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Physical Review Letters

Towards Bose-Einstein Condensation of Semiconductor Excitons: The Biexciton Polarization Effect

D. Hägele, S. Pfalz, M. Oestreich

Published Sep 30, 2009• 4 citations
Publisher

Abstract

We theoretically predict a strong influence of stimulated exciton-exciton scattering on semiconductor luminescence. The stimulated scattering causes circularly polarized instead of unpolarized emission at the biexciton emission line in a degenerate gas of partly spin polarized excitons. The biexciton polarization effect increases with increasing exciton densities and decreasing temperatures and approaches almost unity in the ultimate case of Bose-Einstein condensation. Time- and polarization-resolved luminescence measurements evidence the biexciton polarization effect both in ZnSe and GaAs quantum wells.

DOI
10.1103/physrevlett.103.146402

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arXiv:0907.3612•Journal of Experimental and Theoretical Physics Letters•Sep 1, 2009•16 citations
We theoretically predict a strong influence of stimulated exciton-exciton scattering on semiconductor luminescence. The stimulated scattering causes circularly polarized instead of unpolarized emission at the biexciton emission line in a degenerate gas of partly spin polarized excitons. The biexciton polarization effect increases with increasing exciton densities and decreasing temperatures and approaches almost unity in the ultimate case of Bose-Einstein condensation. Time- and polarization-resolved luminescence measurements evidence the biexciton polarization effect both in ZnSe and GaAs quantum wells.
Introduction. Polaritons and Semiconductor Microcavities As we have mentioned previously, BEC of excitons or biexcitons and lasing can be seen as two limits of the same theory. Lasing occurs in the case of strong electron-photon coupling (recombination rate fast compared with interparticle-scattering rate) while excitonic BEC occurs in the case of weak electron-photon coupling (recombination rate slow compared with the interparticle-scattering rate.) A laser can be seen as a Bose condensate in which the long-range phase coherence exists in the photon states [1], while in the exciton condensate the coherence exists in the electronic states. This is one of the reasons for some of the confusing debates in the early history of excitonic Bose condensation – in many systems there is not a sharp distinction between an excitonic condensate and supperradiance, i.e., luminescence with enhanced intensity due to stimulated emission [2-4]. In the previous chapters, we have so far considered a laser light source only as a source of excitons by means of quantum transitions. In Chapter 6, the laser radiation was taken into account as a given external factor. This chapter is dedicated to phenomena related to a strong and noticeable exciton-photon interaction, when the light significantly influences the energy spectrum of the high-density excitons [5-9]. As we will see, this leads to many fascinating effects related to instabilities. A strong exciton-photon interaction implies a strong polariton effect, in which photon and exciton states are mixed (as in Fig. 1.3). When this mixing is strong, it is not obvious how to define the ground state of the system.
The case of excitons as candidates for Bose–Einstein condensation is discussed, and experimental results in CuCl and Cu 2 O are presented. In CuCl, spectral analysis of the luminescence from biexcitons as a function of their density reveals a gradual evolution from classical statistics towards a quantum degenerate regime. The appearance of a sharp emission line below a critical temperature and above a critical density is attributed to the presence of a laser-induced Bose–Einstein condensate of excitonic molecules. This interpretation is supported by pump-probe experiments which show that additional particles injected in the presence of a biexciton condensate are drawn into it. In Cu 2 O, free exciton luminescence spectral analysis of ortho- and paraexcitons reveals a gradual evolution from a classical to a Bose quantum degenerate regime with increasing particle densities. Orthoexciton densities close to the critical density for condensation are obtained at high incoherent excitation. Under similar pumping, paraexciton densities exceeding the critical value are inferred from luminescence intensity ratios. Anomalous transport properties of paraexcitons, such as ballistic propagation over macroscopic distances and formation of soliton-like excitonic packets are discussed as evidence for excitonic superfluidity. Introduction Excitons The lowest electronically excited state of a non-metallic crystal corresponds to the promotion of one electron from the top of the highest fully occupied valence band to the bottom of the next empty conduction band. A correct evaluation of the required energy must include the Coulomb correlation between the promoted electron and all other electrons left behind in the valence band.
The experiments on Bose-Einstein condensation (BEC) of dipolar (spatially-indirect) excitons in the lateral traps in GaAs/AlGaAs Schottky-diode heterostructures with double and single quantum wells are presented. The condensed part of dipolar excitons under detection in the far zone is placed in k -space in the range which is almost two orders of magnitude less than thermal exciton wave vector. BEC occurs spontaneously in a reservoir of thermalized excitons. Luminescence images of Bose-condensate of dipolar excitons exhibit along perimeter of circular trap axially symmetrical spatial structures of equidistant bright spots which strongly depend on excitation power and temperature. By means of two-beam interference experiments with the use of cw and pulsed photoexcitation it was found that the state of dipolar exciton Bose-condensate is spatially coherent and the whole patterned luminescence configuration in real space is described by a common wave function.
The phonon scattering assisted luminescence of semiconductor quantum well excitons after short pulse excitation is investigated. The presented analysis is based on the low-density limit of a set of equations for quantum correlation functions for electrons, phonons, and photons. The dynamics of the correlation functions describes the optical excitation and the decay of the coherent exciton polarization as well as the generation of an incoherent exciton occupation and its luminescence decay. Numerical solutions of the equations of motion demonstrate strong competition effects of the exciton-phonon and the exciton-photon interaction on a picosecond time scale and lead to a nonmonotonous temperature dependence of the time-resolved spontaneous emission. The angle resolved emission resembles the generation and decay dynamics of the exciton density for different in-plane momenta.
The influence of the radiative decay of excitonic molecules on a possible quasiequilibrium Bose–Einstein condensation (BEC) of excitonic molecule's is examined with respect to the radiative renormalization of the excitonic molecule energy (excitonic molecule Lamb shift). For the excitonic molecule wave function, a Schrödinger equation which contains polariton effects is derived and analyzed. Both the inverse excitonic molecule radiative lifetime γ m and the biexciton Lamb shift Δ m depend strongly on the total excitonic molecule momentum K. The energy renormalization Δ m (K) leads to the excitonic molecule effective mass modification and can result in a camel-back structure at K = 0, which opposes a BEC of excitonic molecules at K = 0. Introduction Observations of a quasiequilibrium Bose–Einstein condensation (BEC) of excitonic molecules (EM) have been attempted [1, 2, 3] following its theoretical prediction [4, 5] (for reviews see, e.g. [6, 7]). Recent approaches [8, 9] with high-precision techniques renewed the interest in this phenomenon. Traditionally, one tries to detect BEC of the EMs in luminescence. In the new approach the appearance of coherence in the thermal system of the EMs has been tested by means of four-wave mixing and treated as a fundamental manifestation of BEC. (See the paper by Hasuo et al . in this book.) Both optical methods for the BEC detection imply that the optical transition to the corresponding intermediate exciton (IE) state is dipole-active. In this case the EM state is unstable against optical decay with a “giant” oscillator strength [6].
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 τc ≲ 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.