Repeated injection of spin polarized carriers in a quantum dot leads to the polarization of nuclear spins, a process known as dynamic nuclear spin polarization (DNP). Here, we report the first observation of p-shell carrier assisted DNP in single QDs at zero external magnetic field. The nuclear field - measured by using the Overhauser shift of the singly charged exciton state of the QDs - continues to increase, even after the carrier population in the s-shell saturates. This is also accompanied by an abrupt increase in nuclear spin buildup time as p-shell emission overtakes that of the s-shell. We attribute the observation to p-shell electrons strongly altering the nuclear spin dynamics in the QD, supported by numerical simulation results based on a rate equation model of coupling between electron and nuclear spin system. DNP with p-shell carriers could open up avenues for further control to increase the degree of nuclear spin polarization in QDs.
new defect-assisted mechanism of multiphonon intraband carrier relaxation in semiconductor quantum dots, where the carrier is found in a coherent superposition of the initial, final, and defect states, is proposed. It is shown that this mechanism is capable of explaining the observed trends in temperature dependences of the intraband relaxation rates for PbSe and CdSe colloidal nanocrystal quantum dots.
Assisted hopping effects in magnetic impurities and quantum dots are analyzed. The magnitude of the assisted hopping term in a quantum dot in the limit of large level spacing is comparable to other corrections induced by the electron-electron interactions. Assisted hopping leads to differences between conductance peaks associated to the same level, and, when the effect is sufficiently strong, to local pairing correlations.
While time-dependent perturbation theory shows inefficient carrier-phonon scattering in semiconductor quantum dots, we demonstrate that a quantum kinetic description of carrier-phonon interaction predicts fast carrier capture and relaxation. The considered processes do not fulfill energy conservation in terms of free-carrier energies because polar coupling of localized quantum-dot states strongly modifies this picture.
We report on electron transport through an artificial molecule formed by two tunnel coupled quantum dots, which are laterally confined in a two-dimensional electron system of an Al$_x$Ga$_{1-x}$As/GaAs heterostructure. Coherent molecular states in the coupled dots are probed by photon-assisted tunneling (PAT). Above 10 GHz, we observe clear PAT as a result of the resonance between the microwave photons and the molecular states. Below 8 GHz, a pronounced superposition of phonon- and photon-assisted tunneling is observed. Coherent superposition of molecular states persists under excitation of ac…
Pauli exclusion principle can lead to a supression of transport through double quantum dots, even if both quantum dots are connected by a resonant driving ac field. In this work, we study how this effect, known as spin blockade, can be removed by means of the influence of the driving field on the contacts to the leads.
We analyze dephasing in single and double quantum dot systems. The decoherence is introduced by the Büttiker model with current conserving fictitious voltage leads connected to the dots. By using the non-equilibrium Green function method, we investigate the dephasing effect on the tunneling current. It is shown that a finite dephasing rate leads to observable effects. The result can be used to measure dephasing rates in quantum dots.
Carrier-dopant exchange interactions in Mn-doped PbS colloidal quantum dots were studied by circularly polarized magneto-photoluminescence. Mn substitutional doping leads to paramagnetic behavior down to 5 K. While undoped quantum dots show negative circular polarization, Mn doping changes its sign to positive. A circular polarization value of 40% was achieved at T=7 K and B=7 tesla. The results are interpreted in terms of Zeeman splitting of the band edge states in the presence of carrier-dopant exchange interactions that are qualitatively different from the s,p-d exchange interactions in II-…
We investigate experimentally and theoretically the resonant emission of single InAs/GaAs quantum dots in a planar microcavity. Due to the presence of at least one residual charge in the quantum dots, the resonant excitation of the neutral exciton is blocked. The influence of the residual doping on the initial quantum dots charge state is analyzed, and the resonant emission quenching is interpreted as a Coulomb blockade effect. The use of an additional non-resonant laser in a specific low power regime leads to the carrier draining in quantum dots and allows an efficient optical gating of the e…
We investigate the thermal quenching of the multimodal photoluminescence from InAs/InP (001) self-assembled quantum dots. The temperature evolution of the photoluminescence spectra of two samples is followed from 10 K to 300 K. We develop a coupled rate-equation model that includes the effect of carrier thermal escape from a quantum dot to the wetting layer and to the InP matrix, followed by transport, recapture or non-radiative recombination. Our model reproduces the temperature dependence of the emission of each family of quantum dots with a single set of parameters. We find that the main es…
We study transport through one or two ultrasmall quantum dots with discrete energy levels to which a time-dependent field is applied (e.g., microwaves). The AC field causes photon-assisted tunneling and also transitions between discrete energy levels of the dot. We treat the problem by introducing a generalization of the rotating-wave approximation to arbitrarily many levels. We calculate the dc-current through one dot and find satisfactory agreement with recent experiments by Oosterkamp et al. . In addition, we propose a novel electron pump consisting of two serially coupled single-level quan…
We review experiments on single electron transport through single quantum dots in the presence of a microwave signal. In the case of a small dot with well-resolved discrete energy states, the applied high-frequency signal allows for inelastic tunnel events that involve the exchange of photons with the microwave field. These photon assisted tunneling (PAT) processes give rise to sideband resonances in addition to the main resonance. Photon absorption can also lead to tunneling via excited states instead of tunneling via the ground state of the quantum dot.
We consider the photon-assisted tunneling (PAT) and the Landau-Zener-Stueckelberg (LZS) interference for double quantum dots induced electrostatically along a semiconducting carbon nanotube. An atomistic tight-binding approach and the time-dependent configuration interaction method are employed for description of the systems of a few confined electrons and holes. We reproduce the patterns of the LZS interference recently observed for the quantum double dots describing transport across hole-localized states. Moreover, we indicate that for charge configurations for which the ground-state is Paul…
We systematically investigate electron transport through double quantum dots with particular emphasis on interference induced via multiple paths of electron propagation. By means of the slave-boson mean-field approximation, we calculate the conductance, the local density of states, the transmission probability in the Kondo regime at zero temperature. It is clarified how the Kondo-assisted transport changes its properties when the system is continuously changed among the serial, parallel and T-shaped double dots. The obtained results for the conductance are explained in terms of the Kondo reson…
We present a theoretical study of the evolution of spatial coherence during relaxation between delocalized exciton states in a pair of vertically stacked semiconductor quantum dots coupled to acoustic phonons. We show that spatial coherence can be transferred to the ground state even in a system of uncoupled non-identical quantum dots if a particular kind of degeneracy between the inter-level energy splittings is present. The phonon-assisted mechanism of coherence transfer leads to a dependence of the amount of the resulting coherence on the inter-dot distance and temperature. We analyze also …
Carrier dynamics of submonolayer (SML) InGaAs/GaAs quantum dots (QDs) were studied by micro-photoluminecence (MPL), selectively excited photoluminescence (SEPL), and time-resolved photoluminescence (TRPL). MPL and SEPL show the coexistence of localized and delocalized states, and different local phonon modes. TRPL reveal shorter recombination lifetimes and longer capture times for the QDs with higher emission energy. This suggests that the smallest SML QDs are formed by perfectly vertically correlated 2D InAs islands, having the highest In content and the lowest emission energy, while a slight…
We image the micro-electroluminescence (EL) spectra of self-assembled InAs quantum dots (QDs) embedded in the intrinsic region of a GaAs p-i-n diode and demonstrate optical detection of resonant carrier injection into a single QD. Resonant tunneling of electrons and holes into the QDs at bias voltages below the flat-band condition leads to sharp EL lines characteristic of individual QDs, accompanied by a spatial fragmentation of the surface EL emission into small and discrete light- emitting areas, each with its own spectral fingerprint and Stark shift. We explain this behavior in terms of Cou…
We investigate the conductance and zero-frequency shot noise of interacting, multi-level quantum dots coupled to leads. We observe that co-tunneling assisted sequential tunneling (CAST) processes play a dominant role in the transition region from Coulomb blockade to sequential tunneling. We analyze for intermediate coupling strength the dependence of the conductance due to CAST processes on temperature, coupling constant, and gate voltage. Remarkably, the width of the CAST transport feature scales only with temperature, but not with the coupling constant. While the onset of inelastic co-tunnel…
With the aim of improving solar cell efficiency, a structure for realizing electron tunneling from In0.6Al0.4As quantum dots (QDs) through an Al0.4Ga0.6As barrier to AlAs has been grown using molecular beam epitaxy. The photoluminescence decay time decreased from 1.1 ns to 390 ps as the barrier thickness decreased from 4 to 2 nm, which indicates that the photo-excited carriers tunneled from the QDs to the AlAs X energy level for a barrier thickness 2 nm in 0.6 ns, which is significantly longer than the tunneling time of GaAs and InAlAs quantum wells. We expect that this structure will assist i…
We show that the carrier ''antibinding'' observed recently in semiconductor quantum dots, i.e., the fact that the ground state energy of two electron-hole pairs goes above twice the ground-state energy of one pair, can entirely be assigned to a charge separation effect, whatever its origin. In the absence of external electric field, this charge separation comes from different ''spreading-out'' of the electron and hole wavefunctions linked to the finite height of the barriers. When the dot size shrinks, the two-pair energy always stays below when the barriers are infinite. On the opposite, beca…
This Chapter contains a review of the recent results, both experimental and theoretical, related to optical control of carriers confined in semiconductor quantum dots. The physics of Rabi oscillations of exciton and biexciton occupations, as well as time-domain interference experiments are discussed. Next, the impact of carrier--phonon interaction in a semiconductor structure is described and modern methods of theoretical description of the carrier--phonon kinetics and of the resulting dephasing are presented.
We analyse various phonon-assisted mechanisms which contribute to the decoherence of excitonic qubits in quantum dot systems coupled by the Förster-type transfer process. We show the significant loss of coherence accompanied by dissipation due to charge carrier oscillations between qubit states by using a model of one-phonon assisted Förster-type transfer process. We obtain explicit expressions for the relaxation and dephasing times for excitonic qubits interacting with acoustic phonons via both deformation potential and piezoelectric coupling. We compare the decoherence times of the GaAs/AlGa…
We consider cotunneling through a quantum dot in the presence of spin-flip processes induced by the coupling to acoustic phonons of the surrounding. An expression for the phonon-assisted cotunneling current is derived by means of a generalized Schrieffer-Wolff transformation. The influence of the spin-phonon coupling on the heating of the dot is considered. The result is evaluated for the case of a parabolic semiconductor quantum dot with Rashba and Dresselhaus spin-orbit coupling and a method for the determination of the spin-phonon relaxation rate is proposed.
We investigate the influence of thermal energy on the current flow and electron spin states in double quantum dots in series. The quadruplet Pauli spin blockade, which is caused by the quadruplet and doublet states, occurs at low temperatures affecting the transport properties. As the temperature increases, the quadruplet Pauli spin blockade occurs as a result of the thermal energy, even in regions where it does not occur at low temperatures. This is because the triplet state is formed in one dot as a result of the gradual change of the Fermi distribution function of the electrodes with increa…
With downscaling of electronic circuits, components based on semiconductor quantum dots are assuming increasing relevance for future technologies. Their response under external stimuli intrinsically depend on their quantum properties. Here we investigate single-electron tunneling in hard-wall InAs/InP nanowires in the presence of an off-resonant microwave drive. Our heterostructured nanowires include InAs quantum dots (QDs) and exhibit different tunnel-current regimes. In particular, for source-drain bias up to few mV Coulomb diamonds spread with increasing contrast as a function of microwave …
Using integrated superconducting single photon detectors we probe ultra-slow exciton capture and relaxation dynamics in single self-assembled InGaAs quantum dots embedded in a GaAs ridge waveguide. Time-resolved luminescence measurements performed with on- and off-chip detection reveal a continuous decrease in the carrier relaxation time from 1.22 $\pm$ 0.07 ns to 0.10 $\pm$ 0.07 ns upon increasing the number of non-resonantly injected carriers. By comparing off-chip time-resolved spectroscopy with spectrally integrated on-chip measurements we identify the observed dynamics in the rise time ($…
We study the evolution of an exciton confined in a quantum dot adiabatically controlled by a frequency-swept (chirped) laser pulse in the presence of carrier-phonon coupling. We focus on the dynamics induced by a linearly polarized beam and analyze the decoherence due to phonon-assisted biexciton generation. We show that if the biexciton state is shifted down by a few meV, as is typically the case, the resulting decoherence is strong even at low temperatures. As a result, efficient state preparation is restricted to a small parameter area corresponding to low temperatures, positive chirps and …
We have investigated the dynamics of bound particles in multilevel current-carrying quantum dots. We look specifically in the regime of resonant tunnelling transport, where several channels are available for transport. Through a non-Markovian formalism under the Born approximation, we investigate the real-time evolution of the confined particles including transport-induced decoherence and relaxation. In the case of a coherent superposition between states with different particle number, we find that a Fock-space coherence may be preserved even in the presence of tunneling into and out of the do…
Spin relaxation in undoped quasi-spherical CdS quantum dots at zero magnetic fields is investigated using time- and polarization-resolved transient absorption measurements. Unlike in previous studies of these systems, the measured signals were corrected for spin-insensitive contributions to the exciton bleaching dynamics, {allowing us to determine} the pure spin-related exciton dynamics. To explain the observed room-temperature spin-relaxation time of several nanoseconds, we propose a novel mechanism based on intralevel exciton transitions with the emission of one LO phonon, the absorption of …
The effect of an ac electric field on quantum transport properties in a system of three quantum dots, two of which are connected in parallel while the third is coupled to one of the other two, is investigated theoretically. Based on the Keldysh nonequilibrium Green's function method, the spin-dependent current, occupation number and spin accumulation can be obtained in our model. An external magnetic flux, Rashba spin orbit coupling (SOC) and intradot Coulomb interactions are considered. The magnitude of the spin-dependent average current and the positions of the photon assisted tunneling (PAT…
We present a study on the intersublevel spacings of electrons and holes in a single layer of InAs self-assembled quantum dots (SAQDs) using Fourier transform infrared (FTIR) transmission spectroscopy without the application of an external magnetic field. Epitaxial, complementary-doped and semi-transparent electrostatic gates are grown within the ultra high vacuum conditions of molecular beam epitaxy to voltage-tune the device, while a two dimensional electron gas (2DEG) serves as back contact. Spacings of the hole sublevels are indirectly calculated using the photoluminescence spectroscopy alo…
The spin dynamics in a broad range of systems can be studied using circularly polarized optical excitation with alternating helicity. The dependence of spin polarization on the frequency of helicity alternation, known as the spin inertia effect, is used here to study the spin dynamics in singly-charged (In,Ga)As/GaAs quantum dots (QDs) providing insight into spin generation and accumulation processes. We demonstrate that the dependence of spin polarization in $n$- and $p$-type QDs on the external magnetic field has a characteristic V- and M-like shape, respectively. This difference is related …
We study the evolution of a quantum dot controlled by a frequency-swept (chirped), linearly polarized laser pulse in the presence of carrier-phonon coupling. The final occupation of the exciton state is limited both due to phonon-induced transitions between the adiabatic spectral branches and because of phonon-assisted transitions to the biexciton state. When the biexciton shift is large enough, the quantum dot can be modeled as a two-level system, which corresponds to excitation with circularly polarized light. For this case, we compare different methods of simulations: (i) a time convolution…
We derive a quantum-kinetic description of phonon-assisted F{ö}rster transfer between two coupled quantum dots (a quantum dot molecule). We show that the exciton state decays to the ground state of the QDM via a combination of the Rabi rotation and exponential decay. For moderately spaced dots this process takes place on a picosecond time scale.
We report on a high resolution x-ray diffraction study unveiling the effect of carriers optically injected into (In,Ga)As quantum dots on the surrounding GaAs crystal matrix. We find a tetragonal lattice expansion with enhanced elongation along the [001] crystal axis that is superimposed on an isotropic lattice extension. The isotropic contribution arises from excitation induced lattice heating as confirmed by temperature dependent reference studies. The tetragonal expansion on the femtometer scale is attributed to polaron formation by carriers trapped in the quantum dots.
A quantum-kinetic approach to the ultrafast dynamics of carrier multiplication in semiconductor quantum dots is presented. We investigate the underlying dynamics in the electronic subband occupations and the time-resolved optical emission spectrum, focusing on the interplay between the light-matter and the Coulomb interaction. We find a transition between qualitatively differing behaviors of carrier multiplication, which is controlled by the ratio of the interaction induced time scale and the pulse duration of the exciting light pulse. On short time scales, i.e., before intra-band relaxation, …
Tunneling-injection structures are incorporated in semiconductor lasers in order to overcome the fundamental dynamical limitation due to hot carrier injection by providing a carrier transport path from a cold carrier reservoir. The tunneling process itself depends on band alignment between quantum-dot levels and the injector quantum well, especially as in these devices LO-phonon scattering is dominant. Quantum dots with their first excited state near the quantum well bottom profit most from tunnel coupling. As inhomogeneous broadening is omnipresent in quantum dot structures, this implies that…
We study the dynamics of excitons in GaAs/(Al,Ga)As core-shell nanowires by continuous-wave and time-resolved photoluminescence and photoluminescence excitation spectroscopy. Strong Al segregation in the shell of the nanowires leads to the formation of Ga-rich inclusions acting as quantum dots. At 10 K, intense light emission associated with these shell quantum dots is observed. The average radiative lifetime of excitons confined in the shell quantum dots is 1.7 ns. We show that excitons may tunnel toward adjacent shell quantum dots and nonradiative point defects. We investigate the changes in…
In the present theoretical work we have considered impurities, either boron or phosphorous, located at different substitutional sites in silicon quantum dots (Si-QDs) with diameters around 1.5\,nm, embedded in a SiO2 matrix. Formation energy calculations reveal that the most energetically-favored doping sites are inside the QD and at the Si/SiO2 interface for P and B impurities, respectively. Furthermore, electron and hole transport calculations show in all the cases a strong reduction of the minimum voltage threshold, and a corresponding increase of the total current in the low-voltage regime…
We measured, for the first time, two photon radiative cascades due to sequential recombination of quantum dot confined electron hole pairs in the presence of an additional spectator charge carrier. We identified direct, all optical cascades involving spin blockaded intermediate states, and indirect cascades, in which non radiative relaxation precedes the second recombination. Our measurements provide also spin dephasing rates of confined carriers.
For a semiconductor quantum dot strongly coupled to a microcavity, we theoretically investigate phonon-assisted transitions from the exciton to a cavity photon, where the energy mismatch is compensated by phonon emission or absorption. By means of a Schrieffer-Wolff transformation we derive an effective Hamiltonian, which describes the combined effect of exciton-cavity and exciton-phonon coupling, and compute the scattering rates within a Fermi golden rule approach. The results of this approach are compared with those of a recently reported description scheme based on the independent Boson mod…
In magnetically-doped quantum dots changing the carrier occupancy, from open to closed shells, leads to qualitatively different forms of carrier-mediated magnetic ordering. While it is common to study such nanoscale magnets within a mean field approximation, excluding the spin fluctuations can mask important phenomena and lead to spurious thermodynamic phase transitions in small magnetic systems. By employing coarse-grained, variational, and Monte Carlo methods on singly and doubly occupied quantum dots to include spin fluctuations, we evaluate the relevance of the mean field description and d…
We present a quantum-mechanical model for surface-assisted carrier excitation by optical fields in plasmonic nanostructures of arbitrary shape. We derive an explicit expression, in terms of local fields inside the metal structure, for surface absorbed power and surface scattering rate that determine the enhancement of carrier excitation efficiency near the metal-dielectric interface. We show that surface scattering is highly sensitive to the local field polarization, and can be incorporated into metal dielectric function along with phonon and impurity scattering. We also show that the obtained…
We calculate the rates of phonon-assisted hyperfine spin flips during electron and hole tunneling between quantum dots in a self-assembled quantum dot molecule. We show that the hyperfine process dominates over the spin-orbit-induced spin relaxation in magnetic fields up to a few Tesla for electrons, while for holes this cross-over takes place at field magnitudes of a fraction of Tesla, upon the assumption of a large $d$-shell admixture to the valence band state, resulting in a strong transverse hyperfine coupling. The interplay of the two spin-flip mechanisms leads to a minimum of the spin-fl…
The coherent spin dynamics of resident carriers, electrons and holes, in semiconductor quantum structures is studied by periodical optical excitation using short laser pulses and in an external magnetic field. The generation and dephasing of spin polarization in an ensemble of carrier spins, for which the relaxation time of individual spins exceeds the repetition period of the laser pulses, are analyzed theoretically. Spin polarization accumulation is manifested either as resonant spin amplification or as mode-locking of carrier spin coherences. It is shown that both regimes have the same orig…
The time evolution of optically excited carriers in semiconductor quantum wells and quantum dots is analyzed for their interaction with LO-phonons. Both the full two-time Green's function formalism and the one-time approximation provided by the generalized Kadanoff-Baym ansatz are considered, in order to compare their description of relaxation processes. It is shown that the two-time quantum kinetics leads to thermalization in all the examined cases, which is not the case for the one-time approach in the intermediate-coupling regime, even though it provides convergence to a steady state. The t…
We report on the carrier dynamics in InGaN/GaN disk-in-a-wire quantum dots with precisely controlled location and structural parameters, including diameter, thickness and material composition. We measured the time-integrated and time-resolved spectra and the second-order correlation function of the photoluminescence from quantum dots with diameters ranging from 19 nm to 33 nm at temperatures of 10 K to 120 K. The influence of the small fluctuations in structural parameters, most importantly the quantum dot thickness, on the optical properties are also investigated through statistical correlati…
We study electrostatic quantum dot confinement for charge carriers in silicene. The confinement is formed by vertical electric field surrounding the quantum dot area. The resulting energy gap in the outside of the quantum dot traps the carriers within, and the difference of electrostatic potentials on the buckled silicene sublattices produces nonzero carrier masses outside the quantum dot. We study the electrostatic confinement defined inside a silicene flake with both the atomistic tight-binding approach as well as with the continuum approximation for a circularly symmetric electrostatic pote…
We present a theoretical analysis of the phonon-assisted relaxation in a system composed of two self-assembled vertically stacked quantum dots. We construct realistic model, which takes into account the geometry and strain distribution in the system. We calculate phonon-assisted relaxation rates between the two lowest states (in one- and two-electron cases). The relaxation rates and energy levels are studied as a function of external (axial) electric field and geometry of the structure (dot sizes). We show that the relaxation times can be as low as 1~ps but efficent relaxation occurs only for …
We present an experimental and theoretical study of the polarized photoluminescence spectrum of single semiconductor quantum dots in various charge states. We compare our high resolution polarization sensitive spectral measurements with a new many-carrier theoretical model, which was developed for this purpose. The model considers both the isotropic and anisotropic exchange interactions between all participating electron-hole pairs. With this addition, we calculate both the energies and polarizations of all optical transitions between collective, quantum dot confined charge carrier states. We …
We propose a nanoscale device consisting of a double quantum dot with strong intra- and inter- dot Coulomb repulsions. In this design, the current can only flow through the lower dot, but is triggered by the gate-controlled occupancy of the upper dot. At low temperatures, our calculations predict the double dot to pass through a narrow Kondo regime, resulting in highly sensitive switching characteristics between three well-defined states : insulating, normal conduction and resonant conduction.
Environmental noise usually hinders the efficiency of charge transport through coherent quantum systems; an exception is dephasing-assisted transport (DAT). We show that linear triple quantum dots in a transport configuration and subjected to pure dephasing exhibit DAT if the coupling to the drain reservoir exceeds a threshold. DAT occurs for arbitrarily weak dephasing and the enhancement can be directly controlled by the coupling to the drain. Moreover, for specific settings, the enhanced current is accompanied by a reduction in relative shot noise. We identify the quantum Zeno effect and lon…
We study the influence of the phonon environment on the electron dynamics in a doped quantum dot molecule. A non-perturbative quantum kinetic theory based on correlation expansion is used in order to describe both diagonal and off-diagonal electron-phonon couplings representing real and virtual processes with relevant acoustic phonons. We show that the relaxation is dominated by phonon-assisted electron tunneling between constituent quantum dots and occurs on a picosecond time scale. The dependence of the time evolution of the quantum dot occupation probabilities on the energy mismatch between…
