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Physical review. B, Condensed matter

Differential measurements of Raman coherence and two-exciton correlations in quantum wells

Scot A. Hawkins, Eric J. Gansen, Martin J. Stevens, Arthur L. Smirl, I. Rumyantsev, Ryu Takayama, N. H. Kwong, Rolf H. Binder, Duncan G. Steel

Published Jul 14, 2003• 21 citations
Publisher

Abstract

Quantum beats involving the light-hole and heavy-hole excitons in GaAs quantum wells are studied using both conventional and novel temporally gated differential detection techniques. The contributions of the exciton-exciton correlations are separated from those of the intervalence-band Raman coherence and the interband (population) coherence by monitoring the signal in the probe direction and by taking advantage of the polarization selection rules for the excitonic transitions. The results are shown to be in agreement with a theoretical analysis based on the dynamics-controlled truncation formalism.

DOI
10.1103/physrevb.68.035313

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Quantum beats involving the light-hole and heavy-hole excitons in GaAs quantum wells are studied using both conventional and novel temporally gated differential detection techniques. The contributions of the exciton-exciton correlations are separated from those of the intervalence-band Raman coherence and the interband (population) coherence by monitoring the signal in the probe direction and by taking advantage of the polarization selection rules for the excitonic transitions. The results are shown to be in agreement with a theoretical analysis based on the dynamics-controlled truncation formalism.
Time-integrated differential detection techniques are used to study quantum beats involving the light-hole and heavy-hole excitons in an optically thin InGaAs multiple quantum well. The contributions of the exciton-exciton correlations are separated from those of the intervalence-band Raman coherence and the interband (population) coherence by monitoring the signal in the probe direction and by taking advantage of the polarization selection rules for the excitonic transitions. Quantum beats are observed for pump and probe pulses with the same circular polarization, providing evidence for two-exciton correlations. A theoretical analysis based on the dynamics-controlled truncation formalism suggests that the beats for the same linear polarization arise from Raman, population, and two-exciton contributions.
A theoretical analysis of intervalence-band coherences is presented. These optically created non-radiative coherences are generalizations of non-radiative coherences in atomic and molecular three-level systems. Whereas in three-level systems these coherences are the basis of important and well-established nonlinear effects, the interpretation of experimental evidence for such coherences in semiconductors needs to be supported by many-body theory. Based on the dynamics-controlled truncation formalism, the respective contributions of intervalence-band coherences and coherent biexcitonic correlations in time-integrated differential transmission spectroscopy is investigated. It is found that the contribution of the biexcitonic correlations to the observable heavy-hole–light-hole beats can be eliminated, either by reducing the light pulse duration or by choosing the central frequency of the light pulses at the heavy-hole exciton.
We demonstrate the presence of strong exciton-exciton correlations in GaAs-AlGaAs multiple quantum wells by using the polarization selection rules for four-wave mixing and a test that was originally designed to distinguish between quantum beats and polarization interference. We show that, when the four-wave-mixing signal is produced by two pulses that have the same circular polarization, dynamic beating behavior is observed at the heavy-hole-light-hole frequency that provides evidence of Coulomb-induced correlations that go beyond those expected from the semiconductor Bloch equations in the Hartree-Fock approximation and beyond the local field corrections used in simple phenomenological models. Moreover, this behavior cannot be explained by invoking biexcitonic effects. We demonstrate that this dynamic excitonic coupling can be explained in terms of a competition between quantum-beat-like and polarization-interference-like behavior, and we show that such behavior can be used to place quantitative limits on the coupling strength. In addition, we use a simple phenomenological model to show that excitation-induced-dephasing can produce such correlations.