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Journal of Physics Condensed Matter

Quantum saturation of ortho-excitons near Bose-Einstein condensation

Y C Lee, Wuming Zhu

Published Dec 21, 1999• 5 citations
Publisher

Abstract

The quantum saturation of ortho-excitons relative to the Bose-Einstein condensation of para-excitons is explained in terms of indefiniteness of N ortho in contrast to the conserved N para as the exciting laser pulse declines in intensity.
DOI
10.1088/0953-8984/12/4/102

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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.
This note discusses the question as to whether quasi-particles, such as excitons, i.e., nonlocalized excited states of solids, can fulfill necessary conditions for a Bose-Einstein condensation, and whether such condensation can be observed. Although uncertainties of present data on excitons preclude precise numerical predictions, it is concluded that under certain experimentally attainable circumstances excitons fulfill the necessary conditions, i.e., condensation is possible. Ways of detecting the condensation are considered, and a specific experiment is proposed.
Photo-excited excitons, i.e. closely bound electron-hole pairs, are in the low-density regime approximately bosons. For sufficiently low temperatures and sufficiently high densities of the exciton gas, a nonequilibrium phase transition in the form of a Bose-Einstein condensation (BEC) can be expected. Various levels of the description of the kinetics of relaxation and condensation due to the coupling of the excitons to a cold reservoir of acoustic phonons are discussed. For noninteracting excitons a rate equation approach with the exciton Boltzmann equation can be used. For interacting excitons the nonmarkovian quantum kinetics is required for the description of the BEC in order to incorporate the changes of the energy spectrum during the condensation self-consistently. Finally colored Langevin fluctuations can be used to calculate the phase diffusion of the condensate.
Abstract The quasiequilibrium state of the two‐component non‐linear ortho‐para‐exciton gas is investigated. The concentration shifts of the exciton levels are taken into account at high densities of quasiparticles. Three exciton phases appear at any value of the chemical potential, due to the effect of optical bistability: the para‐phase, the ortho‐phase and the mixed ortho‐para‐phase. It is pointed out that Bose‐Einstein condensation (BEC) in the para‐ and ortho‐phase is possible, in spite of the fact that the initial level of ortho‐excitons is situated higher on the energetic scale than the initial level of para‐excitons.