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Physical review. B, Condensed matter

Mixed biexcitons in single quantum wells

Hans-Peter Wagner, W. Langbein, J. M. Hvam

Published Feb 15, 1999• 50 citations
Publisher

Abstract

Biexcitonic complexes in a ZnSe single quantum well are investigated by spectrally resolved four-wave mixing (FWM). The formation of heavy-heavy-hole ${\mathrm{XX}}_{h}$ and of mixed heavy-light-hole ${\mathrm{XX}}_{m}$ biexcitons showing binding energies of ${\ensuremath{\Delta}}_{h}=4.8\mathrm{meV}$ and ${\ensuremath{\Delta}}_{m}=2.8\mathrm{meV}$ is identified by polarization selection rules. The coherent dynamics of the FWM response and the observed FWM intensity ratio between the ${\mathrm{XX}}_{h}$ and ${\mathrm{XX}}_{m}$ biexciton-induced nonlinear signals are in agreement with the solution of an extended optical Bloch equation.

DOI
10.1103/physrevb.59.4584

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Biexcitonic complexes in a ZnSe single quantum well are investigated by spectrally resolved four-wave mixing (FWM). The formation of heavy-heavy-hole XXh{\mathrm{XX}}_{h}XXh​ and of mixed heavy-light-hole XXm{\mathrm{XX}}_{m}XXm​ biexcitons showing binding energies of \ensuremathΔh=4.8meV{\ensuremath{\Delta}}_{h}=4.8\mathrm{meV}\ensuremathΔh​=4.8meV and \ensuremathΔm=2.8meV{\ensuremath{\Delta}}_{m}=2.8\mathrm{meV}\ensuremathΔm​=2.8meV is identified by polarization selection rules. The coherent dynamics of the FWM response and the observed FWM intensity ratio between the XXh{\mathrm{XX}}_{h}XXh​ and XXm{\mathrm{XX}}_{m}XXm​ biexciton-induced nonlinear signals are in agreement with the solution of an extended optical Bloch equation.
The contribution of bound excitons and biexcitons to degenerate four-wave mixing signals is investigated in high-quality biaxially strained ZnSe layers. For the former complexes signatures of polarization interference with free excitons are found in time-resolved four-wave mixing, whereas spectrally resolved data point to the occurrence of quantum beating. Thus this system behaves as a mixture of independent two-level systems on the one hand and three-level systems on the other. Biexcitons contribute to the signal mainly at negative delay between the exciting pulses and are identified by means of spectrally resolved measurements and by use of different configurations of the pulse polarization. Complete agreement is found between the selection rules for biexcitons (and excitons) and the experimental data.
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.
The coherent control of excitonic and biexcitonic polarization in pulse-transmission and four-wave-mixing (FWM) experiments is analysed with real time resolution. As a model system a ZnSe single quantum well is exclusively excited at the heavy-hole exciton and exciton–biexciton resonance. In pulse-transmission experiments the coherent control of excitonic polarization is shown for low excitation intensities. At elevated excitation intensities the dephasing time of the polarization is found to be strongly dependent on the relative phase of two phase-locked laser pulses which perform the coherent manipulation of the polarization. In FWM experiments the separate coherent control of the excitonic and biexcitonic FWM polarization is demonstrated which enables a coherent manipulation of the amplitude and phase of exciton–biexciton beats which are observed on the FWM polarization transients.
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We investigate interband coherences as well as coherences between ${\ensuremath{\sigma}}^{+}$ and ${\ensuremath{\sigma}}^{\ensuremath{-}}$ exciton states in a 10 nm thick ZnSe/ZnMgSe single quantum well by spectrally resolved three-pulse degenerate four-wave mixing using circularly polarized 100 fs pulses. Polarization and intensity dependent measurements are performed to identify the coherent processes responsible for the nonlinear signal into the ${\mathbf{k}}_{3}+{\mathbf{k}}_{2}\ensuremath{-}{\mathbf{k}}_{1}$ direction and to study the influence of Coulomb scattering on the dephasing rates. The experiments reveal nearly equal zero-density dephasing rates for coherences between ${\ensuremath{\sigma}}^{+}$ and ${\ensuremath{\sigma}}^{\ensuremath{-}}$ heavy- and/or light-hole exciton states as compared to the dephasing rate of the interband coherence between these states and the ground state. The measurements also demonstrate that exciton--exciton scattering destroys the phase coherence between heavy- and light-hole excitons about three times more effectively than the coherence between ${\ensuremath{\sigma}}^{+}$ and ${\ensuremath{\sigma}}^{\ensuremath{-}}$ heavy-hole excitons. The characteristic features of the experimental results are explained and reproduced by numerical calculations of the optical Bloch equations for a ten-level model including excitation induced dephasing.
We demonstrate spectroscopically how optical gain is formed in an interacting system of excitons and biexcitons in a single ZnSe quantum well. The dynamics of gain formation are studied on a subpicosecond time scale in pump-probe experiments, revealing the influence of coherent effects and the impact of exciton-exciton and exciton-biexciton interactions. Spectrally resolved, polarization-dependent degenerate four-wave-mixing experiments further demonstrate how the excitonic many-body phenomena profoundly influence the nonlinear optical response in this II-VI semiconductor heterostructure. \textcopyright{} 1996 The American Physical Society.