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Physical review. B, Condensed matter

Biexcitonic contribution to the degenerate-four-wave-mixing signal from a GaAs/ Alx Ga1−x As quantum well

B. F. Feuerbacher, J. Kühl, Klaus Ploog

Published Jan 15, 1991• 116 citations
Publisher

Abstract

We report experiments on degenerate four-wave mixing in a high-quality GaAs/${\mathrm{Al}}_{0.3}$${\mathrm{Ga}}_{0.7}$As quantum well using the time-resolved self-diffraction technique. Frequency-dependent measurements around the heavy-hole exciton transition reveal a strong biexcitonic nonlinearity.

DOI
10.1103/physrevb.43.2439

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We report experiments on degenerate four-wave mixing in a high-quality GaAs/{\mathrm{Al}}_{0.3}$${\mathrm{Ga}}_{0.7}As quantum well using the time-resolved self-diffraction technique. Frequency-dependent measurements around the heavy-hole exciton transition reveal a strong biexcitonic nonlinearity.
We report measurements of two-photon transitions to the biexciton state and exciton-biexciton transitions (M band) in GaAs/Alx{\mathrm{Al}}_{\mathit{x}}Alx​${\mathrm{Ga}}_{1\mathrm{\ensuremath{-}}\mathit{x}}$As multiple quantum wells by spectrally resolving the self-diffraction in a four-wave-mixing experiment. Furthermore, nonlinear quantum beats between a coherently prepared population of excitons and biexcitons are observed. The analysis yields a binding energy of 1.8 meV for the biexciton in 116-A\r{} quantum wells.
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.
We present an experimental and theoretical study of the dephasing of heavy-hole excitons in a 70-\AA{} GaAs/Alx{\mathrm{Al}}_{\mathit{x}}Alx​${\mathrm{Ga}}_{1\mathrm{\ensuremath{-}}\mathit{x}}$As multiple-quantum-well stucture. We measure the time-integrated three-pulse four-wave-mixing signal of heavy-hole excitons in the quantum-well sample. We model the third-order nonlinear optical response incorporating the effects of a stochastic modulation of the transition frequency. We find that the dephasing of the nonlinear polarization is mainly the result of a spectral-migration process of the excitons and, to a lesser extent, due to a homogeneous dephasing process. The time dependence of the four-wave-mixing signal is very well described by theory if the spectral-migration process is assumed to be energy dependent.
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 investigate the properties of coherent exciton states in GaAs/Alx{\mathrm{Al}}_{\mathit{x}}Alx​${\mathrm{Ga}}_{1\mathrm{\ensuremath{-}}\mathit{x}}$As quantum wells using the four-wave-mixing technique with subpicosecond time resolution. In the first part of this work, we show that many-body interactions in a solid manifest themselves in a line shape of the four-wave-mixing signal that is substantially different from the predictions of the generally used simple two-level model. In particular, the coherent interaction of the quasiparticles leads to a signal at negative delay times, in agreement with recent theoretical predictions. In the second part, we report in detail about experiments where energetically close exciton transitions are excited coherently with a short laser pulse. The quantum or polarization interference leads to the observation of quantum beats in the decay of the diffracted signal. These results demonstrate that quantum-beat spectroscopy can be applied to study intrinsic excitations in solids.
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.