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Physica Scripta

Linear response theory for a highly excited exciton-electron-hole-pair system in direct gap semiconductors in the athermal stage of evolution

E. Heiner

Published Jun 1, 1992• 1 citation
Publisher

Abstract

The evolution of a highly excited exciton-electron-hole-pair system in the athermal stage is examined in a first principle theory by use of a time-dependent projection operator technique. The expectation values of excitons and electrons are cast out under the assumption of a Gaussian pulse shape in a theory, suitable for the description of transient properties. The linear response with respect to a white probe pulse is investigated by a Green's function technique, being an extension of the Kubo formalism for reference systems far off equilibrium. This formalism results in a correct description of the time-dependent behavior of effects like blue-shift and bleaching of exciton levels.

DOI
10.1088/0031-8949/45/6/016

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The evolution of a highly excited exciton-electron-hole-pair system in the athermal stage is examined in a first principle theory by use of a time-dependent projection operator technique. The expectation values of excitons and electrons are cast out under the assumption of a Gaussian pulse shape in a theory, suitable for the description of transient properties. The linear response with respect to a white probe pulse is investigated by a Green's function technique, being an extension of the Kubo formalism for reference systems far off equilibrium. This formalism results in a correct description of the time-dependent behavior of effects like blue-shift and bleaching of exciton levels.
Evolution equations of a laser-excited direct gap two-band semiconductor in the transient stage have been derived by using the first principle Liouville-von Neumann equation and the statistical projection operator method. To be more general, the photon field is described in a quantum mechanical manner. Quantum effects of the electron-photon coupoling as well as charge carrier Coulomb screening and dissipation are involved. The evolution of the time dependent coherent photon state is investigated. It results in additionally evolution equations. Numerical solutions of these systems are cast out for realistic parameters and are compared with previous results.
The paper presents a description of two-pair correlations in an electron-hole system in laser-excited direct-gap semiconductors in terms of the exciton-boson formalism. The dependence of the states of quasi-particles on their angular momentum orientation is properly taken into account following group theory rules. It is shown for the example of heavy hole excitons in GaAs quantum wells that Coulomb two-exciton correlations include effective repulsion between excitons with nonzero total momenta and effective attraction between excitons with zero total momenta. They generate exciton and biexciton nonlinearities, respectively, in the exciton-biexciton system. The Heisenberg equations of motion derived are applied to four-wave mixing in the coherent mode. Two components of Coulomb two-exciton correlations were found to generate coherent four-wave mixing either separately, one at the cocircular and the other at the perpendicular-linear polarization of applied pulses, or jointly at parallel-linear polarization. General equations are obtained for the amplitude of four-wave mixing signals with time resolution in these polarization configurations, which, in the limit of ultranarrow pulses, reduce to analytic functions of time and excitation and sample parameters. These equations are used to analyze signal characteristics in every polarization configuration. The results give a correct picture of biexciton effects and the polarization dependence of coherent four-wave mixing in GaAs quantum wells.
The semiconductor Bloch equations are solved numerically for a two-pulse photon-echo configuration. The time-dependent diffracted signal is computed and the significance of many-body effects, carrier relaxation, and dephasing is investigated in detail. Assuming femtosecond-pulse excitation at various intensities and frequencies, distinctly different results are obtained if the exciton or the continuum electron-hole-pair states are excited. It is shown that pure exciton excitation produces a free-induction decay signal and no photon echo. An echo signal is obtained only if continuum states are excited either directly by choosing the central pulse frequencies appropriately or if the band-gap renormalization is sufficiently strong to shift continuum states into resonance. A continuous transition between free-induction decay and photon-echo signal is obtained with increasing excitation amplitude. A perturbative analytical analysis of the equations allows one to identify the role of the many-body effects in producing the different features.
The coherent response of a semiconductor three-state system to one or two intense light pulses is investigated experimentally on a 100 fs time scale. Three experiments constitute this dissertation: observation of excitonic Rabi oscillations, measurement of two-exciton coupled Stark shifting, and an attempt to observe dark states. Basic concepts of time-resolved ultrafast semiconductor spectroscopy are explained, followed by an analysis of semiconductor two- and three-state systems. Pure two- and three-state dynamics are derived from first principles, followed by the development of the appropriate semiconductor Bloch equations (SBE). Two-color pump-probe, two-color pump-pump, and pump-pump-probe techniques are explained in the context of three-state semiconductor experiments. The experimental setup is explained in detail. Resonant two-color pump-probe measurements resulted in the first observation of multiple excitonic Rabi oscillations. The common conduction band shared by the light-hole and heavy-hole excitons of an InGaAs multiple quantum well allowed us to measure hh-exciton density (Rabi) oscillations by probing lh-exciton absorption. By studying the intensity dependence of the Rabi frequency, we showed the important role of many-body effects in renormalizing the dipole energy. The shared conduction band also causes the lh-exciton resonance to Stark shift when the hh exciton is Stark shifted. We measured a transient Stark shifting of both resonances due to virtual hh-exciton transitions. We observed that the ratio of the hh-exciton shift to lh-exciton shift was 2:1 at large pump-exciton detuning, as predicted from a simple three-state dressed exciton picture. For smaller detunings we saw an increase in the ratio and a redshift of the non-dipole coupled exciton state. Both of these observations are consistent with the most recent theories and experiments on excitonic Stark shifting. For strong near-resonant pumping of both lh- and hh-exciton transitions, an intervalence-band Raman-type coherence follows from the SBE that results in a transparent eigenstate (dark state) when both pumps are equally detuned from resonance. The existence of this coherence is well-known in atomic-optical systems, but has been elusive in semiconductors. Our inconclusive experimental result is presented along with an evaluation of experimental shortcomings. In brief, the expected change is absorption was too small to see.
The optical spectra of laser-excited semiconductors change with varying laser intensity. Close to exciton or biexciton resonances these optical nonlinearities are, e.g., large enough to obtain optical bistability. The cause for these large nonlinearities are many-body effects in the system of the electron-hole pair excitation. The use of nonequilibrium Green’s functions, or if a quasi-equilibrium exists of thermal Green’s functions, makes it possible to take radiative and Coulomb interactions consistently into account.