We introduced an elevated trap technique and exploited it for lowering the effective temperature of indirect excitons. We observed narrow photoluminescence lines which correspond to the emission of individual states of indirect excitons in a disorder potential. We studied the effect of exciton-exciton interaction on the localized and delocalized exciton states and found that the homogeneous line broadening increases with density and dominates the linewidth at high densities.
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…
Characteristics of GaAs/In$_{x}$Ga$_{1-x}$As/GaAs heterostructures with a single quantum well, which were obtained at various growth parameters, are evaluated according to the results of measurements of low-temperature photoluminescence spectra and their corresponding theoretical analysis.
Two-dimensional stacking fault defects embedded in a bulk crystal can provide a homogeneous trapping potential for carriers and excitons. Here we utilize state-of-the-art structural imaging coupled with density functional and effective-mass theory to build a microscopic model of the stacking-fault exciton. The diamagnetic shift and exciton dipole moment at different magnetic fields are calculated and compared with the experimental photoluminescence of excitons bound to a single stacking fault in GaAs. The model is used to further provide insight into the properties of excitons bound to the dou…
The magnetophotoluminescence (MPL) behavior of a GaAs/Al(0.3)Ga(0.7)As single heterojunction has been investigated to 60T. We observed negatively charged singlet and triplet exciton states that are formed at high magnetic fields beyond the nu=1 quantum Hall state. The variation of the charged exciton binding energies are in good agreement with theoretical predictions. The MPL transition intensities for these states showed intensity variations (maxima and minima) at the nu=1/3 and 1/5 fractional quantum Hall (FQH) state as a consequence of a large reduction of electron-hole screening at these f…
We present a systematic study of the exciton/electron-hole plasma photoluminescence dynamics in bulk GaAs for various lattice temperatures and excitation densities. The competition between the exciton and electron-hole pair recombination dominates the onset of the luminescence. We show that the metal-to-insulator transition, induced by temperature and/or excitation density, can be directly monitored by the carrier dynamics and the time-resolved spectral characteristics of the light emission. The dependence on carrier density of the photoluminescence rise time is strongly modified around a latt…
Photoluminescence (PL) and reflectivity spectra of a high-quality InGaAs/GaAs quantum well structure reveal a series of ultra-narrow peaks attributed to the quantum confined exciton states. The intensity of these peaks decreases as a function of temperature, while the linewidths demonstrate a complex and peculiar behavior. At low pumping the widths of all peaks remain quite narrow ($< 0.1$ meV) in the whole temperature range studied, $4 - 30K$. At the stronger pumping, the linewidth first increases and than drops down with the temperature rise. Pump-probe experiments show two characteristic ti…
We investigate pump induced modulation in the temporal evolution of the excitonic coherent polarization generated by a probe pulse in GaAs multiple quantum wells. For this, we perform fs time resolved pump-probe reflectivity measurements using frequency upconversion at both positive and negative pump-probe delays. A contribution arising from interference of excitonic linear and nonlinear polarization, which is usually not considered in describing pump-probe experiments, is required to understand the results.
The exciton spin dynamics are investigated both experimentally and theoretically in two-monolayer-thick GaAs/AlAs quantum wells with an indirect band gap and a type-II band alignment. The magnetic-field-induced circular polarization of photoluminescence, $P_c$, is studied as function of the magnetic field strength and direction as well as sample temperature. The observed nonmonotonic behaviour of these functions is provided by the interplay of bright and dark exciton states contributing to the emission. To interpret the experiment, we have developed a kinetic master equation model which accoun…
Magnetic-field driven hybridization of heavy- and light-hole Rydberg excitons in GaAs quantum wells
Universidad Autónoma de Madrid（马德里自治大学）；Condensed Matter Physics Center (IFIMAC)（凝聚态物理中心（IFIMAC））；CNR Nanotec, Institute of Nanotechnology（意大利国家研究委员会纳米技术研究所）；School of Physics and Astronomy, Monash University（莫纳什大学物理与天文学院）
In-plane magnetic field is found to change drastically the photoluminescence spectra and kinetics of interwell excitons in GaAs/AlGaAs coupled quantum wells. The effect is due to the in-plane magnetic field induced displacement of the interwell exciton dispersion in a momentum space, which results in the transition from the momentum-space direct exciton ground state to the momentum-space indirect exciton ground state. In-plane magnetic field is, therefore, an effective tool for the exciton dispersion engineering.
The variety of excitonic states in tungsten-based dichalcogenide monolayers stems from unique interplay between the spin and valley degrees of freedom. One of the exciton species is the indirect exciton (momentum or valley dark), which is responsible to a series of resonances when the monolayer is charge neutral. We investigate the short-range electron-hole exchange interaction of the indirect exciton, as well as its recombination mechanism mediated by impurities. The analysis provides thorough understanding of the energy and polarization of the zero-phonon indirect exciton resonance in the em…
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 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 derive analytically the change of exciton fine structure splitting (FSS) under the external stresses in the self-assembled InAs/GaAs quantum dots using the Bir-Pikus model. We find that the FSS change is mainly due to the strain induced valence bands mixing and valence-conduction band coupling. The exciton polarization angle under strain are determined by the argument of the electron-hole off-diagonal exchange integrals. The theory agrees well with the empirical pseudopotential calculations.
Monolayer transition metal dichalcogenides are a promising platform to investigate many-body interactions of excitonic complexes. In monolayer tungsten diselenide, the ground-state exciton is dark (spin-indirect), and the valley degeneracy allows low-energy dark momentum-indirect excitons to form. Interactions between the dark exciton species and the optically accessible bright exciton (X) are likely to play significant roles in determining the optical properties of X at high power, as well as limiting the ultimate exciton densities that can be achieved, yet so far little is known about these …
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…
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…
A variational calculus method is applied for hydrogen-like impurities states and exciton states in AlGaAs/GaAs quantum wells within the effective masses approach. The hamiltonian is separated into radial and transversal parts to be considered and optimized using trial wavefunctions. The results satifsy the well-known cases of three-dimentional and two-dimentional hydrogen. The donor and exciton bound energy is shown to decrease while widthening the quantum well. The non-symmetrical donor position also decreases the bound energy.
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…
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.
We have observed photoinduced negative optical conductivity, or gain, in the terahertz frequency range in a GaAs multiple-quantum-well structure in a strong perpendicular magnetic field at low temperatures. The gain is narrow-band: it appears as a sharp peak (linewidth $<$0.45 meV) whose frequency shifts with applied magnetic field. The gain has a circular-polarization selection rule: a strong line is observed for hole-cyclotron-resonance-active polarization. Furthermore, the gain appears only when the exciton $1s$ state is populated, which rules out intraexcitonic transitions to be its origin…
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…
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 …
Electronic structures of wurtzite GaAs nanowires in the [0001] direction were studied using first-principles calculations. It was found that the band gap of GaAs nanowires experience a direct-to-indirect transition when the diameter of the nanowires is smaller than ~28 Å. For those thin GaAs nanowires with an indirect band gap, it was found that the gap can be tuned to be direct if a moderate external uniaxial strain is applied. Both tensile and compressive strain can trigger the indirect-to-direct gap transition. The critical strains for the gap-transition are determined by the energy crossov…
All known superfluid and superconducting states of condensed matter are enabled by composite bosons (atoms, molecules, Cooper pairs) made of an even number of fermions. Temperatures where such macroscopic quantum phenomena occur are limited by the lesser of the binding energy and the degeneracy temperature of the bosons. High critical temperature cuprate superconductors set the present record of ~100 K. Here we propose a design for artificially structured materials to rival this record. The main elements of the structure are two monolayers of a transition metal dichalcogenide separated by an a…
We report here a giant $\left|χ_{baa}^{2}\right|=$780 pm/V second harmonic and $\left|χ_{aaaa}^{3}\right|=$1.4$\times$10$^{-17}$ m$^{2}$/V$^{2}$ third harmonic signal from single atomic sheet of buckled hexagonal GaAs. We demonstrate this through the solution of an ab-initio real-time Bethe-Salpeter equation by including the electron-hole screened-exchange self-energy. The coupling between time-dependent external electric field and correlated electrons is treated within the modern theory of polarization. The result of our calculation envisage monolayer GaAs to be a prominent member in the mate…
We present a comprehensive study of the optical properties of InAs/InP self-assembled quantum dots (QDs) using an empirical pseudopotential method and configuration interaction treatment of the many-particle effects. The results are compared to those of InAs/GaAs QDs. The main results are: (i) The alignment of emission lines of neutral exciton, charged exciton and biexciton in InAs/InP QDs is quite different from that in InAs/GaAs QDs. (ii) The hidden correlation in InAs/InP QDs is 0.7 - 0.9 meV, smaller than that in InAs/GaAs QDs. (iii) The radiative lifetimes of neutral exciton, charged exci…
We propose a double channel mechanism for the formation of charged excitons (trions); they are formed through bi- and tri-molecular processes. This directly implies that both negatively and positively charged excitons coexist in a quantum well, even in the absence of excess carriers. The model is applied to a time-resolved photoluminescence experiment performed on a very high quality InGaAs quantum well sample, in which the photoluminescence contributions at the energy of the trion, exciton and at the band edge can be clearly separated and traced over a broad range of times and densities. The …
Carrier and spin recombination are investigated in p-type GaAs of acceptor concentration NA = 1.5 x 10^(17) cm^(-3) using time-resolved photoluminescence spectroscopy at 15 K. At low pho- tocarrier concentration, acceptors are mostly neutral and photoelectrons can either recombine with holes bound to acceptors (e-A0 line) or form excitons which are mostly trapped on neutral acceptors forming the (A0X) complex. It is found that the spin lifetime is shorter for electrons that recombine through the e-A0 transition due to spin relaxation generated by the exchange scattering of free electrons with …
By combining an atomistic pseudopotential method with the configuration interaction approach, we predict the pressure dependence of the binding energies of neutral and charged excitons: $X^0$ (neutral monoexciton), $X^{-}$ and $X^{+}$ (charged trions), and $XX^0$ (biexciton) in lens-shaped, self-assembled In$_{0.6}$Ga$_{0.4}$As/GaAs quantum dots. We predict that (i) with applied pressure the binding energy of $X^0$ and $X^+$ increases and that of $X^-$ decreases, whereas the binding energy of $XX^0$ is nearly pressure independent. (ii) Correlations have a small effect in the binding energy of …
We present a theory of spatially indirect exciton condensate states in systems composed of a pair of electrically isolated Bernal graphene bilayers. The ground state phase diagram in a two-dimensional displacement-field/inter-bilayer-bias space includes layer-polarized semiconductors, spin-density-wave states, exciton condensates, and states with mixed excitonic and spin order. We find that two different condensate states, distinguished by a chirality index, are stable under different electrical control conditions.
We present the direct measurements of magnetoexciton transport. Excitons give the opportunity to realize the high magnetic field regime for composite bosons with magnetic fields of a few Tesla. Long lifetimes of indirect excitons allow the study kinetics of magnetoexciton transport with time-resolved optical imaging of exciton photoluminescence. We performed spatially, spectrally, and time-resolved optical imaging of transport of indirect excitons in high magnetic fields. We observed that increasing magnetic field slows down magnetoexciton transport. The time-resolved measurements of the magne…
We investigate the lifetime of indirect excitons in extremely high purity diamond grown by the chemical vapor deposition method. A clear correlation is found between the lifetime and small strain (magnitude $< $10$^{-4}$) assessed using birefringence, thanks to the effective absence of impurity traps. A surface recombination model, extended for nonradiative recombination at dislocations due to exciton diffusion, is proposed to explain the temperature-dependent lifetime. Based on the derived radiative lifetime, our model enables the prediction of lifetimes at any temperature as well as the high…
A quantitative analysis of the excitonic luminescence efficiency in hexagonal boron nitride (hBN) is carried out by cathodoluminescence in the ultraviolet range and compared with zinc oxide and diamond single crystals. A high quantum yield value of ~50% is found for hBN at 10 K comparable to that of direct bandgap semiconductors. This bright luminescence at 215 nm remains stable up to room temperature, evidencing the strongly bound character of excitons in bulk hBN. Ab initio calculations of the exciton dispersion confirm the indirect nature of the lowest-energy exciton whose binding energy is…
We study photon bunching phenomena associated with biexciton-exciton cascade in single GaAs self-assembled quantum dots. Experiments carried out with a pulsed excitation source show that significant bunching is only detectable at very low excitation, where the typical intensity of photon streams is less than the half of their saturation value. Our findings are qualitatively understood with a model which accounts for Poissonian statistics in the number of excitons, predicting the height of a bunching peak being determined by the inverse of probability of finding more than one exciton.
Exciton-polaritons are hybrid light-matter states that arise from strong coupling between an exciton resonance and a photonic cavity mode. As bosonic excitations, they can undergo a phase transition to a condensed state that can emit coherent light without a population inversion. This aspect makes them good candidates for thresholdless lasers, yet short exciton-polariton lifetime has made it difficult to achieve condensation at very low power densities. In this sense, long-lived symmetry-protected states are excellent candidates to overcome the limitations that arise from the finite mirror ref…
Monolayer black and blue phosphorenes possess electronic and optical properties that result in unique features when the two materials are stacked. We devise a low-strain van-der-Waals double layer and investigate its properties with ab initio many-body perturbation theory techniques. A type-II band alignment and optical absorption in the visible range are found. The study demonstrates that spatially indirect excitons with full charge separation can be obtained between two layers with the same elemental composition but different crystalline structure, proving the system interesting for further …
The novel method of observation and controlling of Bose-Einstein condensation in the system of spatially and momentum-space indirect excitons in coupled quantum wells using in-plane magnetic and normal electric fields is proposed. Fields are used for exciton dispersion engeneering. In the presence of in-plane magnetic field ground state of spatially indirect exciton becomes also indirect in the momentum space. Manipulation of electric field magnitude is used for tuning to resonance of transition of "dark" long-life spatially and momentum-space indirect exciton in condensate into spatially and …
Electron-hole excitations in the surface bands of GaAs(110) are analyzed using constrained density-functional theory calculations. The results show that Frenkel-type autolocalized excitons are formed. The excitons induce a local surface unrelaxation which results in a strong exciton-exciton attraction and makes complexes of two or three electron-hole pairs more favorable than separate excitons. In such microscopic exciton "droplets" the electron density is mainly concentrated in the dangling orbital of a surface Ga atom whereas the holes are distributed over the bonds of this atom to…
