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International Conference on Ultrafast Phenomena

Stimulated Photon Echoes and Free Polarization Decay in GaAs Multiple Quantum Well Structures: Evidence for Localized and Delocalized Excitons

M. D. Webb, Steven T. Cundiff, Duncan G. Steel

Published Jan 1, 1990• 0 citations
Publisher

Abstract

Recent experimental and theoretical work suggests that excitons in GaAs/AlGaAs multiple quantum wells may be localized by disorder, or delocalized with Bloch-type wavefunctions1. At low temperature, localized excitons are expected to be characterized by spectral diffusion and by long optical coherence times, while delocalized excitons have short coherence times and exhibit spatial mobility2. The short optical coherence time associated with delocalized excitons results in a linear absorption profile that is primarily homogeneously broadened, while the disorder associated with localized excitons leads to an inhomogeneously broadened profile. In this work, we investigate the energy and phase relaxation of HH1 excitons in GaAs/AlGaAs MQW's at low temperature, and provide evidence that, dependent on the exciton density, both localized and delocalized excitons contribute to the nonlinear optical response.

DOI
10.1364/up.1990.me4

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This work presents new results of experimental studies of exciton relaxation in GaAs/AlGaAs multiple quantum well materials, using transient nonlinear laser spectroscopy techniques. In the low excitation regime, effective optical Bloch equations similar to the density matrix formalism of a two-level system describe the response. Solutions of these equations appropriate for three-pulse scattering studies are presented, along with a discussion of new experimental techniques used in this work. Non-ideal conditions present in the molecular beam epitaxy growth process introduce monolayer fluctuations in the quantum well thickness, leading to inhomogeneous broadening and exciton localization at sites of minimum energy. Localized excitons are separated in energy from extended, quasi-delocalized states by the mobility edge. Studies of localized exciton relaxation indicate that these excitons relax on a much slower timescale than delocalized excitons. The temperature dependence of the localized exciton relaxation rate shows that above 15K, the excitons are thermally activated to extended states above the mobility edge. Below 15K the excitons relax by phonon assisted migration between localization sites. For temperatures above 5K, and for exciton energies greater than 1 meV below line center, an extra dephasing mechanism characterizes the exciton relaxation. The inhomogeneous broadening of the exciton leads to the emission of stimulated photon echoes in the experimental geometry used in this work. The time-resolved emission demonstrates the stimulated photon echo nature at low excitation densities. At higher excitation densities, the decay dynamics is more complex. The time-resolved emission shows the presence of a stimulated photon echo and a free polarization decay. This unusual result suggests that both a homogeneous and an inhomogeneous exciton distribution comprise the exciton resonance. Exciton relaxation at low excitation densities represents the interaction of the exciton with the lattice. At higher excitation densities, exciton-exciton and exciton-free carrier interactions modify the relaxation rates. The dependence of the exciton relaxation rate on excitation density shows that many-body effects play an important role in the exciton physics. Free carrier interactions are more efficient at increasing the exciton relaxation rate; both types of interactions are more important in quantum well systems than in bulk materials.
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Photon echo spectroscopy provides an important tool for studying excitonic relaxation in disor- dered GaAs/AlGaAs quantum wells. In this paper, we review the application of this methodology to the study of excitons localized due to interface fluctuations, which result in inhomogeneous broadening of the spectrum and relaxation due to migration among localization sites. The temperature and energy dependence of the relax- ation rates indicate complex scattering mechanisms. The dependence of the photon echo signal on polarization of the incident pulses shows a dramatic change in the broadening and dephasing characteristics. This response is interpreted in terms of polarization selection of localized versus delocalized excitons. Mechanisms for the polarization dependence are discussed in terms of coupling between opposite spin excitons.
We have studied picosecond two-pulse degenerate four-wave mixing in GaAs/AlAs quantum wells under different polarization configurations of the two pump beams and the analyzed optical polarization. We observe two components, a prompt free polarization decay (FPD) and a delayed photon echo (PE), which show different polarization rules and dephasing times. The observed polarization rules are consistently explained in a theoretical model. Within this model, the two-component behavior is a direct consequence of short-range disorder. The PE dephasing rate is associated with the homogeneous broadening of the excitons while the FPD corresponds to the total dephasing rate, consisting of the homogeneous and inhomogeneous (short-range and long-range) broadenings.