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Physical review. B, Condensed matter

Gain spectroscopy of excitonic molecules and its dynamics in a ZnSe single quantum well

Vladimir G. Kozlov, P. Kelkar, A. Vertikov, Arto V Nurmikko, C.-C. Chu, Jung Woo Han, C. G. Hua, Robert L. Gunshor

Published Nov 15, 1996• 27 citations
Publisher

Abstract

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.

DOI
10.1103/physrevb.54.13932

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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.
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 ${\ensuremath{\Delta}}_{h}=4.8\mathrm{meV}$ 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 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 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.
Ultrafast nonlinear optical spectroscopy is used to study the coherent dynamics of optically excited electron-hole pairs in semiconductors. Coulomb interaction implies that the optical inter-band transitions are dominated, at least at low temperatures, by excitonic effects. They are further enhanced in quantum confined lower-dimensional systems, where exciton and biexciton effects dominate the spectra even at room temperature. The coherent dynamics of excitons are at modest densities well described by the optical Bloch equations and a number of the dynamical effects known from atomic and molecular systems are found and studied in the exciton-biexciton system of semiconductors. At densities where strong exciton interactions, or many-body effects, become dominant, the semiconductor Bloch equations present a more rigorous treatment of the phenomena. Ultrafast degenerate four-wave mixing is used as a tool to study the coherent exciton dynamics, and the importance of performing transform limited spectroscopy is demonstrated throughout.
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.