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Physical review. B, Condensed matter

Theory of the decay luminescence spectrum of a Bose-condensed interacting exciton gas

H. Shi, G. Verechaka, Adam Griffin

Published Jul 1, 1994• 38 citations
Publisher

Abstract

Recent experimental studies by Wolfe, Snoke, and Lin have given strong evidence that paraexcitons in optically excited ${\mathrm{Cu}}_{2}$O crystals form a Bose condensate. In these studies, the observed recombination decay luminescence line shape I(\ensuremath{\omega}) has been analyzed in terms of an ideal Bose-condensed gas. We derive a general expression for I(\ensuremath{\omega}) in terms of the exact single-particle spectral density A(k,\ensuremath{\omega}) of a Bose fluid. This expression is then used to calculate I(\ensuremath{\omega}) for a dilute, weakly interacting Bose gas. Our analytic results, based on the approximate theory due to Popov, are valid in the region just below the Bose-Einstein transition temperature. When formally extended down to T=0, they reproduce the well-known Bogoliubov approximation.

DOI
10.1103/physrevb.50.1119

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In Chapter 3, we have shown how a Bose condensate leads to the single-particle Green's function G αβ ( Q , ω) appearing as a distinct component of the the dynamic structure factor S ( Q , ω). This feature is a direct consequence of (3.13) and is explicitly shown by the expression for S ( Q , ω) in (3.18). In the present chapter, we review the many-body diagrammatic analysis which specifies the precise relation between G αβ ( Q , ω) and S ( Q , ω) in a Bose-condensed fluid ( n 0 ≠ 0). The power of this “dielectric formalism” lies in showing that both functions mirror each other, as a result of the condensate-induced intermixing of single-particle and density excitations. At the same time, the formalism emphasizes the continuity of these excitations as the fluid passes through T λ, although these excitations have very temperature-dependent weights in G αβ ( Q , ω) and S ( Q , ω). While it is the poles of the single-particle Green's function which describe the elementary excitations, experimentally it is difficult to probe directly this field-fluctuation spectrum. In particular, it is only in a Bose-condensed fluid that one can obtain information about G αβ ( Q , ω) from inelastic neutron-scattering data on S ( Q , ω). In the absence of a condensate, there is little relation between the density-fluctuation modes and the single-particle excitations in a Bose fluid. After setting up the dielectric formalism in Section 5.1, the next two sections consider some model approximations at finite temperatures. These models are most appropriate to a dilute weakly interacting Bose gas (WIDBG), but we believe they also give crucial insight into various aspects of superfluid 4 He.

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Evidence for Bose-Einstein condensation of a two-component exciton gas

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

Time-resolved spectral and spatial measurements of photoluminescence in ${\mathrm{Cu}}_{2}$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.

Physical Review Letters•May 21, 1990•110 citations
Recent experimental studies by Wolfe, Snoke, and Lin have given strong evidence that paraexcitons in optically excited Cu2{\mathrm{Cu}}_{2}Cu2​O crystals form a Bose condensate. In these studies, the observed recombination decay luminescence line shape I(\ensuremath{\omega}) has been analyzed in terms of an ideal Bose-condensed gas. We derive a general expression for I(\ensuremath{\omega}) in terms of the exact single-particle spectral density A(k,\ensuremath{\omega}) of a Bose fluid. This expression is then used to calculate I(\ensuremath{\omega}) for a dilute, weakly interacting Bose gas. Our analytic results, based on the approximate theory due to Popov, are valid in the region just below the Bose-Einstein transition temperature. When formally extended down to T=0, they reproduce the well-known Bogoliubov approximation.
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.
We calculate the spatially resolved optical emission spectrum of a weakly interacting Bose gas of excitons confined in a three dimensional potential trap due to interband transitions involving weak direct and phonon mediated exciton-photon interactions. Applying the local-density approximation, we show that for a noncondensed system the spatiospectral lineshape of the direct process reflects directly the shape of the potential. The existence of a Bose-Einstein condensate changes the spectrum in a characteristic way so that it directly reflects the constant chemical potential of the excitons and the renormalization of the quasiparticle excitation spectrum. Typical examples are given for parameters of the lowest yellow excitons in Cu2O{\text{Cu}}_{2}\text{O}Cu2​O.
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 system under consideration is a multicomponent gas of interacting paraexcitons and orthoexcitons confined in a three-dimensional potential trap. We calculate the spatially resolved optical emission spectrum due to interband transitions involving weak direct and phonon-mediated exciton-photon interactions. For each component, the occurrence of a Bose-Einstein condensate changes the spectrum in a characteristic way so that it directly reflects the constant chemical potential of the excitons and the renormalization of the quasiparticle excitation spectrum. Moreover, the interaction between the components leads, in dependence on temperature and particle number, to modifications of the spectra indicating phase separation of the subsystems. Typical examples of density profiles and luminescence spectra of ground-state paraexcitons and orthoexcitons in Cu2O{\text{Cu}}_{2}\text{O}Cu2​O are given.
In Chapter 3, we have shown how a Bose condensate leads to the single-particle Green's function G αβ ( Q , ω) appearing as a distinct component of the the dynamic structure factor S ( Q , ω). This feature is a direct consequence of (3.13) and is explicitly shown by the expression for S ( Q , ω) in (3.18). In the present chapter, we review the many-body diagrammatic analysis which specifies the precise relation between G αβ ( Q , ω) and S ( Q , ω) in a Bose-condensed fluid ( n 0 ≠ 0). The power of this “dielectric formalism” lies in showing that both functions mirror each other, as a result of the condensate-induced intermixing of single-particle and density excitations. At the same time, the formalism emphasizes the continuity of these excitations as the fluid passes through T λ, although these excitations have very temperature-dependent weights in G αβ ( Q , ω) and S ( Q , ω). While it is the poles of the single-particle Green's function which describe the elementary excitations, experimentally it is difficult to probe directly this field-fluctuation spectrum. In particular, it is only in a Bose-condensed fluid that one can obtain information about G αβ ( Q , ω) from inelastic neutron-scattering data on S ( Q , ω). In the absence of a condensate, there is little relation between the density-fluctuation modes and the single-particle excitations in a Bose fluid. After setting up the dielectric formalism in Section 5.1, the next two sections consider some model approximations at finite temperatures. These models are most appropriate to a dilute weakly interacting Bose gas (WIDBG), but we believe they also give crucial insight into various aspects of superfluid 4 He.
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.