Electrical control of hole spin relaxation in charge tunable InAs/GaAs quantum dots

We report on optical orientation of singly charged excitons (trions) in charge-tunable self-assembled InAs/GaAs quantum dots. When the charge varies from 0 to -2, the trion photoluminescence of a single quantum dot shows up and under quasiresonant excitation gets progressively polarized from zero to approximately 100%. This behavior is interpreted as the electric control of the trion thermalization process, which subsequently acts on the hole-spin relaxation driven in nanosecond time scale by the anisotropic electron-hole exchange. This is supported by the excitation spectroscopy and time-resolved measurements of a quantum dot ensemble.     

Stimulated and spontaneous optical generation of electron spin coherence in charged GaAs quantum dots

We report on the coherent optical excitation of electron spin polarization in the ground state of charged GaAs quantum dots via an intermediate charged exciton (trion) state. Coherent optical fields are used for the creation and detection of the Raman spin coherence between the spin ground states of the charged quantum dot. The measured spin decoherence time, which is likely limited by the nature of the spin ensemble, approaches 10 ns at zero field. We also show that the Raman spin coherence in the quantum beats is caused not only by the usual stimulated Raman interaction but also by simultaneous spontaneous radiative decay of either excited trion state to a coherent combination of the two spin states.     

Polarized fine structure in the photoluminescence excitation spectrum of a negatively charged quantum dot

We report polarized photoluminescence excitation spectroscopy of the negative trion in single charge-tunable quantum dots. The spectrum exhibits a p-shell resonance with polarized fine structure arising from the direct excitation of the electron spin triplet states. The energy splitting arises from the axially symmetric electron-hole exchange interaction. The magnitude and sign of the polarization are understood from the spin character of the triplet states and a small amount of quantum dot asymmetry, which mixes the wave functions through asymmetric e-e and e-h exchange interactions.     

Kinetics of an exciton-trion system in shallow GaAs/AlGaAs quantum wells

The formation of three-particle charged exciton complexes (trions) in shallow GaAs/AlGaAs quantum wells in the temperature range 1.7–15 K has been investigated by luminescence spectroscopy and resonant light scattering. The effect of the photon energy and the intensity of additional above-barrier illumination on the trion formation kinetics has been analyzed. It is established that, upon intrawell excitation, illumination leads to the formation of trions when the light photon energy corresponds to the regions of effective formation of trions in the photoluminescence excitation spectra. It is shown that, with an increase in the illumination level, the trion concentration first increases and then reaches a plateau since the quantum well acquires an electric charge whose field equalizes the electron and hole capture rates.     

Nuclear spin nanomagnet in an optically excited quantum dot

Linearly polarized light tuned slightly below the optical transition of the negatively charged exciton (trion) in a single quantum dot causes the spontaneous nuclear spin polarization (self-polarization) at a level close to 100%. The effective magnetic field of spin-polarized nuclei shifts the optical transition energy close to resonance with photon energy. The resonantly enhanced Overhauser effect sustains the stability of the nuclear self-polarization even in the absence of spin polarization of the quantum dot electron. As a result the optically selected single quantum dot represents a tiny magnet with the ferromagnetic ordering of nuclear spins-the nuclear spin nanomagnet.     

Charged-Exciton Complexes in Quantum Dots

It is known experimentally that stable charged-exciton complexes can exist in low-dimensional semiconductor nanostructures. Much less is known about the properties of such charged-exciton complexes since three-body problems are very difficult to be solved, even numerically. Here we introduce the correlated hyperspherical harmonics as basis functions to solve the hyperangular equation for negatively and positively charged excitons (trions) in a harmonic quantum dot. By using this method, we have calculated the energy spectra of the low-lying states of a charged exciton as a function of the radius of quantum dot. Based on symmetry analysis, the level crossover as the dot radius increases can be fully explained as the results of symmetry constraint.``     

Charged-Exciton Complexes in Quantum Dots

It is known experimentally that stable charged-exciton complexes can exist in low-dimensional semiconductor nanostructures. Much less is known about the properties of such charged-exciton complexes since three-body problems are very difficult to be solved, even numerically. Here we introduce the correlated hyperspherical harmonics as basis functions to solve the hyperangular equation for negatively and positively charged excitons (trions) in a harmonic quantum dot. By using this method, we have calculated the energy spectra of the low-lying states of a charged exciton as a function of the radius of quantum dot. Based on symmetry analysis, the level crossover as the dot radius increases can be fully explained as the results of symmetry constraint.     

Charged magneto-exciton states in semiconductor quantum dots

By embedding a layer of self-assembled quantum dots into a field-effect structure, we are able to control the exciton charge in a single dot. We present the results of photoluminescence experiments as a function of both charge and magnetic field. The results demonstrate a hierarchy of energy scales determined by quantization, the direct Coulomb interaction, the electron–electron exchange interaction, and the electron–hole exchange interaction. For excitons up to the triply charged exciton, the behavior can be understood from a model assuming discrete levels within the quantum dot. For the triply charged exciton, this is no longer the case. In a magnetic field, we discover a coherent interaction with the continuum states, the Landau levels associated with the wetting layer.     

Optical orientation and spin relaxation of resident electrons in n-doped InAs/GaAs self-assembled quantum dots

We report on optical orientation of electrons in n-doped InAs/GaAs quantum dots. Under non-resonant cw optical pumping, we measure a negative circular polarization of the luminescence of charged excitons (or trions) at low temperature (T=10 K). The dynamics of the recombination and of the circular polarization is studied by time-resolved spectroscopy. We discuss a simple theoretical model for the trion relaxation, that accounts for this remarkable polarization reversal. The interpretation relies on the bypass of Pauli blocking allowed by the anisotropic electron–hole exchange. Eventually, the spin relaxation time of doping electrons trapped in quantum dots is measured by a non-resonant pump–probe experiment.     

Correlated photons from multi-carrier complexes in GaAs quantum dots

We have studied micro-photoluminescence spectra of a self-assembled single GaAs quantum dot under 8 K. With strong pulsed excitation, the micro-photoluminescence spectrum shows bright emission lines originated from an exciton, a positively charged exciton, and a biexciton, together with weak lower energy emissions reflecting multi-excitonic structures with more carriers. We have identified the origins of these weak emission lines, and showed the existence of charged biexciton states, through single photon correlation measurements and excitation power dependence of the photoluminescence intensity. In addition, investigating the radiative recombination process of the charged biexciton, we have determined the electron–hole exchange energy in the GaAs quantum dot.     

Variation of photoluminescence spectral line shape of monolayer WS2

The origin of the variation of photoluminescence (PL) spectra of monolayer tungsten disulfide (WS₂) is investigated systematically. Dependence of the PL spectrum on the excitation power show that the relatively sharp component corresponds to excitons whereas the broader component at slightly lower energy corresponds to negatively charged trions. PL imaging and second harmonic generation measurements show that the trion signals are suppressed more than the exciton signals near the edges, thereby relatively enhancing the excitonic feature in the PL spectrum and that such relative enhancement of the exciton signals is more pronounced near approximately armchair edges. This effect is interpreted in terms of depletion of free electrons near the edges caused by structural defects and adsorption of electron acceptors such as oxygen atoms.     

Behavior of excitons and trions in CdTe/CdMgTe quantum-well structures with variations in temperature

The temperature-induced variations in the photoluminescence spectra measured in a magnetic field of trions and excitons in CdTe/CdMgTe quantum wells with modulated doping are studied. It is found that the temperature-induced redistribution of the intensity between the exciton and trion emission lines in a magnetic field is opposite to that expected from the simple Boltzmann distribution model. Coupled rate equations for the trion-exciton system are solved to construct the temperature dependences of the exciton and trion emission line intensities. The relations thus calculated are in good agreement with experiment.     

Optical pumping of the electronic and nuclear spin of single charge-tunable quantum dots

We present a comprehensive examination of optical pumping of spins in individual GaAs quantum dots as we change the net charge from positive to neutral to negative with a charge-tunable heterostructure. Negative photoluminescence polarization memory is enhanced by optical pumping of ground state electron spins, which we prove with the first measurements of the Hanle effect on an individual quantum dot. We use the Overhauser effect in a high longitudinal magnetic field to demonstrate efficient optical pumping of nuclear spins for all three charge states of the quantum dot.     

Charged excitons in quantum dots: novel magnetic behavior and Auger processes

We describe theoretically multiply-charged excitons interacting with a continuum of delocalized states. Such excitons exist in relatively shallow quantum dots and have been observed in recent optical experiments on InAs self-assembled dots. The interaction of an exciton and delocalized states occurs via Auger-like processes. To describe the optical spectra, we employ the Anderson-like Hamiltonian by including the interaction between the localized exciton and delocalized states of the wetting layer. In the absence of a magnetic field, the photoluminescence line shapes exhibit interference effects. When a magnetic field is applied, the photoluminescence spectrum demonstrates anticrossings with the Landau levels of the extended states. We show that the magnetic-field behavior of charged excitons is very different to that of diamagnetic excitons in three and two-dimensional systems.     

Electron–Nuclear Spin Dynamics in Semiconductor QDs

This work presents an overview of investigations of the nuclear spin dynamics in nanostructures with negatively charged InGaAs/GaAs quantum dots characterized by strong quadrupole splitting of nuclear spin sublevels. The main method of the investigations is the experimental measurements and the theoretical analysis of the photoluminescence polarization as a function of the transverse magnetic field (effect Hanle). The dependence of the Hanle curve profile on the temporal protocol of optical excitation is examined. Experimental data are analyzed using an original approach based on separate consideration of behavior of the longitudinal and transverse components of the nuclear polarization. The rise and decay times of each component of the nuclear polarization and their dependence on transverse magnetic field strength are determined. To study the role of the Knight field in the dynamic of nuclear polarization, a weak additional magnetic field parallel to the optical axis is used. We have found that, only taking into account the nuclear spin fluctuations, we can accurately describe the measured Hanle curves and evaluate the parameters of the electron–nuclear spin system in the studied quantum dots. A new effect of the resonant optical pumping of nuclear spin polarization in an ensemble of the singly charged (In,Ga)As/GaAs quantum dots subjected to a transverse magnetic field is discussed. Nuclear spin resonances for all isotopes in the quantum dots are detected in that way. In particular, transitions between the states split off from the ±1/2 doublets by the nuclear quadrupole interaction are identified.     

Optical pumping and a nondestructive readout of a single magnetic impurity spin in an InAs/GaAs quantum dot

We report on the resonant optical pumping of the | ± 1? spin states of a single Mn dopant in an InAs/GaAs quantum dot which is embedded in a charge tunable device. The experiment relies on a W scheme of transitions reached when a suitable longitudinal magnetic field is applied. The optical pumping is achieved via the resonant excitation of the central Λ system at the neutral exciton X(0) energy. For a specific gate voltage, the redshifted photoluminescence of the charged exciton X- is observed, which allows a nondestructive readout of the spin polarization. An arbitrary spin preparation in the | + 1? or |-1? state characterized by a polarization near or above 50% is evidenced.     

Exciton-electron interaction in quantum wells with a two dimensional electron gas of low density

II–VI quantum-well structures containing a 2DEG of low density have been investigated by means of polarized photoluminescence, photoluminescence excitation and reflectivity in external magnetic fields up to 20 T. The spin splittings of the exciton X and the negatively charged exciton X ⁻ are measured as a function of the magnetic field strength. The behavior of the magnetic-field-induced polarization degree of the luminescence line related to X ⁻ demonstrates the formation process of negatively charged excitons from excitons and free carriers polarized by the external magnetic field. We have determined the binding energies of the trion formed either with the heavy-hole or the light-hole exciton. The optically detected magnetic resonance (ODMR) technique was applied for the first time to study the optical transition processes in a nanosecond timescale. The electron ODMR was observed with the detection on either the direct exciton or the negatively charged exciton X. Further evidence for the interaction of excitons with the electrons of the two-dimensional gas are demonstrated by a combined exciton-cyclotron resonance line observed in reflectivity and luminescence excitation, shake-up processes observed in photoluminescence, as well as inelastic and spin-dependent scattering processes. Fiz. Tverd. Tela (St. Petersburg) 41, 831–836 (May 1999) Published in English in the original Russian journal. Reproduced here with stylistic changes by the Translation Editor.     

Femtosecond study of the interplay between excitons, trions, and carriers in (Cd,Mn)Te quantum wells

We study the absorption by neutral excitons and positively charged excitons (trions) following a femtosecond, circularly polarized, resonant pump pulse. Three populations are involved: free holes, excitons, and trions, all exhibiting transient spin polarization. In particular, a polarization of the gas of free holes is created by the formation of trions. The evolution of these populations is described, including spin flip and trion formation. We evaluate the contributions of phase space filling and spin-dependent screening. We propose a new explanation of the oscillator strength stealing phenomena observed in doped quantum wells, based on the screening of neutral excitons by charge carriers. We have also found that binding holes into charged excitons excludes them from the interaction with the rest of the system, so that oscillator strength stealing is partially blocked.     

Stabilization energies of charged multiexciton complexes calculated at configuration interaction level

Recombination and stabilization energies of multiexcitons confined in positively and negatively charged semiconductor InGaAs/GaAs quantum dot (QD) samples have been studied by employing large-scale configuration interaction (CI) calculations. The CI calculations show that at most six electrons or two holes can be confined in the QD. Multiply charged multiexciton complexes with up to five excess electrons or two excess holes are also found to be stable, even when a few electron–hole pairs are present in the QD. The chemical potential functions for charged QD samples do not possess the pronounced stepped form as obtained for the corresponding neutral multiexciton complexes. The negatively and the positively charged excitons (negative and positive trions) lie lower in energy as compared to a neutral exciton and a single non-interacting charge carrier in the lowest single-particle state of another quantum dot. The other charged multiexciton complexes studied are not confined with respect to the corresponding neutral multiexciton and a non-interacting charge carrier. To include the contributions from the heavy-hole light-hole (HH–LH) coupling, a perturbative treatment of the band-mixing effects was implemented. The perturbation-theory calculations show that the HH–LH coupling does not shift the energies in the present InGaAs/GaAs QD sample.     

Coherent spin precession of electrons and excitons in charge tunable InP quantum dots

Coherent spin precession of electrons and excitons is observed in charge tunable InP quantum dots under the transverse magnetic field by means of time-resolved Kerr rotation. In a quantum dot doped by one electron, spin precession of the doped electron in the quantum dot starts out of phase with spin precession of the doped electrons in a GaAs substrate just after a trion is formed and persists for more than 2 ns even after the trion recombines. Simultaneously spin precession of a trion (hole) starts. Observation of spin precession of both a doped electron and a trion (hole) confirms creating coherent superposition of an electron and a trion as the initialization process of spin of doped electrons in quantum dots. In a neutral quantum dot, the exciton spin precession starts out of phase with spin precession of the doped electrons in a GaAs substrate and the precession frequency does not converge to 0 at the zero field limit. It contains the electron–hole exchange interaction and corresponds to the splitting between bright and dark excitons under the transverse magnetic field.