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Physical review. B, Condensed matter

Evidence for Bose-Einstein condensation of excitons in Cu2 O

David W. Snoke, James P. Wolfe, A. Mysyrowicz

Published Jun 1, 1990• 122 citations
Publisher

Abstract

Pulsed-laser excitation of naturally grown crystals of ${\mathrm{Cu}}_{2}$O produces a dense gas of excitons, which exhibits Bose-Einstein quantum statistics. Both orthoexcitons and paraexcitons, split by a 12-meV electron-hole exchange energy, are formed. At high excitation levels, the time-resolved luminescence of orthoexcitons yields a density-temperature relation that follows the phase boundary for Bose-Einstein condensation, n=${\mathit{CT}}^{3/2}$, but no striking evidence for a condensed fraction is observed. We have now measured the time-resolved spectrum of the lower-lying paraexcitons whose luminescence is 1500 times weaker than the orthoexciton luminescence. At intermediate power levels, the paraexciton distribution is more degenerate than the orthoexcitons. The relative intensities of the two species indicate that at high excitation levels the paraexciton density exceeds the critical density for condensation. At these high densities the paraexciton spectrum develops a structure that cannot be explained in terms of the thermalized Bose-Einstein distribution. Time-resolved spatial measurements of the luminescence indicate a rapid nondiffusive expansion of the gas at supersonic velocities that approach the expected ballistic velocities of the excitons. The rapid transport and the concurrent changes in the spectral distribution of paraexcitons may be the first observation of excitonic Bose-Einstein condensation and superfluidity.

DOI
10.1103/physrevb.41.11171

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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.

Nature Communications•Sep 14, 2022•38 citations
Pulsed-laser excitation of naturally grown crystals of Cu2{\mathrm{Cu}}_{2}Cu2​O produces a dense gas of excitons, which exhibits Bose-Einstein quantum statistics. Both orthoexcitons and paraexcitons, split by a 12-meV electron-hole exchange energy, are formed. At high excitation levels, the time-resolved luminescence of orthoexcitons yields a density-temperature relation that follows the phase boundary for Bose-Einstein condensation, n=CT3/2{\mathit{CT}}^{3/2}CT3/2, but no striking evidence for a condensed fraction is observed. We have now measured the time-resolved spectrum of the lower-lying paraexcitons whose luminescence is 1500 times weaker than the orthoexciton luminescence. At intermediate power levels, the paraexciton distribution is more degenerate than the orthoexcitons. The relative intensities of the two species indicate that at high excitation levels the paraexciton density exceeds the critical density for condensation. At these high densities the paraexciton spectrum develops a structure that cannot be explained in terms of the thermalized Bose-Einstein distribution. Time-resolved spatial measurements of the luminescence indicate a rapid nondiffusive expansion of the gas at supersonic velocities that approach the expected ballistic velocities of the excitons. The rapid transport and the concurrent changes in the spectral distribution of paraexcitons may be the first observation of excitonic Bose-Einstein condensation and superfluidity.
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.
Time-resolved spectral and spatial measurements of photoluminescence in Cu2{\mathrm{Cu}}_{2}Cu2​O at low temperatures suggest that the gas of paraexcitons undergoes Bose-Einstein condensation at high densities. As a result of the two-component nature of the gas (orthoexcitons and paraexcitons with different ground-state energies and spin multiplicities) and the nonequilibrium nature of photoproduced excitons, the condensation process is quite different from the simple ideal-gas case envisioned by Einstein.
Supercooled orthoexcitons are generated in Cu2O{\mathrm{Cu}}_{2}\mathrm{O}Cu2​O by resonant two-photon excitation with a femtosecond laser pulse. The excitonic Lyman series is systematically analyzed by time-resolved induced-absorption measurements. The decay time of orthoexcitons as well as the buildup and decay times of paraexcitons are found to be dependent on their respective densities. With these results, the two-body excitonic spin-exchange and the exciton dissociation processes are investigated. The collision-induced spin-exchange process is found to dominate in the early stage of photoexcitation. The conditions required to obtain a Bose-Einstein condensate with paraexcitons are discussed.
A comprehensive investigation of the optical properties of excitonic molecules in CuCl films is presented and discussed. The experimental work includes resonant two-photon absorption (TPA), observations of the resonantly excited biexciton emission, and optical pump-and-probe studies. The collision broadening of the TPA implies a collision rate \ensuremath{\sim}${10}^{\ensuremath{-}12}$ sec for the biexcitons, which is sufficiently rapid to establish a quasithermal equilibrium for the particles on a time scale that is short in comparison with the biexciton lifetime and the duration of the laser pump pulse. The biexciton luminescence line shapes obtained with resonant $\stackrel{\ensuremath{\rightarrow}}{\mathrm{k}}=0$ two-photon excitation have been fitted using a Bose-Einstein thermal distribution of biexcitons. The chemical potential obtained from the fits goes to zero as the biexciton density is increased at a fixed lattice temperature or if the lattice temperature is decreased at fixed density. The sharp luminescence features that are observed at high densities and low temperatures with single-beam, two-photon excitation are interpreted as resulting from a Bose-Einstein---condensed state of the biexcitons at twice the wave vector of the laser pumping photons. Further evidence for a condensed state is obtained from optical-probe measurements in which a small number of probe biexcitons is injected into the sample, with and without the presence of a condensed state produced by an intense laser pump beam. The luminescence of these injected probe biexcitons is modified in the presence of the pump beam such that it exhibits the sharp features of the emission from the condensed state. Measurements of optical gain and stimulated emission in the presence of the pump beam show that the redistribution of the probe luminescence does not result from those processes, but must involve a preferential redistribution of the probe particles in momentum space via collisions. Such a redistribution is expected when additional particles are added to a condensed system of bosons.
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.