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Oxford University Press eBooks

Experiments on excitons in bulk semiconductors

Makoto Kuwata‐Gonokami

Published Feb 28, 2013• 0 citations
Publisher

Abstract

Abstract This chapter begins with a discussion of excitonic matter in semiconductors. It then describes experimental methods for generating highly degenerate excitonic particles by using energy- and momentum-selective optical excitation processes for biexcitons in CuCl and orthoexcitons in Cu2O. Phase-sensitive interference of particles demonstrates the macroscopic coherence of such ensembles of cold particles prepared in the quantum degenerate regime. This is followed by a discussion of the search for spontaneous Bose–Einstein condensation of excitons in a bulk crystal of Cu2O.

DOI
10.1093/acprof:oso/9780199585915.003.0008

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•Sep 24, 2004•4 citations
Abstract This chapter begins with a discussion of excitonic matter in semiconductors. It then describes experimental methods for generating highly degenerate excitonic particles by using energy- and momentum-selective optical excitation processes for biexcitons in CuCl and orthoexcitons in Cu2O. Phase-sensitive interference of particles demonstrates the macroscopic coherence of such ensembles of cold particles prepared in the quantum degenerate regime. This is followed by a discussion of the search for spontaneous Bose–Einstein condensation of excitons in a bulk crystal of Cu2O.
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.
Abstract An unambiguous observation of the Bose-Einstein condensation (BEC) of excitons in a photoexcited bulk semiconductor and elucidation of its inherent nature have been longstanding problems in condensed matter physics. Here, we observe the quantum phase transition and a Bose-Einstein condensate appearing in a trapped gas of 1s paraexcitons in bulk Cu2O below 400 mK, by directly visualizing the exciton cloud in real space using mid-infrared induced absorption imaging that we realized in a dilution refrigerator. Our study shows that the paraexciton condensate is undetectable by conventional luminescence spectroscopy. We find an unconventionally small condensate fraction of 0.016 with the spatial profile of the condensate well described by mean-field theory. Our discovery of this new type of BEC in the purely matter-like exciton system interacting with a cold phonon bath could pave the way for the classification of its long-range order, and for essential understanding of quantum statistical mechanics of non-equilibrium open systems.
In a first part, a brief review of some excitonic properties is presented, with the accent put on their relevance with respect to the possibility of Bose-Einstein condensation. In a second part, recent experimental evidence is described, which supports the idea that excitonic particles may form a highly quantum fluid. In Cu20, the analysis of the exciton decay spectrum shows a gradual evolution of the gas from a classical regime at low densities up to a strongly degenerate one at high densities, with a chemical potential µ ~ 0. In CuCl excitons are unstable against formation of molecules (biexcitons). It is possible to generate directly a high density gas of biexcitons with momentum K ~ 0 by giant two-photon absorption. At low excitation, the observed molecular emission is in agreement with Maxwell -Boltzmann statistics. At high densities, strong deviations occur. In particular, the appearance of a sharp emission line is attributed to the presence of a Bose-Einstein condensate of excitonic molecules.
We present our recent experimental studies on anomalous luminescence and its connection to Bose–Einstein condensation (BEC) transition of dark excitons in a bulk semiconductor. Our sensitive and quantitative detection of this nonluminous quasi-particle using hydrogen-like internal transitions allows obtaining continuous spectra of dark excitons using a quantum cascade laser. According to quantitative measurements on the two-body inelastic collision cross section of excitons, the system needs to be cooled to sub-Kelvin temperatures. We discuss in detail our recent observation of an explosive phenomenon when the BEC criterion is satisfied (Yoshioka et al 2011 Nature Commun . 2 328) for trapped excitons using a helium-3 refrigerator, and outline a plausible scenario when the BEC transition occurs in an inelastic environment. We also discuss how to increase the condensate fraction in order to study the unique ground state of many-body electric excitations in solids.
Experimental observations are presented on Bose-Einstein condensation of excitons in Cu2O at low temperatures. These observations deal with traveling exciton packets in a high quality natural crystal. The properties of the exciton packets are examined using two different excitation depths of formation of the excitons (affecting the size of initial exciton cloud). The properties of the condensate include for example: the amplitude, the velocity of the exciton packet, the critical conditions for condensation and phase diagram. Interference effects of two coherent packets are also studied using these different initial excitation depths. Stimulated emission of particles into the exciton packet by injection of thermal excitons in the crystal volume is investigated in greater detail as well as the attenuation of the lateral laser beam (used to create the thermal excitons that trigger the amplification phenomenon).
There is a 40-year long history in the search for Bose-Einstein condensation (BEC) of excitons in semiconductors. This thesis presents research directed toward this goal in bulk crystal Cu2O in three dimensions and in GaAs-based coupled quantum wells (CQW) in two dimensions.The Auger recombination process in Cu2O plays a major role in limiting the density of the excitons. We find that the rate for this process increases with applied stress and lattice temperature. We create paraexcitons in Cu2O through a resonant two-photon excitation in a harmonic potential trap with the Auger recombination process as small as possible (at low temperature and low stress), and find that the exciton creation efficiency in the resonant two-photon excitation is greater for one-beam excitation than for two colliding pulses, but the colliding pulse method may be useful for direct creation of a condensate in the ground state. The paraexciton density in this work is about thirty times less than the required density for BEC of paraexcitons. One promising direction for BEC of excitons in Cu2O is that with higher laser power from stronger IR laser sources, or at lower temperature, the critical density can be approached under one-beam two-photon excitation resonant with the paraexciton state.In two dimensions, the CQW structure has been modified with four design strategies: highest possible barriers, introducing into the barriers a superlattice of 60 angstrom GaAs wells, p-i-n doping, and wider quantum wells, which provides indirect excitons low disorder and high mobility. With a cold near-resonant excitation, we conclude that the excitons act as a free gas, travelling distances of hundreds of microns. We also present observations of a narrow beam of emitted light, when the indirect excitons are confined in a two-dimensional harmonic potential trap, in a way quite similar to the first observations of BEC in alkali atoms. A beam-like emission has been suggested as a telltale for BEC of excitons. This opens the door to a whole range of investigations, including attempts to observe coherence of the emitted light, proof of superfludity of the excitons, and other fascinating effects.