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Physical review. B, Condensed matter

Coherent generation and interference of excitons and biexcitons in GaAs/ Alx Ga1−x As quantum wells

K.‐H. Pantke, D. Oberhauser, Vadim G. Lyssenko, J. M. Hvam, G. Weimann

Published Jan 15, 1993• 135 citations
Publisher

Abstract

We report measurements of two-photon transitions to the biexciton state and exciton-biexciton transitions (M band) in GaAs/${\mathrm{Al}}_{\mathit{x}}$${\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.

DOI
10.1103/physrevb.47.2413

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We report measurements of two-photon transitions to the biexciton state and exciton-biexciton transitions (M band) in GaAs/{\mathrm{Al}}_{\mathit{x}}$${\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 experiments on degenerate four-wave mixing in a high-quality GaAs/Al0.3{\mathrm{Al}}_{0.3}Al0.3​Ga0.7{\mathrm{Ga}}_{0.7}Ga0.7​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 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 study the induced absorption due to biexciton formation in absorption bleaching pump-probe signals and the quantum beats between exciton and biexciton in the four-wave-mixing signals. The origin is confirmed by the polarization dependence of the signals in both experiments. The definite discrimination between exciton-biexciton quantum beats and the others by the polarization choices is demonstrated clearly. We also show the well-width dependence of the biexciton binding energy that is determined by the period of the quantum beats in the range of well width 45--150 \AA{} of GaAs/Alx{\mathrm{Al}}_{\mathrm{x}}Alx​${\mathrm{Ga}}_{1\mathrm{\ensuremath{-}}\mathrm{x}}$As (x=0.3--1.0) multiple quantum wells.
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 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 a model for the nonlinear optical response of quantum wells, which includes biexcitons. We show that within this model, the interaction of two laser pulses, mediated by the nonlinear susceptibility, results in oscillations and in coupling between ${\mathrm{\ensuremath{\sigma}}}^{+}$ and ${\mathrm{\ensuremath{\sigma}}}^{\mathrm{\ensuremath{-}}}$ excitons. This explains the temporal behavior of the differential absorption and four-wave mixing in recent experiments [Phys. Rev. Lett. 68, 349 (1992); 68, 1880 (1992)]. The oscillations have a frequency equal to the biexciton binding energy, and are different from known interference and quantum beat phenomena.