We investigate theoretically the spin splitting of the exciton states in semiconductor coupled quantum dots (CQDs) containing a single magnetic ion. We find that the spin splitting can be switched on/off in the CQDs \textit{via} the \textit{sp-d}exchange interaction using the electric field. An interesting bright-to-dark exciton transition can be found and significantly affects the photoluminescence spectrum. This phenonmenon is induced by the transition of the ground exciton state, arising from the hole mixing effect, between the bonding and antibonding states.
The optical orientation of the exciton spin in an ensemble of self-organized cubic GaN/AlN quantum dots is studied by time-resolved photoluminescence. Under a polarized quasi-resonant excitation, the luminescence linear polarization exhibits no temporal decay, even at room temperature. This demonstrates the robustness of the exciton spin polarization in these cubic nitride nanostructures, with characteristic decay times longer than 10 ns.
The exciton-exciton interaction energy of Tellurium doped CdSe colloidal quantum dots is experimentally investigated. The dots exhibit a strong Coulomb repulsion between the two excitons, which results in a huge measured biexciton blue shift of up to 300 meV. Such a strong Coulomb repulsion implies a very narrow hole wave function localized around the defect, which is manifested by a large Stokes shift. Moreover, we show that the biexciton blue shift increases linearly with the Stokes shift. This result is highly relevant for the use of colloidal QDs as optical gain media, where a large biexci…
We demonstrate a new method of measuring the exciton spin relaxation time in semiconductor nanostructures by continuous-wave photoluminescence. We find that for self-assembled CdTe quantum dots the degree of circular polarization of emission is larger when exciting polarized excitons into the lower energy spin state than in the case when the excitons are excited into the higher energy spin state. A simple rate equation model gives the exciton spin relaxation time in CdTe quantum dots equal to 4.8+/-0.3 ns, significantly longer than the quantum dot exciton recombination time 300 ps.
We present a fully three-dimensional study of the multiexciton optical response of vertically coupled GaN-based quantum dots via a direct-diagonalization approach. The proposed analysis is crucial in understanding the fundamental properties of few-particle/exciton interactions and, more important, may play an essential role in the design/optimization of semiconductor-based quantum information processing schemes. In particular, we focus on the interdot exciton-exciton coupling, key ingredient in recently proposed all-optical quantum processors. Our analysis demonstrates that there is a large wi…
We report on the exciton spin dynamics of nanowire embedded GaN/AlN Quantum Dots (QDs) investigated by time-resolved photoluminescence spectroscopy. Under a linearly polarized quasiresonant excitation we evidence the quenching of the exciton spin relaxation and a temperature insensitive degree of the exciton linear polarization, demonstrating the robustness of the optical alignment of the exciton spin in these nanowire embedded QDs. A detailed examination of the luminescence polarization angular dependence shows orthogonal linear exciton eigenstates with no preferential crystallographic orient…
Exciton spin dynamics in quasi-spherical CdS quantum dots is studied in detail experimentally and theoretically. Exciton states are calculated using the 6-band k.p Hamiltonian. It is shown that for various sets of Luttinger parameters, when the wurtzite lattice crystal field splitting and Coulomb interaction between the electron-hole pair are taken into account exactly, both the electron and hole wavefunction in the lowest exciton state are of S-type. This rules out the spatial-symmetry-induced origin of the dark exciton in CdS quantum dots. The exciton bleaching dynamics is studied using time…
We investigate exciton spin memory in individual InAs/GaAs self-assembled quantum dots via optical alignment and conversion of exciton polarization in a magnetic field. Quasiresonant phonon-assisted excitation is successfully employed to define the initial spin polarization of neutral excitons. The conservation of the linear polarization generated along the bright exciton eigenaxes of up to 90% and the conversion from circular- to linear polarization of up to 47% both demonstrate a very long spin relaxation time with respect to the radiative lifetime. Results are quantitatively compared with a…
The near-field scanning optical microscopy images of excitonic wavefunctions in self-assembled InAs/GaAs quantum dots are calculated using an empirical pseudopotential method, followed by the configuration interaction (CI) treatment of many-particle effects. We show the wavefunctions of neutral exciton $X^0$ of different polarizations, and compare them to those of the biexciton $XX$ and the charged excitons $X^+$ and $X^-$. We further show that the exciton $X(P_h \to S_e)$ transition which is forbidden in the far-field photoluminescence has comparable intensities to that of $X(S_h \to S_e)$ tr…
We observe a strong dependence of the exciton spin relaxation in CdTe quantum dots on the average dot size and the depth of the confining potential. For the excitons confined to the as-grown CdTe quantum dots we find the spin relaxation time to be 4.8 ns. After rapid thermal annealing, which increases the average dot size and leads to weaker confinement, we measure the spin relaxation tine to be 1.5 ns, resulting in smaller values of the absolute polarization of the quantum dot emission. This dramatic enhancement of the spin scattering efficiency upon annealing is attributed to increased mixin…
Using time correlated single photon counting combined with temperature dependent diffraction limited confocal photoluminescence spectroscopy we accurately determine, for the first time, the intrinsic radiative lifetime of single excitons confined within semiconductor quantum dots. Their lifetime is one (two) orders of magnitude longer than the intrinsic radiative lifetime of single excitons confined in semiconductor quantum wires (wells) of comparable confining dimensions. We quantitatively explain this long radiative time in terms of the reduced spatial coherence between the confined exciton …
We investigate the interband transitions in several ensembles of self-assembled InAs/GaAs quantum dots by using photoluminescence excitation spectroscopy under strong magnetic field. Well defined resonances are observed in the spectra. A strong anticrossing between two transitions is observed in all samples, which cannot be accounted for by a purely excitonic model. The coupling between the mixed exciton-LO phonon states is calculated using the Fröhlich Hamiltonian. The excitonic polaron energies as well as the oscillator strengths of the interband transitions are determined. An anticrossing i…
We describe novel excitons in quantum dots by allowing for an interaction with a Fermi sea of electrons. We argue that these excitons can be realized very simply with self-assembled quantum dots, using the wetting layer as host for the Fermi sea. We show that a tunnel hybridization of a charged exciton with the Fermi sea leads to two striking effects in the optical spectra. First, the photoluminescence lines become strongly dependent on the vertical bias. Secondly, if the exciton spin is nonzero, the Kondo effect leads to peculiar photoluminescence line shapes with a line width determined by t…
We calculate the acoustic phonon-assisted exciton spin relaxation in single self-assembled In$_{1-x}$Ga$_x$As/GaAs quantum dots using an atomic empirical pseudopotential method. We show that the transition from bright to dark exciton states is induced by Coulomb correlation effects. The exciton spin relaxation time obtained from sophisticated configuration interaction calculations is approximately 15--55 $μ$s in pure InAs/GaAs QDs and even longer in alloy dots. These results contradict previous theoretical and experimental results, which suggest very short exciton spin times (a few ns), but ag…
Cathodoluminescence spectra employing a shadow mask technique of InGaN layers grown by metal organic chemical vapor deposition on Si(111) substrates are reported. Sharp lines originating from InGaN quantum dots are observed. Temperature dependent measurements reveal thermally induced carrier redistribution between the quantum dots. Spectral diffusion is observed and was used as a tool to correlate up to three lines that originate from the same quantum dot. Variation of excitation density leads to identification of exciton and biexciton. Binding and anti-binding complexes are discovered.
We report on a new approach to detect excitonic qubits in semiconductor quantum dots by observing spontaneous emissions from the relevant qubit level. The ground state of excitons is resonantly excited by picosecond optical pulses. Emissions from the same state are temporally resolved with picosecond time resolution. To capture weak emissions, we greatly suppress the elastic scattering of excitation beams, by applying obliquely incident geometry to the micro photoluminescence set-up. Rabi oscillations of the ground-state excitons appear to be involved in the dependence of emission intensity on…
We report on polarization-resolved resonant photoluminescence (PL) spectroscopy of bright (spin-1) and dark (spin-2) excitons in colloidal CdSe nanocrystal quantum dots. Using high magnetic fields to 33 T, we resonantly excite (and selectively analyze PL from) spin-up or spin-down excitons. At low temperatures (<4K) and above ~10 T, the spectra develop a narrow, circularly polarized peak due to spin-flipped bright excitons. Its evolution with magnetic field directly reveals a large (1-2 meV), intrinsic fine structure splitting of bright excitons, due to anisotropic exchange. These findings are…
Systematic time-resolved measurements on neutral and charged excitonic complexes (X, XX, X+, and XX+) of 26 different single InAs/GaAs quantum dots are reported. The ratios of the decay times are discussed in terms of the number of transition channels determined by the excitonic fine structure and a specific transition time for each channel. The measured ratio for the neutral complexes is 1.7 deviating from the theoretically predicted value of 2. A ratio of 1.5 for the positively charged exciton and biexciton decay time is predicted and exactly matched by the measured ratio indicating identica…
We study spin dynamics of excitons confined in self-assembled CdSe quantum dots by means of optical orientation in magnetic field. At zero field the exciton emission from QDs populated via LO phonon-assisted absorption shows a circular polarization of 14%. The polarization degree of the excitonic emission increases dramatically when a magnetic field is applied. Using a simple model, we extract the exciton spin relaxation times of 100 ps and 2.2 ns in the absence and presence of magnetic field, respectively. With increasing temperature the polarization of the QD emission gradually decreases. Re…
We use a many-body, atomistic empirical pseudopotential approach to predict the multi-exciton emission spectrum of a lens shaped InAs/GaAs self-assembled quantum dot. We discuss the effects of (i) The direct Coulomb energies, including the differences of electron and hole wavefunctions, (ii) the exchange Coulomb energies and (iii) correlation energies given by a configuration interaction calculation. Emission from the groundstate of the $N$ exciton system to the $N-1$ exciton system involving $e_0\to h_0$ and $e_1\to h_1$ recombinations are discussed. A comparison with a simpler single-band, e…
We report semi-empirical pseudopotential calculations of emission spectra of charged excitons and biexcitons in CdSe nanocrystals. We find that the main emission peak of charged multiexcitons - originating from the recombination of an electron in an s-like state with a hole in an s-like state - is blue shifted with respect to the neutral mono exciton. In the case of the negatively charged biexciton, we observe additional emission peaks of lower intensity at higher energy, which we attribute to the recombination of an electron in a p state with a hole in a p state.
A systematic study of the impact of annealing on the electronic properties of single InAs/GaAs quantum dots (QDs) is presented. We are able to record single QD cathodoluminescence spectra and trace the evolution of one and the same QD over several steps of annealing. A systematic reduction of the excitonic fine-structure splitting is reported. In addition the binding energies of different excitonic complexes change dramatically. The results are interpreted in terms of a change of electron and hole wavefunction shape and mutual position.
Cathodoluminescence measurements on single InGaN/GaN quantum dots (QDs) are reported. Complex spectra with up to five emission lines per QD are observed. The lines are polarized along the orthogonal crystal directions [1 1 -2 0] and [-1 1 0 0]. Realistic eight-band k.p electronic structure calculations show that the polarization of the lines can be explained by excitonic recombinations involving hole states which are either formed by the A or the B valence band.
The dephasing time of the lowest bright exciton in CdSe/ZnS wurtzite quantum dots is measured from 5 K to 170 K and compared with density dynamics within the exciton fine structure using a sensitive three-beam four-wave-mixing technique unaffected by spectral diffusion. Pure dephasing via acoustic phonons dominates the initial dynamics, followed by an exponential zero-phonon line dephasing of 109 ps at 5 K, much faster than the ~10 ns exciton radiative lifetime. The zero-phonon line dephasing is explained by phonon-assisted spin-flip from the lowest bright state to dark exciton states. This is…
The binding energies of trions ($X^+$, $X^-$) and biexciton (XX) in self-assembled semiconductor quantum dots (QDs) are very sensitive to the geometry and chemical composition of the QDs, and are random from dots to dots. However, in this letter, we show through analytical and numerical methods that the transition energies of the exciton complexes in self-assembled quantum dots and rings follow a simple and robust rule, i.e., the sum of exciton and biexciton transition energies minus the transition energies of trions is always positive and almost a constant for the same type of quantum dots an…
Excitonic polaron is directly demonstrated for the first time in InAs/GaAs quantum dots with photoluminescence method. A new peak ($s'$) below the ground state of exciton ($s$) comes out as the temperature varies from 4.2 K to 285 K, and a huge anticrossing energy of 31 meV between $s'$ and $s$ is observed at 225 K, which can only be explained by the formation of excitonic polaron. The results also provide a strong evidence for the invalidity of Huang-Rhys formulism in dealing with carrier-longitudinal optical phonon interaction in quantum dot. Instead, we propose a simple two-band model, and …
Eliminating the fine structure splitting (FSS) of excitons in self-assembled quantum dots (QDs) is essential to the generation of high quality entangled photon pairs. It has been shown that the FSS has a lower bound under uniaxial stress. In this letter, we show that the FSS of excitons in a general self-assembled InGaAs/GaAs QD can be fully suppressed via combined stresses along the [110] and [010] directions. The result is confirmed by atomic empirical pseudopotential calculations. For all the QDs we studied, the FSS can be tuned to be vanishingly small ($<$ 0.1 $μ$eV), which is sufficient s…
A systematic study of the impact of annealing on the electronic properties of single InAs/GaAs quantum dots (QDs) is presented. Single QD cathodoluminescence spectra are recorded to trace the evolution of one and the same QD over several steps of annealing. A substantial reduction of the excitonic fine-structure splitting upon annealing is observed. In addition, the binding energies of different excitonic complexes change dramatically. The results are compared to model calculations within eight-band k.p theory and the configuration interaction method, suggesting a change of electron and hole w…
The emission spectral pattern of a charged exciton in a semiconductor quantum dot is composed of a quadruplet of linearly polarized lines in the presence of a magnetic field oriented perpendicularly to the direction of the photon momentum. By measuring the Zeeman splittings, we obtain the effective g factors of the carriers and find that the hole g factor is very sensitive to the QD shape asymmetry. By comparing the effective g factors obtained for the neutral and the charged excitons in the same quantum dot, we uncover the role of Coulomb correlations in these excitonic states.
First-order perturbation theory and many-body Green function analysis are used to quantify the influence of size, surface reconstruction and surface treatment on exciton transport between small silicon quantum dots. Competing radiative processes are also considered in order to determine how exciton transport efficiency is influenced. The analysis shows that quantum confinement causes small (~1 nm) Si quantum dots to exhibit exciton transport efficiencies far exceeding that of their larger counterparts. We also find that surface reconstruction significantly influences the absorption cross secti…
We study the multi-exciton optical spectrum of vertically coupled GaN/AlN quantum dots with a realistic three-dimensional direct-diagonalization approach for the description of few-particle Coulomb-correlated states. We present a detailed analysis of the fundamental properties of few-particle/exciton interactions peculiar of nitride materials. The giant intrinsic electric fields and the high electron/hole effective masses give rise to different effects compared to GaAs-based quantum dots: intrinsic exciton-exciton coupling, non-molecular character of coupled dot exciton wavefunction, strong de…
We report on some surprising optical properties of diluted nitride InGaAs_(1-y)N_y /GaAs (y<<1) pyramidal site-controlled quantum dots, grown by metalorganic vapor phase epitaxy on patterned GaAs (111)B substrates. Microphotoluminescence characterizations showed antibinding exciton/ biexciton behavior, a spread of exciton lifetimes in an otherwise very uniform sample, with unexpected long neutral exciton lifetimes (up to 7 ns) and a nearly zero fine structure splitting on a majority of dots.
Micro-photoluminescence spectroscopy at variable temperature, excitation intensity and energy was performed on a single InAs/AlAs self-assembled quantum dot. The exciton emission line (zero-phonon line, ZPL) exhibits a broad sideband due to exciton-acoustic phonon coupling by the deformation potential mechanism. Additionally, narrow low-energy sidebands at about 0.25 meV of the ZPL are attributed to exciton-acoustic phonon piezoelectric coupling. In lowering the excitation energy or intensity these bands gradually dominate the emission spectrum of the quantum dot while the ZPL disappears. At h…
We describe theoretically novel excitons in self-assembled quantum dots interacting with a two-dimensional electron gas in the wetting layer. In the presence of the Fermi sea, the optical lines become strongly voltage-dependent. If the electron spin is nonzero, the width of optical lines is given by k_BT_K, where T_K is Kondo temperature. If the spin is zero, the exciton couples with the continuum due to Auger-like processes. This leads to anticrossings in a magnetic field. Some of the described phenomena are observed in recent experiments.
Photoluminescence data from single, self-assembled InAs/InP quantum dots in magnetic fields up to 7 T are presented. Exciton g-factors are obtained for dots of varying height, corresponding to ground state emission energies ranging from 780 meV to 1100 meV. A monotonic increase of the g-factor from -2 to +1.2 is observed as the dot height decreases. The trend is well reproduced by sp3 tight binding calculations, which show that the hole g-factor is sensitive to confinement effects through orbital angular momentum mixing between the light-hole and heavy-hole valence bands. We demonstrate tunabi…
Exciton fine structures in cubic III-V semiconductor GaAs, InAs and GaN quantum dots are investigated systematically and the exciton spin relaxation in GaN quantum dots is calculated by first setting up the effective exciton Hamiltonian. The electron-hole exchange interaction Hamiltonian, which consists of the long- and short-range parts, is derived within the effective-mass approximation by taking into account the conduction, heavy- and light-hole bands, and especially the split-off band. The scheme applied in this work allows the description of excitons in both the strong and weak confinemen…
Optically-controlled exciton dynamics in coupled quantum dots is studied. We show that the maximally entangled Bell states and Greenberger-Horne-Zeilinger (GHZ) states can be robustly generated by manipulating the system parameters to be at the avoided crossings in the eigenenergy spectrum. The analysis of population transfer is systematically carried out using a dressed-state picture. In addition to the quantum dot configuration that have been discussed by Quiroga and Johnson [Phys. Rev. Lett. \QTR{bf}{83}, 2270 (1999)], we show that the GHZ states also may be produced in a ray of three quant…
We report on a multiband microscopic theory of many-exciton complexes in self-assembled quantum dots. The single particle states are obtained by three methods: single-band effective-mass approximation, the multiband $k\cdot p$ method, and the tight-binding method. The electronic structure calculations are coupled with strain calculations via Bir-Pikus Hamiltonian. The many-body wave functions of $N$ electrons and $N$ valence holes are expanded in the basis of Slater determinants. The Coulomb matrix elements are evaluated using statically screened interaction for the three different sets of sin…
Using atomistic pseudopotential and configuration-interaction many-body calculations, we predict a metal-nonmetal transition and an excitonic ground state in the InAs/InSb quantum dot (QD) system. For large dots, the conduction band minimum of the InAs dot lies below the valence band maximum of the InSb matrix. Due to quantum confinement, at a critical size calculated here for various shapes, the single-particle gap $E_g$ becomes very small. Strong electron-hole correlation effects are induced by the spatial proximity of the electron and hole wavefunctions, and by the lack of strong (exciton u…
The lack of structural symmetry which usually characterizes semiconductor quantum dots lifts the energetic degeneracy of the bright excitonic states and hampers severely their use as high fidelity sources of entangled photons. We demonstrate experimentally and theoretically that it is always possible to restore the excitonic degeneracy by the simultaneous application of large strain and electric fields, despite the fact that this possibility has fundamentally been doubted. This is achieved by using one external perturbation to align the polarization of the exciton emission along the axis of th…
Using an approximate time-dependent density functional theory method, we calculate the absorption and luminescence spectra for hydrogen passivated silicon nanoscale structures with large aspect ratio. The effect of electron confinement in axial and radial directions is systematically investigated. Excited state relaxation leads to significant Stokes shifts for short nanorods with lengths less than 2 nm, but has little effect on the luminescence intensity. The formation of self-trapped excitons is likewise observed for short nanostructures only; longer wires exhibit fully delocalized excitons w…
We describe the effects of the crossing of the exciton levels in moire quantum dots in external magnetic field. We demonstrate that the unpolarized light can create significant dynamic valley polarization of interlayer excitons in the conditions where the Zeeman energy is much smaller than the thermal energy. The angular momentum is gained by the excitons from the nuclear spin fluctuations. In the $n$-type moire quantum dots for the typical experimental parameters, the unpolarized light can lead to the complete valley polarization of the resident electrons.
Coupling to phonon modes is a primary mechanism of excitonic dephasing and energy loss in semiconductors. However, low-energy phonons in colloidal quantum dots and their coupling to excitons are poorly understood, since their experimental signatures are weak and usually obscured by unavoidable inhomogeneous broadening of colloidal dot ensembles. We use multi-dimensional coherent spectroscopy at cryogenic temperatures to extract the homogeneous nonlinear optical response of excitons in a CdSe/CdZnS core/shell colloidal quantum dot ensemble. Comparison to simulation provides evidence that the ob…
We present results of atomistic empirical pseudopotential calculations and configuration interaction for excitons, positive and negative trions (X\pm), positive and negative quartons (X2\pm) and biexcitons. The structure investigated are laterally aligned InGaAs quantum dot molecules embedded in GaAs under a lateral electric field. The rather simple energetic of excitons becomes more complex in the case of charged quasiparticles but remains tractable. The negative trion spectrum shows four anticrossings in the presently available range of fields while the positive trion shows two. The magnitud…
We measure the photoluminescence (PL) lifetime, $τ$, of excitons in colloidal PbSe nanocrystals (NCs) at low temperatures to 270~mK and in high magnetic fields to 15~T. For all NCs (1.3-2.3~nm radii), $τ$ increases sharply below 10~K but saturates by 500~mK. In contrast to the usual picture of well-separated ``bright" and ``dark" exciton states (found, e.g., in CdSe NCs), these dynamics fit remarkably well to a system having two exciton states with comparable - but small - oscillator strengths that are separated by only 300-900 $μ$eV. Importantly, magnetic fields reduce $τ$ below 10~K, consist…
