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Soviet Physics Uspekhi

Excitonic molecules in semiconductors

V. D. Kulakovskiĭ, Valery G. Lysenko, Vladislav B. Timofeev

Published Sep 30, 1985• 34 citations
Publisher

Abstract

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.

DOI
10.1070/pu1985v028n09abeh003990

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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.
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.
Bose-Einstein condensation of excitons is a unique effect in which the electronic states of a solid can self-organize to acquire quantum phase coherence. The phenomenon is closely linked to Bose-Einstein condensation in other systems such as liquid helium and laser-cooled atomic gases. This is the first book to provide a comprehensive survey of this field, covering theoretical aspects as well as recent experimental work. After setting out the relevant basic physics of excitons, the authors discuss exciton-phonon interactions as well as the behaviour of biexcitons. They cover exciton phase transitions and give particular attention to nonlinear optical effects including the optical Stark effect and chaos in excitonic systems. The thermodynamics of equilibrium, quasi-equilibrium, and nonequilibrium systems are examined in detail. The authors interweave theoretical and experimental results throughout the book, and it will be of great interest to graduate students and researchers in semiconductor and superconductor physics, quantum optics, and atomic physics.
This dissertation addresses both fundamental aspects of the coherent exciton kinetics in single semiconductor quantum wells and more application-oriented aspects of the collective excitonic optical properties in quantum well Bragg structures. We use a bosonic theory to investigate the ultrafast coherent exciton dynamics after an optical excitation in a single semiconductor quantum well. It is shown that, on intermediate time scales, nonlinear mean-field interactions between excitons lead to a coherent, wave-like evolution in the momentum distribution of optically inactive excitons, which can survive for some time before dephasing sets in. Driven by two-exciton correlations, this coherent quantum kinetic effect bridges the well-known kinetics associated with optical excitation on the one hand and incoherent relaxation on the other. We also study more general dynamical properties of bosonic mean field systems with N-species of excitons (in a single semiconductor quantum well). We find that the momentum-conserving exciton mean field equations, including the coupling to external fields and fermionic corrections, have the dynamical structure su(N,N). We show that one can define a non-real generalized "Bloch vector" and a non-hermitian "density matrix" description, which allow us to explicitly obtain all the constants of motion associated with the su(N,N) symmetry. The many-body effects and correlations of excitons in a single quantum well are mainly induced by the Coulomb interactions. In the case of a semiconductor quantum well Bragg structure, the light induced coupling between different quantum wells also dramatically affects the excitons' behavior, especially through the collective excitations of excitons in the whole structure. We investigate the linear excitonic optical properties of the quantum well Bragg structure induced by the collective excitations using the transfer matrix approach. We show that the so called "intermediate band" (IB) created by the exciton resonance, which does not exist in conventional photonic crystals, can be used for the stopping, storing and releasing of light, which is important in information processing devices. We also discuss the compensation of the dispersive distortion in the light delay process through reversing the IB band structure. Other conceptual and practical issues such as the decay rate of the IB modes and the generalized anti-reflection coating are also investigated.
The influence of the radiative decay of excitonic molecules on a possible quasiequilibrium Bose–Einstein condensation (BEC) of excitonic molecule's is examined with respect to the radiative renormalization of the excitonic molecule energy (excitonic molecule Lamb shift). For the excitonic molecule wave function, a Schrödinger equation which contains polariton effects is derived and analyzed. Both the inverse excitonic molecule radiative lifetime γ m and the biexciton Lamb shift Δ m depend strongly on the total excitonic molecule momentum K. The energy renormalization Δ m (K) leads to the excitonic molecule effective mass modification and can result in a camel-back structure at K = 0, which opposes a BEC of excitonic molecules at K = 0. Introduction Observations of a quasiequilibrium Bose–Einstein condensation (BEC) of excitonic molecules (EM) have been attempted [1, 2, 3] following its theoretical prediction [4, 5] (for reviews see, e.g. [6, 7]). Recent approaches [8, 9] with high-precision techniques renewed the interest in this phenomenon. Traditionally, one tries to detect BEC of the EMs in luminescence. In the new approach the appearance of coherence in the thermal system of the EMs has been tested by means of four-wave mixing and treated as a fundamental manifestation of BEC. (See the paper by Hasuo et al . in this book.) Both optical methods for the BEC detection imply that the optical transition to the corresponding intermediate exciton (IE) state is dipole-active. In this case the EM state is unstable against optical decay with a “giant” oscillator strength [6].
Transient optical nonlinearities of semiconductor quantum dots in the strongly confined regime are studied, in which the exciton, biexciton and magnetic field effects are taken into account. The photo induced band-to-band electronic transitions are considered from both the heavy-hole (hh) and light-hole (lh) valence bands to the lowest (1s) exciton state below the fundamental absorption edge. The time dependent perturbation technique for a three-level system, under the near band gap resonant excitation regime, has been employed; with the incorporation of the relaxation and dephasing mechanisms phenomenologically. The induced polarization is calculated from where the real and imaginary parts of the third-order nonlinear optical susceptibility, responsible for the occurrence of nonlinear refraction and nonlinear absorption respectively, have been derived. The temporal and detuning spectra of nonlinear refraction and absorption; and their dependence on density of biexcitons and a moderately strong magnetic field, have been analyzed. It is observed that the nonlinear refraction and nonlinear absorption enhance with increasing magnetic field in small CdS quantum dots.