Two-photon correlations of luminescence at the Bose-Einstein condensation of dipolar excitons

Correlations of the luminescence intensity (the second-order correlation function g ⁽²⁾(τ)), where τ is the delay time between the photons detected in pairs) under the conditions of the Bose-Einstein condensation (BEC) of dipolar excitons has been studied in a temperature range of 0.45–4.2 K. Photoexcited dipolar excitons have been accumulated in a lateral trap in a GaAs/AlGaAs Schottky diode with a 25-nm wide single quantum well with an electric bias applied across the heterolayers. Two-photon correlations have been measured with the use of a two-beam intensity interferometer with a time resolution of }~0.4 ns according to the well-known classical Hanbury-Brown-Twiss scheme. The photon bunching has been observed at the onset of Bose-Einstein condensation manifested by the appearance of a narrow exciton condensate line in the luminescence spectrum at an increase in the optical pumping (the line width near the threshold is ?200 μeV). At the same time, the two-photon correlation function itself obeys the super-Poisson distribution, g ⁽²⁾(τ) > 1, at time scale τ_c ? 1 ns of the system coherence. The photon bunching is absent at a pumping level substantially below the condensation threshold. The effect of bunching also decreases at pumping significantly above the threshold, when the narrow exciton condensate line starts to dominate in the luminescence spectra, and finally disappears with the further increase in the optical excitation. In this region, the distribution of pair photon correlations is a Poisson distribution manifesting the united quantum coherent state of the exciton condensate. Under the same conditions, the first-order spatial correlation function g ⁽¹⁾(r) determined from the interference pattern of the luminescence signals from the spatially separated parts of the condensate at constant pumping remains noticeable at distances of no less than 4 μm. The discovered effect of photon bunching is very sensitive to temperature and decreases by several times with a temperature increase in the range of 0.45–4.2 K. Assuming that the luminescence of the dipolar excitons directly reflects the coherence properties of the gas of interacting excitons, the discovered photon bunching at the onset of condensation, where the fluctuations of the exciton density and, consequently, of the luminescence intensity are most significant, indicates a phase transition in the interacting Bose gas of excitons, which is an independent way of detecting the Bose-Einstein condensation of excitons.     

Coulomb binding of electrons to multiply charged GaSb/GaAs self-assembled quantum dots

We explore the Coulomb binding of electrons to holes confined to type-II GaSb self-assembled quantum dots. We demonstrate that at low laser power electrons are more weakly bound to holes trapped by the dots than to holes in the wetting layer. On the other hand, at high laser power the hydrogenic binding energy of dot excitons increases by more than a factor of two, and so exceeds that of wetting layer excitons. We attribute this to the strong binding of ‘core’ electrons to dots that are highly charged with holes by optical pumping.     

Excitons in hybrid organic-inorganic nanostructures

In two-dimensional heterostructures made of semiconductor and organic layers, when resonance between the Wannier and Frenkel excitons is realized, the dipole-dipole interaction coupling them leads to novel effects. First, we discuss the pronounced nonlinear optical properties of the hybrid Frenkel-Wannier excitons appearing when the energy splitting of the excitonic spectrum is large compared to the exciton linewidths (the case of strong resonant coupling). Next, we consider the case of weak resonant coupling for which the Förster mechanism of energy transfer from an inorganic quantum well to an organic overlayer is of great interest: the electrical pumping of excitons in the semiconductor quantum well could be employed to turn on efficiently the organic material luminescence.     

Rabi oscillations of excitons in single quantum dots

Transient nonlinear optical spectroscopy, performed on excitons confined to single GaAs quantum dots, shows oscillations that are analogous to Rabi oscillations in two-level atomic systems. This demonstration corresponds to a one-qubit rotation in a single quantum dot which is important for proposals using quantum dot excitons for quantum computing. The dipole moment inferred from the data is consistent with that directly obtained from linear absorption studies. The measurement extends the artificial atom model of quantum dot excitonic transitions into the strong-field limit, and makes possible full coherent optical control of the quantum state of single excitons using optical pi pulses.     

Micro-Photoluminescence Confocal Mapping of Single V-Grooved GaAs Quantum Wire

We perform the micro-photoluminescence measurement at low temperatures and a scanning optical mapping with high spatial resolution of a single V-grooved GaAs quantum wire modified by the selective ion-implantation and rapid thermally annealing. While the mapping shows the luminescences respectively from the quantum wires and from quantum well areas between quantum wires in general, the micro-photoluminescence at liquid He temperatures reveals a plenty of spectral structures of the PL band for a single quantum wire. The spectral structures are attributed to the inhomogeneity and non-uniformity of both the space structure and compositions of real wires as well as the defects nearby the interface between quantum wire and surrounding quantum well structures. All these make the excitons farther localized in quasi-zero-dimensional quantum potential boxes related to these non-uniformity and/or defects. The results also demonstrate the ability of micro-photoluminescence measurement and mapping for the characterization of both opto-electronic and structural properties of real quantum wires.     

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.     

Interwell excitons in GaAs/AlGaAs double quantum wells and their collective properties

Luminescence spectra of interwell excitons in GaAs/AlGaAs double quantum wells with electric-field-tilted bands (n-i-n) structures were studied. In these structures the electron and the hole in the interwell exciton are spatially separated between neighboring quantum wells by a narrow AlAs barrier. Under resonant excitation by circularly polarized light the luminescence line of the interwell excitons exhibited appreciable narrowing as their concentration increased and the degree of circular polarization of the photoluminescence increased substantially. Under resonant excitation by linearly polarized light the alignment of the interwell excitons increased as a threshold process with increasing optical pumping. By analyzing time-resolved spectra and the kinetics of the photoluminescence intensity under pulsed excitation it was established that under these conditions the rate of radiative recombination increases substantially. The observed effect occurs at below-critical temperatures and is interpreted in terms of the collective behavior of the interwell excitons. Studies of the luminescence spectra in a magnetic field showed that the collective exciton phase is dielectric and in this phase the interwell excitons retain their individual properties.     

Phase coherent photorefractivity in ZnSe single quantum wells

We observe an efficient phase coherent photorefractive effect in ZnSe single quantum wells for ultrashort light pulses resonant to the excitonic transition. The effect is attributed to the formation of an electron grating in the quantum well induced by the interference of coherent excitons that preserve phase and polarization of the incident light fields. All characteristic features of the diffracted signal are explained and reproduced by numerical calculations that are based on the optical Bloch equations for a three-level system.     

Collective state in a bose gas of interacting interwell excitons

Experiments associated with direct observations of a collective state in a gas of interacting interwell excitons in GaAs/AlGaAs double quantum wells are discussed. The structures constitute Schottky photodiodes. In a metallic gate, circular windows of various sizes (diameters of 2 to 20 μm) are etched by means of electronic-beam lithography. Through these windows, the photoluminescence of interwell and intrawell excitons is excited and detected. A microscopic device allows the observation of the spatial structure of luminescence with a resolution of 1 μm through the windows of a sample placed in superfluid helium. Using optical interference filters, the spatial structure of the luminescence is analyzed selectively in the spectrum for interwell and intrawell excitons under the same experimental conditions. It is found that the photoluminescence of interwell excitons under certain conditions exhibits an axisymmetric spatial structure: along the perimeter of the windows through which the photoluminescence is observed, a regular ring pattern of equidistant bright spots of the luminescence of interwell excitons appears. This structure appears only above the photoexcitation power threshold and the number of equidistant bright spots in the ring increases with the pumping power. At high pumping powers, the structure of distinct periodic luminescence spots is smeared. At a fixed pumping power, the phenomenon exhibits explicit critical temperature dependence: the structure of regularly located luminescence spots is smeared at T > 4 K. Axisymmetric spatial configurations of equidistant luminescence spots are observed in windows of the diameters 2, 5, and 10 μm. For intrawell excitons, the spatial structure of luminescence is not observed under similar experimental conditions: the luminescence of intrawell excitons is spatially uniform in all the windows under investigation. The effect is a result of the collective behavior of interacting interwell excitons.     

Stark shifts of charged particles in semiconductor quantum wells

 We calculate the effect of a homogeneous electric field on electrons, holes and excitons confined in a quantum well structure consisting of alternate thin layers of well and barrier material. The electric field which acts perpendicular to the quantum well is taken as a perturbation on the quantum well structure confining the charges. The electron and hole energies in the conduction and valence subbands are calculated by solving a one-dimensional Schr?dinger equation. The exciton binding energy is calculated using an improved excitonic model. Results obtained indicate the importance of higher-order excitons in optical transitions at high electric fields. Received: 29 February 1996/Accepted: 19 August 1996     

Electro-optical trap for dipolar excitons in a GaAs/AlAs Schottky diode with a single quantum well

An electro-optical trap for spatially indirect dipolar excitons has been implemented in a GaAs/AlAs Schottky diode with a 400-Å-wide single quantum well. In the presence of a bias voltage applied to a gate, the trap for excitons appears upon ring illumination of the structure by a continuous-wave or pulsed laser generating hot electron-hole pairs in the quantum well. A barrier for excitons collected inside the illuminated ring appears because of the screening of the applied electric field by nonequilibrium carriers directly in the excitation region. Excitons are collected inside the ring owing to the ambipolar drift of carriers and dipole-dipole exciton repulsion in the optical pump region. For dipolar excitons thus collected in the center of the ring electrooptical trap, a significant narrowing of the luminescence line that accompanies an increase in the density of excitations indicates the collective behavior of dipolar excitons.     

Few-particle effects in semiconductor quantum dots: observation of multicharged excitons

We investigate experimentally and theoretically few-particle effects in the optical spectra of single quantum dots (QDs). Photodepletion of the QD together with the slow hopping transport of impurity-bound electrons back to the QD are employed to efficiently control the number of electrons present in the QD. By investigating structurally identical QDs, we show that the spectral evolutions observed can be attributed to intrinsic, multi-particle-related effects, as opposed to extrinsic QD-impurity environment-related interactions. From our theoretical calculations we identify the distinct transitions related to excitons and excitons charged with up to five additional electrons, as well as neutral and charged biexcitons.     

基于有机异质结的有机-无机复合单量子阱发光性质的研究

制备了包含有机异质结的有机-无机复合单量子阱器件ITO＼SiO₂(60 nm)＼MEH-PPV(40 nm)＼Alq₃(40 nm)＼SiO₂(60 nm)＼Al。通过对这种新结构器件光致发光和电致发光的研究,发现介电限域效应和量子尺寸效应对它的发光和电学性质有明显的影响。在交流电驱动下,OISQWOH(organic-inorganic quantum well with organic heterojunction)有三个发光峰：410,510和590 nm。其中410 nm的发光与MEH-PPV的扩展态相关,510和590 nm的发光分别来源于Alq₃和MEH-PPV的激子发光。     

Quantum wells for femtosecond optoelectronics applications

The ultrafast nonlinear optical properties of quantum well excitons have been studied extensively in recent years. Quantum well excitons, which are sharp and well-resolved at room temperature, are well suited to optoelectronics applications, having large electroabsorption response. In this review, we discuss experiments which use simultaneously the nonlinear optical response of the quantum well exciton and the electroabsorption response in order to characterize electrical signals in the femtosecond time scale. In addition, we discuss intrinsic speed limitations in excitonic optoelectronics and extensions to one- and two-dimensional spatiotemporal field mapping.     

Temperature dependence of luminescence intensity under Bose condensation of interwell excitons

Photoluminescence of interwell excitons in GaAs/AlGaAs double quantum wells (n-i-n heterostructure) containing large-scale random potential fluctuations in the planes of heteroboundaries is studied. The properties of excitons, in which a photoexcited electron and a hole are spatially separated in neighboring quantum wells, were investigated upon variation of the power density of off-resonance laser excitation and temperature (1.5–4.2 K), both under lateral (in the heteroboundary plane) confinement of the excitation region to a few micrometers and without such a limitation (directly from the region of laser-induced photoexcitation focused to a spot not exceeding 30 μ. Under low pumping (with a power smaller than a microwatt), interwell excitons are strongly localized due to small-scale random potential fluctuations and the corresponding photoluminescence line is nonhomogeneously broadened to 2.5–3.0 meV. With increasing pumping power, the narrow line of delocalized excitons with a width of approximately 1 meV emerges in a threshold manner (the intensity of this line increases superlinearly near the threshold with increasing pumping). For a fixed pumping, the intensity of this line decreases linearly upon heating until it completely vanishes from the spectrum. The observed effect is attributed to Bose condensation in a quasi-two-dimensional system of interwell excitons. Within the proposed model, we show that the linear mode in the behavior of the luminescence intensity until its disappearance in the continuum of the photoluminescence spectrum upon a change in temperature is observed only for the condensed part of interwell excitons. At the same time, the luminescence of the above-the-condensate part of excitons is almost insensitive to temperature variations in the temperature range studied.     

Emission from neutral and charged excitons in a single quantum dot in a magnetic field

We report on optical spectroscopy of self-assembled InAs quantum dots in a magnetic field. We describe how we measure the emission characteristics of a single quantum dot (QD) in high magnetic fields at low temperature using a miniature, fiber-based confocal microscope. Example results are presented on a QD whose charge can be controlled using a field-effect device. For the uncharged, singly and doubly charged excitons we find a diamagnetism and the spin Zeeman effect. In contrast, for the triply-charged exciton we find a fundamentally different behavior. Anti-crossings in magnetic field imply that confined states of the QD are hybridized with Landau-like levels associated with the two-dimensional continuum.     

High-resolution nonlinear laser spectroscopy of exciton relaxation in GaAs quantum wells

This paper describes measurements of exciton relaxation in GaAs/AlGaAs quantum well structures based on high resolution nonlinear laser spectroscopy. The nonlinear optical measurements show that low energy excitons can be localized by monolayer disorder of the quantum well interface. We show that these excitons migrate between localization sites by phonon assisted migration, leading to spectral diffusion of the excitons. The frequency domain measurements give a direct measure of the quasi-equilibrium exciton spectral redistribution due to exciton energy relaxation, and the temperature dependence of the measured migration rates confirms recent theoretical predictions. The observed line shapes are interpreted based on solutions we obtain to modified Bloch equations which include the effects of spectral diffusion.     

The electronic and optical properties of a triexciton in CdSe/ZnS core/shell quantum dot nanocrystals

In the study, we aim to investigate the electronic and optical properties of single excitons, biexcions and triexcitons in a CdSe/ZnS core/shell quantum dot nanocrystal. The electronic structure has been determined by solving of the Poisson–Schrödinger equations self-consistently. In calculations, the exchange-correlation effects between identical particles have been taken into account in the frame of the local density approximation. We have demonstrated that the optical properties of triexciton systems are remarkably different from the single and biexciton systems. Absorption peaks or transition energies of the triexciton system are well separated from those of single- and bi-exciton systems. We have observed that the core-radius dependent transition energy variations of triexcitons are higher when compared with single- and bi-excitonic systems. The transition energy shifts of double and triple excitons with respect to the single exciton have been calculated as a function of the core radius and we have shown that the energy shifts are inversely proportional with the radius. We have also investigated the radius-dependent changes in binding energies and lifetimes of the structures and the comparative results have been discussed in a detail manner.     

Correlated room temperature ferromagnetism and photoluminescence in Al-doped SnO2 nanoparticles

We investigated the single exciton and multiple exciton generation (MEG) behavior in Ag₇ and single Cu atom-doped Ag₇ quantum clusters using ab initio. MEG is observed for the first time in metal clusters. The results indicate that multiple excitons appear in the visible and near ultraviolet light ranges. Single excitations are main contribution for the optical spectra, while the multiple excitons merely contribute for some peaks at the higher energies. However, occurrence of MEG enhances the optical absorption in Ag₇ cluster. The optical spectrum of pure Ag₇ cluster obtained using the symmetry-adapted cluster theory with configuration interaction, and time-dependent density functional theory is in excellent agreement with experiment spectrum. As observed in both single Cu atom-doped Ag₇ clusters, redshifts and suppressions of the MEG-related absorption peaks are observed compared with pure Ag₇ cluster.     

Lasing behaviour from the condensation of polaronic excitons in a ZnO nanowire

Atoms under optical and magnetic trapping in a limited space at a very low temperature can lead to Bose-Einstein condensation (BEC),even in a one-dimensional (1D) optical lattice. However,can the confinment of dense excitons in a 1D semiconductor microstructure easily reach the excitonic BEC A lightly Mn(Ⅱ)-doped ZnO nanowire under a femtosecond laser pulse pump at room temperature produces single-mode lasing from coherent bipolaronic excitons,which is much like a macroscopic quantum state due to the condensation of the bipoaronic excitons if not real BEC. In this process,longitudinal biphonon binding with the exciton plays an important role. We revisit this system and propose possibility of bipolaronic exciton condensation. More studies are needed for this condensation phenomenon in 1D microcavity systems.