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Journal of Experimental and Theoretical Physics

Exciton and biexciton nonlinearities in coherent four-wave mixing in semiconductor quantum wells

Hoang Ngoc Cam

Published Feb 1, 2006• 1 citation
Publisher

Abstract

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.

DOI
10.1134/s1063776106020099

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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.
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 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 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.
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.
By use of an optical coherent-control technique we demonstrate and analyze the control of transitions involved in the generation of four-wave-mixing signals in a semiconductor quantum well for the two different four-wave-mixing directions and for different sequences of the excitation pulses. Results are presented for frequency- as well as for time-resolved signals. A doubling of the coherent switching frequency is found which occurs if the laser pulses performing the control process contribute quadratically to the wave-mixing signal. A direct comparison between experiment and microscopic theory reveals how the coherent-control process acts on the coherent polarization of the exciton-biexciton system in all different configurations. An additional interpretation of the experimental results based on a simplified few-level model is able to provide an intuitive understanding of the relevant processes which govern the coherent control of the excitonic and biexcitonic wave-mixing polarizations.
Summary form only given. Here, we use the polarization selection rules for four-wave mixing (FWM) and a test that was originally designed to distinguish between quantum beats and polarization interference to demonstrate the presence of strong exciton-exciton correlations in GaAs-AlGaAs multiple quantum wells. We show that when the four-wave-mixing signal is produced by two pulses having the same circular polarizations that quantum-beat-like behavior is observed. The latter observation is contrary to the predictions based on either the density matrix equations for two independent three-level systems (without many body effects) or the conventional semiconductor Bloch equations (SBE), both of which predict that polarization interference, but not quantum beats, should be observed. Consequently, these observations provide clear evidence for exciton-exciton correlations and evidence that those correlations go beyond those contained in the SBE. The procedure described here provides a simple effective test for such processes. Finally, we show that the quantum-beating-like behavior can be reproduced by including a density-dependent dephasing term (so-called excitation-induced dephasing, or EID) in the density matrix equations.