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Journal of the Optical Society of America B

Polarization dependence and selection rules of transient four-wave mixing in GaAs quantum-well excitons

Henry H. Yaffe, James P. Harbison, Leigh T. Florez, Yehiam Prior

Published Apr 1, 1993• 51 citations
Publisher

Abstract

We report the experimental results of two-pulse transient four-wave mixing near the first heavy-hole quantum-well exciton. Input pulses with similar polarizations (circular or linear) measure the exciton dephasing rate; opposite circular polarized pulses produce no four-wave mixing signal, while crossed linear polarized pulses generate a weaker signal with a faster dephasing rate. This signal is attributed to the biexcitonic transition, which was directly observed in a separate nondegenerate four-wave mixing experiment. The selection rules for these transitions are discussed and confirm the treatment of the excitonic transition as a three-level system.

DOI
10.1364/josab.10.000578

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We report the experimental results of two-pulse transient four-wave mixing near the first heavy-hole quantum-well exciton. Input pulses with similar polarizations (circular or linear) measure the exciton dephasing rate; opposite circular polarized pulses produce no four-wave mixing signal, while crossed linear polarized pulses generate a weaker signal with a faster dephasing rate. This signal is attributed to the biexcitonic transition, which was directly observed in a separate nondegenerate four-wave mixing experiment. The selection rules for these transitions are discussed and confirm the treatment of the excitonic transition as a three-level system.
We report time-resolved degenerate four-wave-mixing experiments on a high-quality single GaAs quantum well. The signals for parallel and cross-polarized exciting pulses show pronounced quantum beats with different frequencies corresponding to the heavy/light-hole splitting and the biexciton binding energy, respectively. Comparison of the experimental data with solutions of the optical Bloch equations for a phenomenological model system shows that these features result from strong contributions of the biexcitonic state. The importance of biexcitons to the nonlinear coherent response of the two-dimension exciton is further confirmed by the frequency dependence of the time-integrated four-wave-mixing signal amplitudes measured for the two polarization geometries.
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We investigate the spectral properties of the excitonic nonlinear response in a GaAs quantum-well sample containing wells of different thicknesses. We observe both the heavy-hole biexciton and the light-hole biexciton in the transient four-wave mixing spectrum and estimate their binding energy dependence on well width. For moderate excitation densities the signal for negative delay at the heavy-hole exciton and biexciton resonances is due to two-photon transitions to the biexciton states through the exciton states. The temporal behavior of the transient four-wave mixing signal from the heavy-hole exciton resonance is strongly dependent on the spectral position of the laser. We show that this effect is due to interference phenomena and to excitation-induced dephasing.
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.
We report measurements of the polarization and time-averaged intensity of four-wave mixing signals from GaAs quantum wells as functions of the pump beam polarizations, laser photon energy, and optical injection density, the latter covering a range of higher levels than has previously been reported. Excitation of heavy-hole excitons produced a sin2 variation of the signal intensity as the pump beam polarizations changed from parallel to perpendicular, while injection of light-hole excitons led to an approximately cos2 dependence. The tuning dependence of the heavy-hole-exciton signal revealed a low-energy signal which is attributed to biexcitons. The dominance of this signal for perpendicular polarization causes the observed sin2 variation of the heavy-hole-exciton signal.