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Physical review. B, Condensed matter

Biexciton-biexciton interaction in semiconductors

Hoang Ngoc Cam

Published Apr 15, 1997• 11 citations
Publisher

Abstract

For a semiconductor with single isotropic conduction and valence bands, the effective biexciton-biexciton interaction is derived starting from the second-quantization representation for the Hamiltonian of the system of interacting excitons and for the biexciton wave function within the framework of the adiabatic approximation. The interaction is found to be an average of the sum of effective interactions between excitons forming interacting biexcitons over the envelope functions of these biexcitons. Depending on the momentum transfer and on the difference between the momenta of interacting biexcitons, the interaction admits an analytical study when the first vanishes. In this case, the interaction has in the r space the form of a function of the interbiexciton distance consisting of a strong repulsive and a weak attractive part. At low temperatures the function describes main features in the behavior of the interaction among biexcitons, in which repulsion predominates over attraction. It is shown that while biexcitons remain stable quasiparticles they weakly attract each other for any value of the distance. A quantitative analysis of obtained results for the CuCl crystal shows that the biexciton system in this model substance is a weakly nonideal Bose gas with positive scattering length ${\mathrm{a}}_{\mathrm{s}}$\ensuremath{\simeq}${3\mathrm{a}}_{\mathrm{x}}$, which closely approaches the ideal one at excitation densities n\ensuremath{\leqslant}${10}^{18}$ ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}$.

DOI
10.1103/physrevb.55.10487

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For a semiconductor with single isotropic conduction and valence bands, the effective biexciton-biexciton interaction is derived starting from the second-quantization representation for the Hamiltonian of the system of interacting excitons and for the biexciton wave function within the framework of the adiabatic approximation. The interaction is found to be an average of the sum of effective interactions between excitons forming interacting biexcitons over the envelope functions of these biexcitons. Depending on the momentum transfer and on the difference between the momenta of interacting biexcitons, the interaction admits an analytical study when the first vanishes. In this case, the interaction has in the r space the form of a function of the interbiexciton distance consisting of a strong repulsive and a weak attractive part. At low temperatures the function describes main features in the behavior of the interaction among biexcitons, in which repulsion predominates over attraction. It is shown that while biexcitons remain stable quasiparticles they weakly attract each other for any value of the distance. A quantitative analysis of obtained results for the CuCl crystal shows that the biexciton system in this model substance is a weakly nonideal Bose gas with positive scattering length as{\mathrm{a}}_{\mathrm{s}}as​\ensuremath{\simeq}3ax{3\mathrm{a}}_{\mathrm{x}}3ax​, which closely approaches the ideal one at excitation densities n\ensuremath{\leqslant}1018{10}^{18}1018 cm\ensuremath−3{\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}cm\ensuremath−3.
Excitons are bound electron-hole pairs in semiconductors whose interactions influence optical properties and determine their collective behavior and emergent correlated phases. Despite the theoretical and experimental significance of these phenomena, a microscopic theory of exciton-exciton interactions that takes into account the full composite nature of these quasiparticles in systems with an arbitrary single-particle Hamiltonian is lacking. Here, we present a general theory of exciton-exciton interactions that builds upon our previous publication [Physical Review B 113, 155440 (2026)], which applied only to conventional semiconductors with weak band hybridization. By contrast, the theory presented here is valid in virtually any crystalline semiconducting system and can be applied to the study of biexciton formation and correlated excitonic phases in systems where band topology, quantum geometry, and moiré effects play a significant role. In addition to the analytical theory, we also present results in simple systems with flat bands with a nontrivial quantum metric and show that the biexcitonic spectrum differs strongly from that in the case without quantum geometry. Our theory paves the way for accurate quantitative calculations of biexciton spectra and excitonic many-body phases in modern condensed-matter systems.
Summary form only given. Large-radius excitons in semiconductors suffer strong Coulomb interaction on close approach. This is a distinctive difference in comparison with two-level systems in quantum optics. A mean field theory of interacting excitons in semiconductors leads to purely repulsive interaction, and does not account for spin-dependent polarization mixing and the formation of excitonic molecules (biexcitons). We have developed a theory for the nonlinear optical response, which can account for both. The coherent polarization is driven by exciton-exciton correlation, which can be expressed in terms of spin-dependent retarded memory functions. The effective equation is a generalized Gross-Pitaevskii equation.
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.
Great progress has been made in recent years in experimental studies of excitonic molecules, both in direct-band and indirect-band semiconductors. The exciton systems in these semiconductors differ substantially. In direct-band semiconductors with dipole-allowed optical transitions, the direct-recombination times are extremely small. Consequently the processes of binding of excitons into excitonic molecules and their decay occur under strongly nonequilibrium conditions. Hence one can obtain the fundamental information on biexcitons in these semiconductors by nonlinear optical methods. This review discusses the processes on which the various methods are based: two-photon resonance excitation of biexcitons, induced one-photon conversion of an exciton into a biexciton, two-photon resonance Raman scattering involving biexciton states, etc., and their application to studying biexcitons with the example of CdS. Problems of bistability involving biexcitons are also briefly discussed. In indirect semiconductors, where recombination occurs with the emission of a phonon, the lifetimes of excitons are large, and quasiequilibrium can be established in the exciton system. Under these conditions the information on the properties of the molecules is obtained by analyzing their radiative-decay spectra. The problem of detecting biexcitons in indirect semiconductors, radiative decay of molecules, and the effect on their stability of external electric, strain, and magnetic fields are discussed in detail with the examples of Si and Ge. Also the results of investigating the quantum statistical behavior of a dense gas of spin-oriented excitons (in a magnetic field under conditions in which the biexcitons are destabilized) are briefly presented (using the example of uniaxially compressed germanium), and the question of the possibility of their Bose condensation is discussed.
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.
The combined influence of biexcitons and the two-exciton scattering continuum is analyzed. The analysis is based on a density matrix description of a two-band semiconductor accounting for mean-field contributions, bound biexcitons and the correlated parts of the two-exciton scattering continuum on a common footing. Consistent with the microscopic formulation, the influence of biexcitons as well as that of the two-exciton continuum is represented by a correlation kernel which is obtained from an integral equation. For a one-dimensional model four-wave mixing signals are calculated solving numerically the resulting coupled nonlinear equations for excitation conditions in the vicinity of the 1s resonance. A strong compensation between the exciton–exciton continuum and the mean-field contribution is found for all excitation conditions studied. Surprisingly, biexcitonic signatures turn out to be enhanced when continua are included in the description.