With the increasing energy crisis and the prevalent concept of green sustainability, quantum dot materials have become a hot spot in the academic and industrial fields of chemistry. Due to unique, tailor-made photovoltaic properties based on marked quantum-confined effects, it's necessary to identify the QD-based charge transfer process connected with a lifetime of stimulated excitons. Additionally, inorganic nanoparticles with a continuum of electron states contribute to the consistency between electron dynamics and their function through complexation with QDs. Ultrafast spectroscopy can be widely used in this system, the most typical of which is the time-resolved transient absorption spectroscopy, especially on a femtosecond or picosecond timescale. In this paper, we used the ZnSe/CdS core-shell quantum dot as the donor, and the TiO2 film as the metal oxide molecule as the acceptor, through steady-state and transient absorption techniques. Within, the electron transfer and related processes between the two composite systems were explored, and the relationship between the electron transfer rate constant (kBET) and particle size and QD core size was further studied. Through the research content of this paper, it is hoped to provide materials for quantum dot sensitization devices with more controllable features.
In this theoretical manuscript I propose a scheme for entangling a single electron semiconductor spin qubit with a single electron semiconductor charge qubit in a triangular triple quantum dot configuration. Two out of three quantum dots are used to define a single electron semiconductor charge qubit. Furthermore, the spin qubit is embedded in the Zeeman sub-levels of the third quantum dot. Combining single qubit gates with entangling CNOT gates allows one to construct a SWAP gate, and therefore to use the semiconductor spin qubit as a long-lived memory for the semiconductor charge qubit.
We propose a solid-state implementation of stimulated Raman adiabatic passage in two coupled semiconductor quantum dots. Proper combination of two pulsed laser fields allows the coherent carrier transfer between the two nanostructures without suffering significant losses due to environment coupling. By use of a general solution scheme for the carrier states in the double-dot structure, we identify the pertinent dot and laser parameters.
Coulomb correlations in the optical spectra of semiconductor quantum dots are investigated using a full-diagonalization approach. The resulting multi-exciton spectra are discussed in terms of the symmetry of the involved states. Characteristic features of the spectra like the nearly equidistantly spaced s-shell emission lines and the approximately constant p-shell transition energies are explained using simplified Hamiltonians that are derived taking into account the relative importance of various interaction contributions. Comparisons with previous results in the literature and their interpre…
Existence of representative longitudinal optical (LO) phonon modes is theoretically discussed for the case of polar semiconductor cylindrical quantum dots embedded in a semiconductor matrix. The approach is developed within the dielectric continuum model considering the Fröhlich interaction between electrons and the confined LO phonons. The theory is applied to cylindrical GaAs/AlAs quantum dots within an adiabatic treatment.
The propagation of a coherent optical linear wave in an ensemble of semiconductor quantum dots is considered. It is shown that a distribution of transition dipole moments of the quantum dots changes significantly the polarization and Beer's absorption length of the ensemble of quantum dots. Explicit analytical expressions for these quantities are presented.
We show that the addition spectra of semiconductor quantum dots in the presence of magnetic field can be studied through a theoretical scheme that allows an accurate and practical treatment of the single particle states and electron-electron interaction up to large numbers of electrons. The calculated addition spectra exhibit the typical structures of Hund-like shell filling, and account for recent experimental findings. A full three dimensional description of Coulomb interaction is found to be essential for predicting the conductance characteristics of few-electron semiconductor structures.
Most optical quantum devices require deterministic single-photon emitters. Schemes so far demonstrated in the solid state imply an energy relaxation which tends to spoil the coherent nature of the time evolution, and with it the photon indistinguishability. We focus our theoretical investigation on semiconductor quantum dots embedded in microcavities. Simple and general relations are identified between the photon indistinguishability and the collection efficiency. The identification of the key parameters and of their interplay provides clear indications for the device optimization.
A set of theoretical results on infrared absorption and inelastic (Raman) scattering of light in semiconductor quantum dots is reviewed. When it is possible, qualitative comparisons with recent experimental results are presented.
Preparation of a specific quantum state is a required step for a variety of proposed practical uses of quantum dynamics. We report an experimental demonstration of optical quantum state preparation in a semiconductor quantum dot with electrical readout, which contrasts with earlier work based on Rabi flopping in that the method is robust with respect to variation in the optical coupling. We use adiabatic rapid passage, which is capable of inverting single dots to a specified upper level. We demonstrate that when the pulse power exceeds a threshold for inversion, the final state is independent …
The spin-orbit coupling influences the total spin of semiconductor quantum dots. We analyze the theoretical prediction for the combined effects of spin-orbit coupling, weak vertical magnetic fields and deformation of the dot. Our results allow the characterization of the quantum dots as spin switches, controllable with electric gates.
As an analogy to the Weyl point in k-space, we search for energy levels which close at a single point as a function of a three dimensional parameter space. Such points are topologically protected in the sense that any perturbation which acts on the two level subsystem can be corrected by tuning the control parameters. We find that parameter controlled Weyl points are ubiquitous in semiconductor-superconductor quantum dots and that they are deeply related to Majorana zero modes. In this paper, we present several semiconductor-superconductor quantum dot devices which host parameter controlled We…
We present a theoretical analysis of four-wave mixing in coupled quantum dots subject to inhomogeneous broadening. For the biexciton transitions a clear signature of interdot-coupling appears in the spectra. The possibility of experimental observation is discussed.
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.
The ground state Lamb shift of a semiconductor spherical Quantum Dot is computed in the effective mass approximation. It appears to be significant enough to be detectable for a wide range of small Quantum Dots synthesized in semiconductors. A possible way to bserve it, via the Casimir effect, is suggested.
The issue of quantum size effects of interactive electron-hole systems in spherical semiconductor quantum dots is put to question. A sharper theoretical approach is suggested based on a new pseudo-potential method. In this new setting, analytical computations can be performed in most intermediate steps lending stronger support to the adopted physical assumptions. The resulting numerical values for physical quantities are found to be much closer to the experimental values than those existing so far in the literature.
We study the quantum-confined Stark effect in single InAs/GaAs quantum dots embedded within a AlGaAs/GaAs/AlGaAs quantum well. By significantly increasing the barrier height we can observe emission from a dot at electric fields of -500 kV/cm, leading to Stark shifts of up to 25 meV. Our results suggest this technique may enable future applications that require self-assembled dots with transitions at the same energy.
The mechanism of Stokes shift in semiconductor quantum dots is investigated by calculating the energy of the excitonic states. We have taken into account all possible contributions to the total electronic energy in the dot, i.e, dielectric mismatch between dot and surrounding medium, the effects of finite barrier height and electron-hole exchange interaction. The Stokes shift is calculated as a function of radius of dot and compared with experimental data on two different semiconductor based quantum dots. These results provide evidence for exchange splitting of excitonic states, as the mechani…
Time resolved intensity cross-correlation measurements of radiative cascades are used for studying non-radiative relaxation processes of excited carriers confined in semiconductor quantum dots. We spectrally identify indirect radiative cascades which include intermediate phonon assisted relaxations. The energy of the first photon reveals the multicarrier configuration prior to the non-radiative relaxation, while the energy of the second photon reveals the configuration after the relaxation. The intensity cross correlation measurements thus provide quantitative measures of the non-radiative pro…
We investigate the characteristic spin dynamics corresponding to semiconductor quantum dots within the multiband envelope function approximation (EFA). By numerically solving an $8\times8$ $k\cdot p$ Hamiltonian we treat systems based on different III-V semiconductor materials.It is shown that, even in the absence of an applied magnetic field, these systems show intrinsic spin dynamics governed by intraband and interband transitions leading to characteristic spin frequencies ranging from the THz to optical frequencies.
The effects of interplay between spin-orbit coupling and Zeeman splitting on weak localisation and universal conductance fluctuations in lateral semiconductor quantum dots are analysed: All possible symmetry classes of corresponding random matrix theories are listed and crossovers between them achievable by sweeping magnetic field and changing the dot parameters are described. We also suggest experiments to measure the spin-orbit coupling constants.
We propose an all-optical implementation of quantum-information processing in semiconductor quantum dots, where electron-hole excitations (excitons) serve as the computational degrees of freedom (qubits). The strong dot confinement leads to a strong renormalization of excitonic states, which, in analogy to NMR-based implementations of quantum-information processing, can be exploited for performing conditional and unconditional qubit operations.
We report the computer-automated tuning of gate-defined semiconductor double quantum dots in GaAs heterostructures. We benchmark the algorithm by creating three double quantum dots inside a linear array of four quantum dots. The algorithm sets the correct gate voltages for all the gates to tune the double quantum dots into the single-electron regime. The algorithm only requires (1) prior knowledge of the gate design and (2) the pinch-off value of the single gate $T$ that is shared by all the quantum dots. This work significantly alleviates the user effort required to tune multiple quantum dot …
The electronic spin precession in semiconductor dots is strongly affected by the spin-orbit coupling. We present a theory of the electronic spin resonance at low magnetic fields that predicts a strong dependence on the dot occupation, the magnetic field and the spin-orbit coupling strength. Coulomb interaction effects are also taken into account in a numerical approach.
The theory of elastic light scattering by semiconductor quantum dots is suggested. The semiclassical method, applying retarded potentials to avoid the problem of bounder conditions for electric and magnetic field, is used. The exact results for the Pointing vector on large distances from a quantum dot, formulas of differential cross sections of light scattering for the monochromatic and pulse irradiation are obtained.
We study the relaxation of the exciton spin (longitudinal relaxation time $T_{1}$) in single asymmetrical quantum dots due to an interplay of the short--range exchange interaction and acoustic phonon deformation. The calculated relaxation rates are found to depend strongly on the dot size, magnetic field and temperature. For typical quantum dots and temperatures below 100 K, the zero--magnetic field relaxation times are long compared to the exciton lifetime, yet they are strongly reduced in high magnetic fields. We discuss explicitly quantum dots based on (In,Ga)As and (Cd,Zn)Se semiconductor …
Elastic strain changes the energies of the conduction band in a semiconductor, which will affect transport through a semiconductor nanostructure. We show that the typical strains in a semiconductor nanostructure from metal gates are large enough to create strain-induced quantum dots (QDs). We simulate a commonly used QD device architecture, metal gates on bulk silicon, and show the formation of strain-induced QDs. The strain-induced QD can be eliminated by replacing the metal gates with poly-silicon gates. Thus strain can be as important as electrostatics to QD device operation operation.
An intense laser pulse propagating in a medium of inhomogeneously broadened quantum dots massively creates entangled exciton states. After passage of the pulse all single-exciton states remain unpopulated (self-induced transparency) whereas biexciton coherence (exciton entanglement) is generated through two-photon transitions. We propose several experimental techniques for the observation of such unexpected behavior.
We calculate the near-field optical spectra of excitons and biexcitons in semiconductor quantum dots naturally occurring at interface fluctuations in GaAs-based quantum wells, using a non-local description of the response function to a spatially modulated electro-magnetic field. The relative intensity of the lowest, far-field forbidden excitonic states is predicted; the spatial extension of the ground biexciton state is found in agreement with recently published experiments.
We study the energy spectra of small three-dimensional (3D) and two-dimensional (2D) semiconductor quantum dots through different theoretical approaches (single-site Hubbard and Hartree-Fock hamiltonians); in the smallest dots we also compare with exact results. We find that purely 2D models often lead to an inadequate description of the Coulomb interaction existing in realistic structures, as a consequence of the overestimated carrier localization. We show that the dimensionality of the dots has a crucial impact on (i) the accuracy of the predicted addition spectra; (ii) the range of validity…
The cross section of light absorption by semiconductor quantum dots in the case of the resonance with excitons $Γ_6 \times Γ_7$ in cubical crystals $T_d$ is calculated. It is shown that an interference of stimulating and induced electric and magnetic fields must be taken into account. The absorption section is proportional to the exciton nonradiative damping $γ$.
The lattice mismatch strain field of core/multishell structures with spherical symmetry is modeled by a linear continuum elasticity approach. The effect of the strain on the energy structure and linear optical absorption in large core/shell/shell spherical semiconductor quantum dots is analyzed. Localization of the photoexcited carriers induced by coating is found to play an important role in explaining the optical stability of large CdSe/CdS/ZnS and ZnTe/ZnSe/ZnS quantum dots.
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.
The possibility of a novel type of semiconductor quantum dots obtained by spatially modulating the spin-orbit coupling intensity in III-V heterostructures is discussed. Using the effective mass model we predict confined one-electron states having peculiar spin properties. Furthermore, from mean field calculations (local-spin-density and Hartree-Fock) we find that even two electrons could form a bound state in these dots.
The optical absorption of a single spherical semiconductor quantum dot in an electrical field is studied taking into account the nonlocal coupling between the field of the light and the polarizability of the semiconductor. These nonlocal effects lead to a small size anf field dependent shift and broadening of the excitonic resonance which may be of interest in future high precision experiments.
A one-band model within the effective mass approximation is adopted to characterize the energy structure and oscillator strength of type-II semiconductor spherical core-shell quantum dots. The heteroepitaxial strain of the core-shell heterostructure is modeled by the elastic continuum approach. The model is applied to ZnTe/ZnSe core-shell, a wide band gap type-II heterostructure. The simulated absorption spectra are in fair agreement with available experimental results.
Semiconductor quantum dots provide a two-dimensional analogy for real atoms and show promise for the implementation of scalable quantum computers. Here, we investigate the charge configurations in a silicon metal-oxide-semiconductor double quantum dot tunnel coupled to a single reservoir of electrons. By operating the system in the few-electron regime, the stability diagram shows hysteretic tunnelling events that depend on the history of the dots charge occupancy. We present a model which accounts for the observed hysteretic behaviour by extending the established description for transport in d…
We consider the several phenomena which are taking place in Quantum Dots (QD) and Quantum Rings (QR): The connection of the Quantum Chaos (QC) with the reflection symmetry of the QD, Disappearance of the QC in the tunnel coupled chaotic QD, electron localization and transition between Double Concentric QR in the transverse magnetic field, transition of electron from QR to the QD located in the center of QR. Basis of this consideration is the effective Schrödinger equation for the corresponding systems.
We study the triplet-singlet relaxation in two-electron semiconductor quantum dots. Both single dots and vertically coupled double dots are discussed. In our work, the electron-electron Coulomb interaction, which plays an important role in the electronic structure, is included. The spin mixing is caused by spin-orbit coupling which is the key to the triplet-singlet relaxation. We show that the selection rule widely used in the literature is incorrect unless near the crossing/anticrossing point in single quantum dots. The triplet/singlet relaxation in double quantum dots can be markedly changed…
We study phonon-assisted dephasing in optically excited semiconductor quantum dots within the frameworks of the independent Boson model and optimal control. Using a realistic description for the quantum dot states and the phonon coupling, we demonstrate that such dephasing has a drastic impact on the coherent optical response. We employ optimal control theory to search for control strategies that allow to fight decoherence, and show that appropriate tailoring of laser pulses allows a complete control of the optical excitation despite the phonon dephasing.
We report the enhancement of the optical second harmonic signal in non-centrosymmetric semiconductor CdS quantum dots, when they are placed in close contact with isolated silver nanoparticles. The intensity enhancement is about 1000. We also show that the enhancement increases when the incoming laser frequency $ω$ is tuned toward the spectral position of the silver plasmon at $2ω$, proving that the silver nanoparticle modifies the nonlinear emission.
We study electron-phonon interaction induced decoherence between two-electron singlet and triplet states in a semiconductor double quantum dot using a spin-boson model. We investigate the onset and time evolution of this dephasing, and study its dependence on quantum dot parameters such as dot size and double dot separations, as well as the host materials (GaAs and Si). At the short time limit, electron-phonon interaction only causes an incomplete initial Gaussian decay of the off-diagonal density matrix element in the singlet-triplet Hilbert space. A complete long-time exponential decay due t…
We review spin properties of semiconductor quantum dots and their effect on optical spectra. Photoluminescence and other types of spectroscopy are used to probe neutral and charged excitons in individual quantum dots with high spectral and spatial resolution. Spectral fine structure and polarization reveal how quantum dot spins interact with each other and with their environment. By taking advantage of the selectivity of optical selection rules and spin relaxation, optical spin pumping of the ground state electron and nuclear spins is achieved. Through such mechanisms, light can be used to pro…
Optical techniques for the quantum control of the dynamics of multiexciton states in a semiconductor quantum dot are explored in theory. Composite bichromatic phase-locked pulses are shown to reduce the time of elementary quantum operations on excitons and biexcitons by an order of magnitude or more. Analytic and numerical methods of designing the pulse sequences are investigated. Fidelity of the operation is used to gauge its quality. A modified Quantum Fourier Transform algorithm is constructed with only Rabi rotations and is shown to reduce the number of operations. Application of the desig…
This paper describes the modeling of quantum dots lasers with the aim of assessing the conditions for stable cw dual-mode operation when the mode separation lies in the THz range. Several possible models suited for InAs quantum dots in InP barriers are analytically evaluated, in particular quantum dots electrically coupled through a direct exchange of excitation by the wetting layer or quantum dots optically coupled through the homogeneous broadening of their optical gain. A stable dual-mode regime is shown possible in all cases when quantum dots are used as active layer whereas a gain medium …
Adiabatic time evolution of degenerate eigenstates of a quantum system provides a means for controlling electronic states since mixing between degenerate levels generates a matrix Berry phase. In the presence of spin-orbit coupling in n-type semiconductor quantum dots the electron Hamiltonian is invariant under time reversal operation and the many body groundstate may be doubly degenerate. This double degeneracy can generate non-Abelian vector potentials when odd number of electrons are present. We find that the antisymmetry of many electron wavefunction has no effect on the matrix Berry phase…
Quantum scars are enhancements of quantum probability density along classical periodic orbits. We study the recently discovered phenomenon of strong, perturbation-induced quantum scarring in the two-dimensional harmonic oscillator exposed to a homogeneous magnetic field. We demonstrate that both the geometry and the orientation of the scars are fully controllable with a magnetic field and a focused perturbative potential, respectively. These properties may open a path into an experimental scheme to manipulate electric currents in nanostructures fabricated in a two-dimensional electron gas.
We have observed the Kondo effect in strongly coupled semiconducting nanowire quantum dots. The devices are made from indium arsenide nanowires, grown by molecular beam epitaxy, and contacted by titanium leads. The device transparency can be tuned by changing the potential on a gate electrode, and for increasing transparencies the effects dominating the transport changes from Coulomb Blockade to Universal Conductance Fluctuations with Kondo physics appearing in the intermediate region.
Quantum dots may display fascinating features of strong correlation such as finite-size Wigner crystallization. We here review a few electron spectroscopies and predict that both inelastic light scattering and tunneling imaging experiments are able to capture clear signatures of crystallization.
We propose a scheme to manipulate the spin relaxation in vertically coupled semiconductor double quantum dots. Up to {\em twelve} orders of magnitude variation of the spin relaxation time can be achieved by a small gate voltage applied vertically on the double dot. Different effects such as the dot size, barrier height, inter-dot distance, and magnetic field on the spin relaxation are investigated in detail. The condition to achieve a large variation is discussed.
We review and extend the composite fermion theory for semiconductor quantum dots in high magnetic fields. The mean-field model of composite fermions is unsatisfactory for the qualitative physics at high angular momenta. Extensive numerical calculations demonstrate that the microscopic CF theory, which incorporates interactions between composite fermions, provides an excellent qualitative and quantitative account of the quantum dot ground state down to the largest angular momenta studied, and allows systematic improvements by inclusion of mixing between composite fermion Landau levels (called $…
More than 80 years passed since the first publication on entangled quantum states. In this period of time the concept of spookily interacting quantum states became an emerging field of science. After various experiments proving the existence of such non-classical states, visionary ideas were put forward to exploit entanglement in quantum information science and technology. These novel concepts have not yet come out of the experimental stage, mostly because of the lack of suitable, deterministic sources of entangled quantum states. Among many systems under investigation, semiconductor quantum d…
We present an Anderson-type model Hamiltonian with exchange coupling between the localized spins and the confined holes in the quantum dots to study the ferromagnetism in diluted magnetic semiconductor (DMS) quantum dot arrays embedded in semiconductors. The hybridization between the quantum-confined holes in the DMS quantum dots and the itinerant holes in the semiconductor valence band makes hole transfer between quantum dots, which can induce the long range ferromagnetic order of the localized spins. In addition, it makes the carrier spins both in the DMS quantum dots and in the semiconducto…
We develop a Maxwell-Schroedinger formalism in order to describe the radiative interaction mechanism between semiconductor quantum dots. We solve the Maxwell equations for the electromagnetic field coupled to the polarization field of a quantum dot ensemble through a linear non-local susceptibility and compute the polariton resonances of the system. The radiative coupling, mediated by both radiative and surface photon modes, causes the emergence of collective modes whose lifetimes are longer or shorter compared to the ones of non-interacting dots. The magnitude of the coupling and the collecti…
We investigate theoretically how the spin-orbit Dresselhaus and Rashba effects influence the electronic structure of quasi-one-dimensional semiconductor quantum dots, similar to those that can be formed inside semiconductor nanorods. We calculate electronic energy levels, eigen-functions, and effective g-factors for coupled, double dots made out of different materials, especially GaAs and InSb. We show that by choosing the form of the lateral confinement, the contributions of the Dresselhaus and Rashba terms can be tuned and suppressed, and we consider several possible cases of interest. We al…
We use temporally resolved intensity cross-correlation measurements to identify the biexciton-exciton radiative cascades in a negatively charged QD. The polarization sensitive correlation measurements show unambiguously that the excited two electron triplet states relax non-radiatively to their singlet ground state via a spin non conserving flip-flop with the ground state heavy hole. We explain this mechanism in terms of resonant coupling between the confined electron states and an LO phonon. This resonant interaction together with the electron-hole exchange interaction provides an efficient m…
Elastic light scattering by low-dimensional semiconductor objects is investigated theoretically. The differential cross section of resonant light scattering on excitons in quantum dots is calculated. The polarization and angular distribution of scattered light do not depend on the quantum-dot form, sizes and potential configuration if light wave lengths exceed considerably the quantum-dot size. In this case the magnitude of the total light scattering cross section does not depend on quantum-dot sizes. The resonant total light scattering cross section is about a square of light wave length if t…
We present a consistent theoretical description of few-particle effects in the optical spectra of semiconductor quantum dots, based on a direct-diagonalization approach. We show that, because of the strong Coulomb interaction among electrons and holes, each configuration of the confined few-particle system leads to its characteristic signature in the optical spectra. We discuss quantitative predictions and comparison with experiments for both absorption and luminescence.
The decay time of the linear polarization degree of the luminescence in strongly confined semiconductor quantum dots with asymmetrical shape is calculated in the frame of second-order quasielastic interaction between quantum dot charge carriers and LO phonons. The phonon bottleneck does not prevent significantly the relaxation processes and the calculated decay times can be of the order of a few tens picoseconds at temperature $T \simeq 100$K, consistent with recent experiments by Paillard et al. [Phys. Rev. Lett. {\bf86}, 1634 (2001)].
