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Physical review. B, Condensed matter

Quasibosonic exciton dynamics near the semiconductor band edge

Margaret Hawton, Delene J. Nelson

Published Feb 15, 1998• 30 citations
Publisher

Abstract

We develop a heirarchy of equations that describes the electrodynamics of the semiconductor band edge. An exciton basis that incorporates intrapair Coulomb interaction is used. The excitons are treated as quasibosons that satisfy commutation relations intermediate between bosonic and fermionic. Their nonlinear dynamics are a consequence of phase-space filling and an effective exciton-exciton interaction that depends only on their center-of-mass wave vectors and internal quantum numbers. The resulting expansion in powers of the optical field is analogous to Axt and Stahl's dynamically controlled truncation, but takes a simpler form. If damping is omitted or if all interband and intraband dephasing time constants are the same, we find a set of relationships among the interband and intraband correlation functions which in the free pair basis give the semiconductor Bloch equations.

DOI
10.1103/physrevb.57.4000

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We develop a heirarchy of equations that describes the electrodynamics of the semiconductor band edge. An exciton basis that incorporates intrapair Coulomb interaction is used. The excitons are treated as quasibosons that satisfy commutation relations intermediate between bosonic and fermionic. Their nonlinear dynamics are a consequence of phase-space filling and an effective exciton-exciton interaction that depends only on their center-of-mass wave vectors and internal quantum numbers. The resulting expansion in powers of the optical field is analogous to Axt and Stahl's dynamically controlled truncation, but takes a simpler form. If damping is omitted or if all interband and intraband dephasing time constants are the same, we find a set of relationships among the interband and intraband correlation functions which in the free pair basis give the semiconductor Bloch equations.
The electron-hole pair operator commutation relations for a semiconductor \nare explicitly derived showing that the pairs are quasi-bosons \nwith statistics intermediate between bosons and fermions. These pair \noperators are transformed into exciton operators, that incorporate the \nintra-pair Coulomb interaction, and it is found that the commutation \nrelations remain quasi-bosonic. The exciton dynamics written in terms \nof the exciton operators are derived in the Heisenberg picture and \ncompared with the traditionally used semiconductor Bloch equations.
A microscopic many-body theory for the optical and electronic properties of semiconductors is reviewed with an emphasis on the role of correlation effects. At the semiclassical level, the semiconductor Bloch equations include many-body effects via bandgap and field renormalization as well as correlation contributions representing two electron-hole pair amplitudes, excitonic populations, and coupled interband and intraband coherences. These Coulomb interaction induced carrier correlations lead to characteristic signatures in nonlinear semiconductor spectroscopy. At the fully quantum mechanical level the dominant light-matter correlations are described by coupled semiconductor Bloch and luminescence equations. Excitonic emission properties of quantum well and microcavity systems are discussed, including effects such as coherent signatures in the secondary emission and coherent control of the emitted light.
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.
Summary form only given. Effects of exciton-exciton correlations (e.g. bound biexciton, exciton-exciton scatterings) have been amply demonstrated in the /spl chi//sup (3)/ contributions to experiments measuring the interband polarization in semiconductor quantum wells. Increasing attention is currently being focussed on higher order excitonic correlation effects. One higher-order quantity is the incoherent exciton density (defined as total exciton density minus the interband polarization squared) which is created by excitons scattering each other out of the coherent component. Other than its role in the dephasing and relaxation of the system, the incoherent exciton density has not received much attention. In this contribution, we present results of our theoretical study on the behavior of this quantity and related correlation functions under conditions that inhibit relaxation. Our theory follows the general formulation of bosonic theories for excitons: the basic degrees of freedom are exact bosons, and the fermionic exchange effects are incorporated into the boson-boson and boson-photon effective Hamiltonians. We truncate the effective interaction at the two-boson level. No formal bosonization procedure is used: the matrix elements of our effective Hamiltonian are chosen in such a way that in the coherent /spl chi//sup (3)/ limit, our boson theory yields formally identical results as the standard fermionic dynamics controlled truncation formalism. Standard many-body techniques are used to derive equations of motion for densities, correlation functions, and measurable quantities such as the interband polarization.
A generalized Bloch-Maxwell formulation for laser-field-coupled semiconductors is derived from a two-band model which includes direct Coulomb interactions. The momentum-dependent, microscopic, electron-hole equations of motion in the time-dependent Hartree-Fock approximation and neglecting interband exchange interactions form the starting point for the formulation. A self-consistent set of coupled equations in four dynamical variables for the medium, together with the electric-field amplitude coupled through the Maxwell wave equation in a semiclassical approximation, are obtained to lowest order in the coherent Coulomb exchange interaction and the density-of-states distribution. Intrinsic optical bistability is predicted in a steady state due to a carrier density-dependent redshift of the band edge due explicitly to coherent Coulomb exchange. Integration of the dynamical equations for conditions which correspond to the ultrafast time regime exhibit intrinsic adiabatic inversion, adiabatic following, anomalous Rabi cycling, and unique, as well as fast, optical switching, all of which depend upon the coherent Coulomb exchange interaction.
Ultrafast nonlinear optical spectroscopy is used to study the coherent dynamics of optically excited electron-hole pairs in semiconductors. Coulomb interaction implies that the optical inter-band transitions are dominated, at least at low temperatures, by excitonic effects. They are further enhanced in quantum confined lower-dimensional systems, where exciton and biexciton effects dominate the spectra even at room temperature. The coherent dynamics of excitons are at modest densities well described by the optical Bloch equations and a number of the dynamical effects known from atomic and molecular systems are found and studied in the exciton-biexciton system of semiconductors. At densities where strong exciton interactions, or many-body effects, become dominant, the semiconductor Bloch equations present a more rigorous treatment of the phenomena. Ultrafast degenerate four-wave mixing is used as a tool to study the coherent exciton dynamics, and the importance of performing transform limited spectroscopy is demonstrated throughout.