions shown in 共a兲, using the same color coding. Changing the gate voltage shifts the
ladder as a whole. Note that the three triplet states appear at only two values of the electrochemical potential. 共c兲 Energetically
allowed 1 ↔ 2 electron transitions as a function of VSD and VG. The lines corresponding to ↑ ↔ S outline the region of transport;
outside this region, where lines are dashed, the dot is in Coulomb blockade. 共d兲 dIDOT / dVSD as a function of VG and VSD around
the 1 ↔ 2 electron transition at B储 = 12 T in device A. The regions labeled with letters A–F correspond well to those in 共c兲. In the
region labeled A only spin-down electrons pass through the dot. Data adapted from Hanson, Vandersypen, et al., 2004.
↑,0↔S = E↑,0 + ⌬EZ + EC , each transition, the two lines originating at VSD = 0 span
a V-shaped region where the corresponding electro-
↑,0↔T+ = E↑,0 + EST + EC , chemical potential is in the bias window. In the region
labeled A, only transitions between the one-electron
↑,0↔T0 = E↑,0 + EST + ⌬EZ + EC , ground state 兩 ↑ , 0典 and the two-electron ground state 兩S典
are possible, since only ↑,0↔S is positioned inside the
bias window. In the other regions several more transi-
↓,0↔S = E↑,0 + EC ,
tions are possible which leads to a more complex, but
still understandable, behavior of the current. Outside
↓,0↔T0 = E↑,0 + EST + EC ,
the V-shaped region spanned by the ground-state transi-
tion ↑,0↔S, Coulomb blockade prohibits first-order elec-
↓,0↔T− = E↑,0 + EST + ⌬EZ + EC . tron transport.
Note that ↑,0↔T+ = ↓,0↔T0 and ↑,0↔T0 = ↓,0↔T−. Con- Experimental results from device A, shown in Fig.
sequently, the three triplet states change the first-order 8共d兲, are in excellent agreement with the predictions of
transport through the dot at only two values of VSD. The Fig. 8共c兲. Comparison of the data with Fig. 6 indicates
reason is that the first-order transport probes the energy that indeed a spin-down electron is added to the one-
difference between states with successive electron num- electron 共spin-up兲 ground state to form the two-electron
ber. In contrast, the onset of second-order 共cotunneling兲 singlet ground state. From the data the singlet-triplet
currents is governed by the energy difference between energy difference EST is found to be ⬇520 eV. The fact
states with the same number of electrons. Therefore the that EST is about half the single-particle level spacing
triplet states change the second-order 共cotunneling兲 cur- 共⌬Eorb = 1 meV兲 indicates the importance of Coulomb
rents at three values of VSD if the ground state is a interactions. The Zeeman energy, and therefore the g
singlet7 共Paaske et al., 2006兲. factor, is found to be the same for the one-electron
In Fig. 8共c兲 we map out the positions of the electro- states as for the two-electron states 共within the measure-
chemical potentials as a function of VG and VSD. For
ment accuracy of ⬇5%兲 on both devices A and B. We
note that the large variation in differential conductance
7
If the ground state is a triplet, the cotunneling current only observed in Fig. 8共d兲 can be explained by a sequential
changes at two values of VSD 共0 and ⌬EZ / 兩e兩兲, due to spin tunneling model with spin- and orbital-dependent tunnel
selection rules. rates 共Hanson, Vink, et al., 2004兲.
electron temperature 共smaller ␣兲 and by making the the reservoir ⌫T is much larger than the rate from the
charge measurement faster 共smaller 兲. singlet state ⌫S, i.e., ⌫T Ⰷ ⌫S 共Hanson, Vink, et al., 2004兲.
The first all-electrical single-shot readout of an elec- The TR-RO has been tested experimentally in Han-
tron spin has thus been performed using ERO. How- son et al. 共2005兲 by applying gate voltage pulses as de-
ever, this scheme has a few drawbacks: 共i兲 ERO requires picted in Fig. 17共a兲. Figure 17共b兲 shows the expected re-
an energy splitting of the spin states larger than the ther- sponse of IQPC to the pulse, and Fig. 17共c兲 depicts the
mal energy of the electrons in the reservoir. Thus for a level diagrams in the three different stages. Before the
single spin the readout is only effective at very low elec- pulse starts, there is one electron on the dot. Then, the
tron temperature and high magnetic fields 共kBT Ⰶ ⌬EZ兲. pulse pulls the levels down so that a second electron can
Also, interesting effects occurring close to degeneracy, tunnel onto the dot 共N = 1 → 2兲, forming either a singlet
e.g., near the singlet-triplet crossing for two electrons, or a triplet state with the first electron. The probability
cannot be probed. 共ii兲 Since the ERO relies on precise that a triplet state is formed is given by 3⌫T / 共⌫S + 3⌫T兲,
positioning of the spin levels with respect to the reser- where the factor of 3 is due to the degeneracy of the
voir, it is very sensitive to fluctuations in the electrostatic triplets. After a variable waiting time twait the pulse ends
potential. Background charge fluctuations 共Jung et al.,
2004兲 can easily push the levels out of the readout con-
figuration. 共iii兲 High-frequency noise can spoil the ERO
by inducing photon-assisted tunneling from the spin
ground state to the reservoir 共Onac et al., 2006兲. Since
the QPC is a source of shot noise, this limits the current
through the QPC and thereby the bandwidth of the
charge detection 共Vandersypen et al., 2004兲. These con-
straints have motivated the search for a different
method for spin-to-charge conversion, and have led to
the demonstration of the tunnel-rate-selective readout
共TR-RO兲 which we treat in the next section.
qជ j
具T±q⬘兩HSO兩Sq典 He,ph = Mqជ jeiqជ rជ共bq†ជ j + bqជ j兲, 共23兲
兩T±q典共1兲 = 兩T±q典 + 兺 ESq⬘ − ET±q
兩Sq⬘典
q⬘⫽q
where Mqជ j is a measure of the electric-field strength of a
具T±q⬘兩HSO兩T0q典
+ 兺 E T0q⬘ − E T±q
兩T0q⬘典, 共21兲 phonon with wave vector qជ and phonon branch j 共one
q⬘⫽q longitudinal and two transverse modes兲, rជ is the position
vector of the electron, and bq†ជ j and bqជ j are the phonon
where q is shorthand for the quantum numbers n1l1n2l2 creation and annihilation operators, respectively.
that label the orbital for each of the two electrons. It can The relaxation rate thus depends on the phonon den-
be seen from inspection of the spin-orbit Hamiltonian sity of states at the spin-flip energy 共the phonons have to
and the form of the wave functions that many of the carry away the energy兲, and on how strongly the
matrix elements in these expressions are zero. A more electron-phonon coupling connects the spin-orbit per-
detailed discussion is beyond the scope of this review turbed spin states 关see Eq. 共22兲兴. The latter in turn de-
but can be found in Climente et al. 共2007兲 and Golovach pends on 共i兲 the degree of admixing between spin and
et al. 共2007兲. orbital states 关see Eqs. 共17兲 and 共18兲兴, 共ii兲 the electric-
field strength of a single phonon 共⬀Mqជ j兲, 共iii兲 the effec-
tiveness of phonons at coupling different dot orbitals,
4. Relaxation via the phonon bath
via eiqជ ·rជ, and 共iv兲 the phonon occupation, via 共bq†ជ j + bqជ j兲. In
Electric fields cannot cause transitions between pure addition, 共v兲 we will show that an external magnetic field
spin states. However, we have seen that the spin-orbit is necessary for spin relaxation to occur. We next discuss
interaction perturbs the spin states and the eigenstates each of these elements separately, starting with the den-
become admixtures of spin and orbital states, see Eqs. sity of states.
共17兲–共21兲. These new eigenstates can be coupled by elec- The phonons are taken to be bulk phonons in most
tric fields 共see Fig. 20兲, and electric-field fluctuations can discussions of relaxation in GaAs quantum dots. This
lead to spin relaxation 共Khaetskii and Nazarov, 2000, may not be fully accurate since the dot is formed at a
2001; Woods et al., 2002兲. As we will see, this indirect heterointerface, and furthermore is in close vicinity to
mechanism is not very efficient, and accordingly very the surface 关e.g., surface acoustic waves have also been
long spin-relaxation times have been observed experi- observed to couple to dots, when explicitly excited
mentally 共Fujisawa et al., 2001b, 2002a; Hanson et al., 共Naber et al., 2006兲兴. Nevertheless, this simplification has
2003, 2005; Elzerman, Hanson, Willems van Beveren, worked reasonably well so far for explaining observa-
Witkamp, et al., 2004; Kroutvar et al., 2004; Amasha et tions of relaxation in dots 共Fujisawa et al., 1998; Krout-
al., 2006; Sasaki et al., 2006; Meunier et al., 2007兲. var et al., 2004; Amasha et al., 2006; Meunier et al., 2007兲.
In general, fluctuating electric fields could arise from In what follows, we therefore consider bulk phonons
many sources, including fluctuations in the gate poten- only. Furthermore, we only include acoustic phonons, as
tials, background charge fluctuations or other electrical the energies for optical phonons are much higher than
noise sources 共Marquardt and Abalmassov, 2005; typical spin-flip energies 共Ashcroft and Mermin, 1974兲.
Borhani et al., 2006兲. However, as we shall see, it appears Since bulk acoustic phonons have a linear dispersion re-
that in carefully designed measurement systems, the lation at low energies 共Ashcroft and Mermin, 1974兲, the
electric-field fluctuations of these extraneous noise phonon density of states increases quadratically with en-
sources is less important than those caused by the pho- ergy.
non bath. Phonons can produce electric-field fluctua- 共i兲 The degree of admixing between spin and orbitals
tions in two ways. First, so-called deformation potential obviously scales with the spin-orbit coupling parameters
phonons inhomogeneously deform the crystal lattice, ␣ and . Since the spin-orbit interaction is anisotropic
thereby altering the band gap in space, which gives rise 共␣ and  can add up or cancel out depending on the
to fluctuating electric fields. This mechanism occurs in magnetic-field orientation with respect to the crystal
all semiconductors. Second, in polar crystals such as axis兲, the admixing and hence the relaxation rate are
GaAs, also homogeneous strain leads to electric fields, anisotropic as well 共Falko et al., 2005兲. Furthermore, the
through the piezoelectric effect 共piezoelectric phonons兲. admixing depends on how close together in energy the
The phonon-induced transition rate between the relevant orbitals are 关see Eqs. 共17兲–共21兲兴. At an avoided
renormalized states 兩n , l , ↑ 典共1兲 and 兩n , l , ↓ 典共1兲 is given by crossing of two levels caused by the spin-orbit interac-
Fermi’s golden rule 共an analogous expression can be de- tion, the admixing will be complete 共Bulaev and Loss,
rived for relaxation from triplet to singlet states, or be- 2005; Stano and Fabian, 2005, 2006兲.
tween other spin states兲: 共ii兲 The electric field associated with a single phonon
scales as 1 / 冑q for piezoelectric phonons and as 冑q for
2
⌫= 兺 円 共1兲具nl↑兩He,ph兩nl↓典共1兲円2D共⌬EZ共1兲兲,
ប n,l
共22兲 deformation potential phonons, where q is the phonon
wave number. This difference can be understood from
the fact that small phonon energies correspond to long
where D共E兲 is the phonon density of states at energy E. wavelengths, and therefore nearly homogeneous crystal
He,ph is the electron-phonon coupling Hamiltonian, strain, which can only create electric fields through the
given by piezoelectric effect. At sufficiently small energies 共below
冉兺 冊
action, there is no pure phase randomization of the elec- N
tron spin, such that in fact T2 = 2T1 共Golovach et al., AkIជk Sជ = gBB
ជ Sជ . 共27兲
N
2004兲. For a magnetic field perpendicular to the plane of k
the 2DEG, this can be understood from the form of the
spin-orbit Hamiltonian. Both the Dresselhaus contribu- When this nuclear field assumes a random, unknown
tion, Eq. 共13兲, and the Rashba contribution, Eq. 共15兲, value, the electron spin will subsequently evolve in a
only contain x and y terms. With B along ẑ, these random way and thus end up in a statistical mixture of
terms lead to spin flips but not to pure phase random- states as well, just like in the quantum-mechanical de-
ization. However, this intuitive argument does not cap- scription.
ture the full story: for B0 along x̂, one would expect the The semiclassical description of nuclear spins yields
x term to contribute to pure phase randomization, but an intuitive picture of the electron-nuclear dynamics and
surprisingly, in leading order in the spin-orbit interac- is sufficient to explain all experimental observations dis-
tion, there is still no pure randomization even with an cussed in this review. However, we note that the full
in-plane magnetic field 共Golovach et al., 2004兲. quantum description is required to analyze correlations
between microscopic nuclear spin states and the single
electron spin state, as, e.g., in a study of the entangle-
B. Hyperfine interaction ment between electron and nuclear spins.
1. Origin The magnitude of the nuclear field BN = 兺kNAkIជk / gB
is maximum when all nuclear spins are fully polarized.
The spin of an electron in an atom can interact with
the spin of “its” atomic nucleus through the hyperfine In GaAs, BN,max is about 5 T 共Paget et al., 1977兲. For any
coupling. An electron spin in a quantum dot, in contrast, given host material, this value is independent of the
may interact with many nuclear spins in the host mate- number of nuclei N that the electron overlaps with—for
rial 共Fig. 24兲. The Hamiltonian for the Fermi contact larger numbers of nuclei, the contribution from each
hyperfine interaction is then given by nuclear spin to BN is smaller 共the typical value for Ak is
proportional to 1 / N兲.
N
This is distinctly different in the case of 共nearly兲 un-
HHF = 兺 AkIជkSជ , 共26兲 polarized nuclear spins, for instance, nuclear spins in
k
thermodynamic equilibrium under typical experimental
where Iជk and Sជ are the spin operator for nucleus k and conditions. First there is a small average nuclear polar-
the electron spin, respectively 共Abragam, 1961; Meier ization, oriented along the external magnetic field and
and Zakharchenya, 1984; Abragam and Bleaney, 1986; with an amplitude given by the Boltzman distribution
Slichter, 1990兲. Since the electron wave function is inho- 共see the Appendix兲. In addition, there is a statistical fluc-
mogeneous, the coupling strength Ak between each tuation about the average, analogous to the case of N
nucleus k and the electron spin varies, as it is propor- coin tosses. For an electron spin interacting with N
tional to the overlap squared between the nucleus and nuclear spins 1 / 2, the root-mean-square value of the sta-
the electron wave function. tistical fluctuation will be BN,max / 冑N T 共Khaetskii et al.,
This asymmetric situation combined with fast 2002; Merkulov et al., 2002兲. This quantity has recently
electron-spin dynamics and slow nuclear-spin dynamics been measured in various semiconductor quantum dots,
gives rise to a subtle and complex many-body quantum- both optically 共Braun et al., 2005; Dutt et al., 2005兲 and
mechanical behavior, whereby nuclear spins affect the electrically 共Johnson, Petta, Taylor, et al., 2005; Koppens
electron-spin time evolution, and the electron spin in et al., 2005兲, giving values in the range of a few mT, as
turn acts back on the dynamics of each of the nuclei. expected since N ⬇ 106 in these dots. Similar values were
Since both nuclear spins and the localized electron spin obtained earlier for electrons bound to shallow donors
are quantum objects, the hyperfine coupling could in in GaAs 共Dzhioev et al., 2002兲.
principle create entanglement between them 关if both the A few comments on the importance of the host mate-
electron spin and nuclear spins had a sufficiently pure rial are in order. First, the value of Ak is typically smaller
initial state; see Braunstein et al., 1999兴. For the electron for lighter nuclei. Second, for particles in p-like orbitals,
spin, this interaction with uncontrolled degrees of free- such as holes in GaAs, the wave function has almost no
dom in the environment leads to decoherence 共Khaetskii overlap with the nuclei 共only s orbitals have a finite am-
et al., 2002, 2003; Merkulov et al., 2002; Coish and Loss, plitude at the nucleus兲, so the Fermi contact hyperfine
free evolution of the spin can be measured by tipping flip energy 共Erlingsson et al., 2001; Erlingsson and Naz-
the spin into the x-y plane, subsequently allowing the arov, 2002, 2004; Abalmassov and Marquardt, 2004兲.
spin to freely evolve about Bជ0 共assumed to be along ẑ兲, Whereas the transition amplitude due to the spin-orbit
and recording the magnetization in this plane as a func- interaction vanishes in lowest order at B0 = 0 共see discus-
tion of the free evolution time interval 关in NMR, this is sion in Sec. VII.A.4兲, this is not the case for hyperfine
known as the free induction decay 共FID兲兴. If the spin can mediated transitions, so the hyperfine mechanism will be
relatively more important at low magnetic fields.
only be measured in the ±ẑ basis, a so-called Ramsey
experiment should be performed instead. It starts off
like an FID but the magnetization is rotated back to the 3. Mechanisms and time scales of nuclear field fluctuations
ẑ axis after the free evolution time interval, so it can be
We have seen that the nuclear field only leads to a loss
measured along ẑ. Averaging each data point in an FID of spin coherence because it is random and unknown—if
or Ramsey experiment over a sufficiently long time, is
Bជ were fixed in time, we could simply determine its
equivalent to averaging over a large number of uncorre- N
lated nuclear field values 共assuming the system is er- value and the uncertainty would be removed. We discuss
godic兲. Such experiments have recently been performed here on what time scale the nuclear field actually fluctu-
共see Sec. IX兲, and gave the expected short time scales for ates. This time scale is denoted by tnuc.
T*2. The study of nuclear dynamics due to internuclear
Also in the case of driven evolution, the nuclear field and electron-nuclear interactions has a long and rich his-
will affect the time evolution. In a spin-resonance ex- tory 共Abragam, 1961; Meier and Zakharchenya, 1984;
Abragam and Bleaney, 1986; Slichter, 1990兲. When ap-
periment, for instance, a rotating magnetic field B1 is
plied to quantum dots, theory predicts that the two most
applied with frequency gBB0 / h 共on-resonance with the
important mechanisms responsible for fluctuations in
Zeeman splitting兲, and perpendicular to Bជ0 共see also Sec. the nuclear field are the internuclear magnetic dipole-
IX.A兲. In the usual rotating reference frame, this corre- dipole interaction 共de Sousa and Das Sarma, 2003a,
sponds to a rotation about the B1 axis. However, a lon- 2003c; Witzel and Rogerio de Sousa, 2005; Yao et al.
gitudinal nuclear field will shift the electron-spin reso- 2005兲 and the electron-nuclear hyperfine interaction
nance frequency, so that B1 is no longer on-resonance 共Khaetskii et al., 2002; Coish and Loss, 2004; Shenvi and
with the electron-spin precession. In the rotating frame, Rogerio de Sousa, 2005兲.
the spin will then rotate about the vector sum of B1 and The Hamiltonian describing magnetic dipole-dipole
BzN 关Fig. 26共b兲兴, which may be a rather different rotation interactions between neighboring nuclei is of the form
冉 冊
than intended. In fact, the nuclear field has been the
0gigj2Nប ជ ជ 3 ជ
main limitation on the fidelity of spin rotations in recent HDD = 兺 Ii · Ij − 共Ii · rជij兲共Iជj · rជij兲 ,
electron-spin resonance experiments in a quantum dot i⬍j 4兩rជij兩 3
兩rជij兩2
共see Sec. IX.A兲. 共29兲
We have so far focused on the effect of the nuclear
field 共mainly BN z
兲 on the electron-spin phase. We now where 0 is the permeability of free space, gi is the g
turn to electron-spin flips caused by the nuclear field factor of nucleus i, N is the nuclear magneton, and rជij is
共mainly by Bx,y N 兲. The semiclassical picture says that for
the vector connecting the two nuclei. The strength of the
B0 Ⰶ Bx,y the electron spin will rotate about Bx,y effective magnetic dipole-dipole interaction between
N N , i.e., it is
changed from spin up to spin down and back, while for neighboring nuclei in GaAs is about 共100 s兲−1 共Shul-
B0 Ⰷ Bx,y man et al., 1958兲. In strong magnetic fields, we can dis-
N , this hardly occurs 共see Fig. 25兲. We arrive at a
similar conclusion from the quantum-mechanical pic- card the nonsecular part of this Hamiltonian, and retain
ture: the hyperfine Hamiltonian, Eq. 共26兲, permits direct sec
HDD,ij ⬀ Iជi · Iជj − 3Izi Izj = Ixi Ixj + Iyi Iyj − 2Izi Izj
electron-nuclear flip-flops only when the two relevant
electron-spin states are very close in energy 共since a = 共I+i I−j + I−i I+j − 4Izi Izj 兲/2 共30兲
nuclear-spin flip can absorb only a small amount of en-
ergy兲. This effect has been observed in recent experi- for the coupling term between nuclear spins i and j of
ments on two-electron singlet and triplet states in a the same species 共for coupling between spins of different
double quantum dot 共Johnson, Petta, Taylor, et al., 2005兲 isotopes, only the Izi Izj term survives at high field兲. Here
共Sec. VIII.D兲. I± are the nuclear spin raising and lowering operators.
There still is another contribution from Bx,y The Izi Izj terms in Eq. 共30兲 are responsible for changing
N to spin
flips 共i.e., to T1兲. Since the nuclear field strength and BxN and ByN. This may occur on the 100 s time scale.
orientation depend on the collection of nuclear spins The flip-flop terms Ixi Ixj + Iyi Iyj affect BN
z
, but the flip-flop
that the electron wave function overlaps with, BN de- rate between nuclei i and i + 1 may be suppressed,
pends on the orbital the electron occupies. As a result, namely when 兩Ai − Ai+1兩 is greater than the internuclear
like the spin-orbit interaction 共see Sec. VII.A兲, the hy- coupling strength 共Deng and Hu, 2005兲 共as this causes an
perfine interaction also leads to admixing of spin and energy mismatch兲. Thus when we consider the dipolar
orbital states. Here too phonons can induce transitions N evolves on a 100 s time scale, but
interaction only, Bx,y
between the perturbed spin states, and absorb the spin- BzN may evolve more slowly.
We now turn to the hyperfine interaction. So far we Now suppose that we do know the orientation and
only considered its effect on the localized electron spin, strength of the nuclear field exactly at time t = 0, but that
but naturally the interaction 关Eq. 共26兲兴 works both ways the nuclear spin bath subsequently evolves in a random
and the nuclei evolve about the electron spin, just like fashion on a time scale tnuc, as described in the previous
the electron spin evolves about the nuclear field. The subsection. On what time scale T2 will the phase of the
apparent field experienced by the nuclei is called the electron spin then be randomized?
Knight shift, and it has a strength Ak ⬇ 共10 s兲−1 共Kha- It may come as a surprise at first that T2 is not simply
etskii et al., 2002; Merkulov et al., 2002; Coish and Loss, the same or even of the same order as tnuc. The reason is
2004兲 共the N nuclei with which the electron wave func- that T2 depends not only on the time scale of the nuclear
tion overlaps share the total coupling strength A兲. When field fluctuations 共tnuc兲, but also on the amplitude and
we look at the hyperfine interaction Hamiltonian, Eq. stochastics of the fluctuations. The typical amplitude is
共26兲, we see that similar to the internuclear dipole-dipole given by the width of the nuclear field distribution,
interaction, it contains Izi Sz terms as well as flip-flop which can be expressed in terms of 1 / T*2. Examples of
terms: different stochastic models include Gaussian noise and
N Lorentzian noise, which lead to distinct decoherence
HHF = 兺 Ak共IkxSx + IkySy + IkzSz兲 characteristics 共Klauder and Anderson, 1962; de Sousa,
k 2006兲. The actual value of T2 is difficult to calculate ex-
N actly, but can be estimated in various regimes to be
= 兺 Ak共Ik+S+ + Ik−S− + 2IkzSz兲/2, 共31兲 1 – 100 s.
k The time scale T2 is also hard to obtain experimen-
where S± are the electron spin raising and lowering op- tally. In principle T2 could be determined by recording
erators. The transverse component of the nuclear field an FID or Ramsey decay, whereby BzN is reset to the
N will evolve due to the Ii S terms, on a 10 s time
Bx,y z z same initial value for every data point. This may require
z
scale. BN will change on the same time scale only near measuring BzN accurately and quickly, i.e., better than
B0 = 0, due to the electron-nuclear flip-flop components the initial uncertainty in BzN and in a time much shorter
in Eq. 共31兲. At finite B0, the energy mismatch between than tnuc 共Giedke et al., 2006; Klauser et al., 2006;
the electron and nuclear Zeeman energies suppresses Stepanenko et al., 2006兲. Alternatively, T2 could be ob-
electron-nuclear flip-flops, so here BzN cannot change by tained by recording all the data points needed to con-
direct electron-nuclear flip-flops. struct an FID or Ramsey experiment within a time short
The hyperfine interaction can also affect BzN indirectly. compared to tnuc.
Two virtual electron-nuclear flip-flops 共between one Experimentally, it may be much easier to obtain a
nucleus and the electron and between the electron and spin-echo decay time Techo, well known from NMR
another nucleus兲 can together lead to a nuclear-nuclear 共Freeman, 1997; Vandersypen and Chuang, 2004兲. In its
flip-flop 共Shenvi and Rogerio de Sousa, 2005; Yao et al., simplest form, the Hahn echo, the random time evolu-
2005; Deng and Hu, 2006兲. Such a flip-flop process be- tion that takes place during a certain time interval , is
tween two nuclei i and j modifies BzN whenever Ai ⫽ Aj. reversed during a second time interval of the same du-
This virtual electron-nuclear flip-flop process continues ration, by applying a so-called echo pulse 共180° rotation兲
to be effective up to much higher B0 than real electron- in between the two time intervals. Importantly, this un-
nuclear flip-flops. Eventually it is suppressed at high B0 winding of random dephasing only takes place to the
as well. extent that the random field causing it is constant for the
Altogether the dipole-dipole and hyperfine interac- duration of the entire echo sequence. Thus the slow time
tions are expected to lead to moderate time scales evolution of the nuclear field implies that the echo will
共10– 100 s兲 for Bx,y
N fluctuations. At low B0, the time
not be complete. We call the time scale of the remaining
scale for BzN fluctuations is similar, but at high B0, BzN loss of phase coherence Techo.
fluctuations are very slow. Here tnuc is certainly longer Like T2, Techo is much longer than T*2 but also much
than 10– 100 s and perhaps longer than a second. This shorter than tnuc. For example, if nuclear field fluctua-
still needs to be confirmed experimentally, but an indi- tions had Gaussian noise characteristics, the electron-
cation that tnuc may indeed be very long is that the decay spin coherence in a Hahn echo experiment would decay
共due to spin diffusion兲 of nuclear polarization built up 2 兲 共Herzog and Hahn, 1956兲. Taking
as exp共−t3 / tnucT*2
locally at a quantum dot or impurity occurs on a time T*2 = 10 ns and tnuc = 10 s, we obtain a T2 of 10 s, much
scale of seconds to minutes 共Paget, 1982; Hüttel et al., faster than tnuc itself. Nuclear field fluctuations may not
2004; Koppens et al., 2005兲 共see Sec. VIII.D兲. be characterized exactly by Gaussian noise, but never-
theless, predictions for T2 still range from 1 to 100 s,
with contributions from the internuclear dipole-dipole
4. Electron-spin decoherence in a fluctuating nuclear field
interaction 共de Sousa and Das Sarma, 2003a; Witzel and
In Sec. VII.B.2, we saw that we lose our knowledge of Rogerio de Sousa, 2005; Yao et al., 2005兲, the electron-
the electron-spin phase after a time T*2, in case the nuclear hyperfine interaction 共Khaetskii et al., 2002;
nuclear field orientation and strength are unknown. Coish and Loss, 2004兲, and indirect nuclear-nuclear in-
teractions, mediated by the hyperfine coupling 共Shenvi 1.75 T, T1 has been measured to be 170 ms. As B0 fur-
and Rogerio de Sousa, 2005; Yao et al., 2005; Deng and ther increases, the phonon density of states increases
Hu, 2006兲. Also, contrary to the usual case, the echo and phonons couple more efficiently to the dot orbitals
decay is not well described by a single exponential. The 共the phonon wavelength gets closer to the dot size兲, so at
predicted form for the echo decay depends on the some point relaxation becomes faster again and T1 de-
magnetic-field strength, and on what terms in the Hamil- creases with field. At 14 T, a 120-s T1 has been ob-
tonian are then important, but can be very complex served. At still higher fields, the phonon wavelength
共Coish and Loss, 2004; Yao et al., 2005; de Sousa, 2006兲. would become shorter than the dot size, and T1 is once
The usefulness of the echo technique for effectively more expected to go up with field.
obtaining an extended coherence time has been demon- Phase coherence is lost on much shorter time scales.
strated experimentally with two electron spins in a Rapid dephasing of the electron spin results from the
double quantum dot, whereby a lower bound on Techo of uncertainty in the nuclear field, T*2 ⬇ 10 ns, irrespective
1 s was obtained at 100 mT 共Petta, Johnson, Taylor, et of B0. If the uncertainty in the nuclear field is removed
al., 2005兲 共Sec. IX.B兲. Similar echolike decay times were or if the resulting unknown time evolution is unwound,
observed in optical measurements on an ensemble of we recover T2 or Techo, respectively, which are much
quantum dots that each contain a single-electron spin longer. Phase randomization of the electron spin then
共Greilich, Yakovlev, et al., 2006兲. results from 共slow兲 fluctuations in the nuclear field,
We note that sometimes a distinction is made between which occur on a time scale of 100 s to perhaps sec-
“dephasing,” referring to a loss of phase coherence that onds, and should lead to a T2 or Techo of 1 – 100 s. In-
can be reversed with echo techniques, and “decoher- deed, a lower bound on Techo of 1 s was experimentally
ence,” referring to a loss of phase coherence that cannot observed at 100 mT. If the effect of the nuclear field on
be reversed. While this distinction is useful in practice, the electron-spin coherence could be suppressed, the
we note that it is also somewhat artificial, in the sense
spin-orbit interaction would limit T2, to a value of 2T1
that any time evolution can in principle be reversed by a
共to first order in the spin-orbit interaction兲, which, is as
sufficiently rapid sequence of multiple generalized echo
we have seen, a very long time.
pulses 共Augustine and Hahn, 1997; Viola and Lloyd,
1998; Viola et al., 1999兲.
Finally, we point out that it may be possible to extend VIII. SPIN STATES IN DOUBLE QUANTUM DOTS
tnuc, i.e., to 共almost兲 freeze the nuclear field fluctuations.
One possibility to do this is to fully polarize the nuclear In this section, we discuss the spin physics of double
spins: if all nuclear spins point the same way, nuclear- quantum dots. We start by describing the properties of
nuclear flip-flop processes can no longer take place and “spinless” electrons. Then, we show how the spin selec-
also electron-nuclear flip-flops can only have a very tion rules can lead to a blockade in electron transport
small effect 共Khaetskii et al., 2002, 2003; Schliemann et through the double dot. Finally, we describe how this
al., 2002兲. For this approach to be effective, the nuclear- spin blockade is influenced by the hyperfine interaction
spin polarization must be really very close to 100% with the nuclear spins, and discuss the resulting dynam-
共Schliemann et al., 2002兲 just 90% polarization hardly ics.
helps. At present the highest nuclear-spin polarizations
reached in quantum dots are 60%, via optical pumping
共Bracker et al., 2005兲. Certainly other mechanisms for A. Electronic properties of electrons in double dots
freezing the nuclear-spin fluctuations could be consid-
ered, but no such effect has been demonstrated to date. We first ignore the spin of electrons and describe the
basic electronic properties of double quantum dots. The
C. Summary of mechanisms and time scales
properties of spinless electrons in double dots have been
treated in detail by Van der Wiel et al. 共2003兲. Here we
Our present understanding of the mechanisms and give all theory relevant for electron spins in double dots
time scales for energy relaxation and phase randomiza- without going into the details of the derivations.
tion of electron spins in few-electron quantum dots is
summarized as follows 共as before, most numbers are
1. Charge stability diagram
specific to GaAs dots, but the underlying physics is simi-
lar in other dot systems兲. Consider two quantum dots, labeled 1 and 2, whose
Energy relaxation is dominated by direct electron- electrochemical potentials are controlled independently
nuclear flip-flops near zero field 共or whenever the rel- by the gate voltages VG,1 and VG,2, respectively. Figure
evant electron-spin states are degenerate兲. In this case, 27共a兲 shows the equilibrium electron numbers 共N1 , N2兲
T1 is as low as 10– 100 ns. As B0 increases, electron- of the quantum dots as a function of VG,1 and VG,2, for
nuclear flip-flops become suppressed, and energy must the case that the dots are completely uncoupled. Such a
be dissipated in the phonon bath. Spin-phonon coupling plot is called a charge stability diagram. The lines indi-
is inefficient, and occurs mostly indirectly, mediated ei- cate the values of the gate voltages at which the number
ther by the hyperfine interaction or by spin-orbit inter- of electrons in the ground state changes. Note that the
action. As a result T1 rapidly increases with B0, and at lines are exactly horizontal and vertical, since the elec-
FIG. 29. Electrochemical potential lines around the triple points for weak tunnel coupling 共solid and dotted lines兲 and strong
tunnel coupling 共dashed lines兲. Each line outlines the gate voltages where the corresponding electrochemical potential in the dots
is equal to the electrochemical potential in the reservoirs 共which is defined as zero兲. The level diagrams indicate the positions of
the electrochemical potentials at several points in gate space. Inset: The naive expectation for the electrochemical potentials when
spin is included 共dotted line兲.
A = 1 − ␣2 . 共34兲 the inset of Fig. 29. However, experiments on double
dots with large tunnel coupling 共Hüttel et al., 2005;
When the single dot states are aligned, the energy of Pioro-Ladrière et al., 2005兲, reproduce the main diagram
bonding orbital is lower by 兩tc兩 than the energy of the of Fig. 29, and not the diagram of the inset that includes
single dot orbitals, and the energy of the antibonding spin. The reason for this is that the Coulomb interaction
orbital is higher by the same amount. is typically one or two orders of magnitude larger than
The tunnel coupling is revealed in the charging dia- the tunnel coupling. Therefore when the double dot is
gram by a bending of the honeycomb lines near the occupied by two electrons, electrons are again strongly
triple points, as depicted by the dashed lines in Fig. 29. localized. The orbital energy of the two-electron system
The value of the tunnel coupling can be determined ex- is then equal to the sum of the two single-dot orbitals,
perimentally from such a plot by measuring the bending which is the same as the sum of the bonding and the
of the lines 共Hüttel et al., 2005; Pioro-Ladrière et al., antibonding orbital. When the second electron is added,
2005兲, or by measuring the charge distribution as a func- the tunnel coupling energy that was gained by the first
tion of detuning between left and right dot potentials electron has to be “paid back,” which causes the second
共DiCarlo et al., 2004; Petta et al., 2004兲. triple point to appear at higher gate voltages than in the
Note that, when drawing the diagram in Fig. 29, we weak-coupling case. Therefore Fig. 29 is recovered when
assumed the electrons to be spinless. Therefore the first spin is included.
electron can enter the molecular bonding orbital which
takes 兩tc兩 less energy than in the case of weak tunnel
2. High bias regime: Bias triangles
coupling. The second has to move into the antibonding
orbital because of the Pauli exclusion principle. Thus the When the source-drain bias voltage is increased, two
extra energy needed to add the second electron is EC different types of tunneling can occur. Up to now, we
+ 2兩tc兩 共兩tc兩 more than for the weak-coupling case兲 and the have only discussed tunneling between aligned levels,
second triple point is pushed to higher gate voltages with where the initial and final electronic state by definition
respect to the weak-coupling case. have the same energy. This is termed elastic tunneling.
When spin is taken into account, the orbitals become However, tunneling can also occur when there is an en-
doubly degenerate and both electrons can occupy the ergy mismatch between the initial and final states 共levels
bonding orbital. Thus it only takes EC extra energy to are misaligned兲, in which case the process is called in-
add the second electron. This changes the charging dia- elastic. For inelastic tunneling to take place, energy ex-
gram drastically; namely, the dashed line in the 共1,1兲 re- change with the environment is required to compensate
gion 共in the upper right corner in Fig. 29兲 moves to the for the energy mismatch, since the process as a whole
other side of the triple point. This scenario is sketched in has to conserve energy. One important example of en-
冉 冊
from 共1,1兲 to 共0,2兲 is the limiting step in the current:
0 gB⌬BN,z
precisely what is expected for a double dot in spin block- H= . 共43兲
ade. gB⌬BN,z 0
Since S and T0 are not eigenstates of this Hamiltonian,
D. Hyperfine interaction in a double dot: the off-diagonal terms will drive rotations between S
Singlet-triplet mixing and T0. Similarly, the x component and the y component
of the nuclear field mix T+共1 , 1兲 and T−共1 , 1兲 with S共1 , 1兲.
Early experiments in semiconducting heterostructures Figure 36共a兲 shows measurements of the leakage cur-
in the quantum Hall regime demonstrated that spin- rent in the Pauli spin blockade regime in vertical double
polarized currents could be used to polarize the nuclei in dots as a function of magnetic field for two different
the substrate 共Wald et al., 1994; Dixon et al., 1997兲. These sweep directions 共Ono and Tarucha, 2004兲. Upon in-
measurements gave a clear indication that electronic ef- creasing the magnetic field, the leakage current was
FIG. 44. 共Color online兲 The control cycle for coherent manipu-
lation of the electron spin via electron-spin resonance.
which rotates the Bloch vector about the z axis of the time ttot = S + S⬘. Figure 49共c兲 shows PS as a function of
Bloch sphere. Exchange is turned off and the spins S − S⬘ for increasing ttot. A singlet state recovery is ob-
evolve for a time S⬘. During this time, the hyperfine served for ttot exceeding 1 s. A best fit to the singlet
fields rotate the Bloch vector back towards S共1 , 1兲, refo- state decay using an exponential form leads to T2
cusing the spin singlet state. = 1.2 s. Remarkably, this spin-echo pulse sequence ex-
Figure 49共b兲 shows PS as a function of and E in the
tends the coherence time by a factor of 100. Experi-
spin-echo pulse sequence. PS shows clear oscillations as
ments are currently underway to determine the physical
a function of E. For , 3, and 5 pulses clear singlet
state recoveries are observed. To determine the coher- origin of the 1.2-s decay. Possible sources of the decay
ence time we set S = S⬘ and vary the total separation are nuclear-spin evolution 共see Sec. VII.B兲, charge
dephasing 共Hu and Das Sarma, 2006兲, and decay to rameters can certainly increase this to ⬎99%. We note
T+共1 , 1兲. also that the QPC charge meter is a fairly simple device
that can be integrated easily in quantum dot circuits.
X. PERSPECTIVES We see that qubits defined by single-electron spins in
quantum dots largely satisfy the DiVincenzo criteria. As
This review has described the spin physics of few- an alternative, it is also possible to encode the logical
electron quantum dots. Much of this work can be evalu- qubit in a combination of spins. For instance, when the
ated within the context of spin-based classical or quan- logical qubit is encoded in three spins instead of a single
tum information processing. In this context, the state of spin, the exchange interaction by itself is sufficient for
the art can be best summarized by making a comparison universal quantum computation 共DiVincenzo et al.,
with the first five DiVincenzo criteria 共DiVincenzo, 2000兲. Adding a difference in Zeeman energy between
2000兲, applied to the Loss-DiVincenzo proposal for en- the two dots reduces the number of spins per logical
coding a logical qubit in a single electron spin 共Loss and qubit to two 共Levy, 2002兲. Coherent operations on this
DiVincenzo, 1998兲. so-called singlet-triplet qubit have already been experi-
共i兲 Have a scalable physical system with well-defined mentally demonstrated 共see Sec. IX.B兲. These two- and
qubits. Electron spins are certainly well-defined qubits. three-electron qubit encodings eliminate the need for
The Zeeman energy difference between the qubit states the technologically challenging single-spin rotations.
can be made much larger than the thermal energy. The Many more variations for encoding qubits in several
states can be measured using transport spectroscopy 共see electron spins have been proposed, each having its own
Sec. III兲. It is difficult to make predictions concerning advantages and drawbacks 共Byrd and Lidar, 2002; Wu
scalability. In principle, circuits of solid-state devices are and Lidar, 2002a, 2002b; Meier et al., 2003; Kyriakidis
scalable, but evidently many practical problems will and Penney, 2005; Taylor et al., 2005; Hanson and
have to be surmounted. Burkard, 2007兲. In the end, the best implementation for
共ii兲 Be able to initialize to a simple fiducial state such a given system will depend on many factors that are
as 兩0000¯典. By waiting until relaxation takes place at hard to oversee at this stage.
low temperature and in high magnetic field, the many- In the near future, the natural continuation of the re-
qubit ground state will be occupied with probability cent work will be to combine the various components
close to 1. Another option is to use the energy difference 共readout, ESR, and exchange gate兲 in a single experi-
between the states or the different coupling to the res- ment. This may allow for new experiments exploring
ervoir to induce spin-selective tunneling from the reser- quantum coherence in the solid state, for instance in-
voir onto the dot. volving entanglement and testing Bell’s inequalities. As
共iii兲 Have long coherence times. The T2-coherence another example, the precise role of quantum measure-
time has not been determined extensively, but already a ments may be investigated in this system as well.
lower bound of ⬃1 s has been established at 100 mT. On a longer time scale, the main challenges are scal-
How quantum coherence scales with the size of the sys- ability and coherence. Scalability is mostly a practical
tem is an interesting open question. The coherence issue. The coherence challenge provides a number of
times of qubits can be prolonged by error correction. interesting open questions. The coherence time is cur-
This can be done effectively only when many manipula- rently limited by the randomness in the nuclear-spin sys-
tions are allowed before decoherence takes place. The tem. If this randomness is suppressed, the coherence
rule of thumb is that the coherence time should be at time will become longer. Polarization of nuclei turns out
least 104 times longer than the time for a typical one-or not to be very efficient, except for polarizations
two-qubit operation. ⬎99.9%. As an alternative, the nuclear spins could be
共iv兲 Have a universal set of quantum gates. The Loss- put and kept in a particular, known quantum state
DiVincenzo proposal provides two gates which together 共Giedke et al., 2006; Klauser et al., 2006; Stepanenko et
allow for universal quantum computing. Single-qubit ro- al., 2006兲.
tations have been implemented by ESR, with a fidelity It is yet unknown if nuclear spins can indeed be con-
of ⬃75% and a duration of 25 ns for a / 2 rotation. The trolled up to a high level of accuracy. A completely dif-
two-qubit gate is based on the two-spin SWAP opera- ferent approach would be using a different material. The
tion, which has been demonstrated as well, combined isotopes of the III-V semiconductors all have a nonzero
with single-spin rotations. The SWAP has already been nuclear spin. In contrast, the group-IV semiconductors
operated at sub-ns levels 共180 ps for a 冑SWAP gate兲, do have isotopes with zero nuclear spin. If spin qubits
although the fidelity is yet unclear. These are only the are realized in a material that is isotopically purified to
first experimental results and further improvements are for instance 28Si or 12C only, the hyperfine interaction is
expected. completely absent.
共v兲 Permit high quantum efficiency, qubit-specific mea- We believe that the techniques and physics described
surements. The procedure of spin to charge conversion in this review will prove valuable regardless of the type
and measuring the charge is a highly efficient measure- of quantum dot that is used to confine electrons. The
ment of the qubit state. It allows for a single-shot read- unprecedented level of control over single-electron spins
out measurement with demonstrated fidelities already will enable exploration of new regimes and pave the way
exceeding 90%. An optimization of experimental pa- for tests of simple quantum protocols in the solid state.
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