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Physical Review B

Excitation-induced dephasing and biexcitonic effects in the coherent control of excitonic polarization in pulse-transmission experiments

T. Voss, Hans Georg Breunig, Ilja Rückmann, J. Gutowski

Published May 27, 2004• 12 citations
Publisher

Abstract

Optical coherent manipulation of excitonic polarization is studied in pulse-transmission experiments at medium to high excitation intensities. As a well-defined model system a ZnSe single-quantum well is used. It is found that for constant excitation intensities the dephasing time of the polarization in the sample changes significantly if the cases of coherent amplification and destruction are compared. This effect is explained in terms of an excitation-induced dephasing. The change of the dephasing time of the polarization is quantified. Furthermore, the simultaneous excitation of the exciton and exciton-biexciton resonances is shown to strongly influence the signal of the polarization in the coherent-control experiments. Both the excitation-induced dephasing and the biexcitonic effects are simulated by use of phenomenological models which give a good agreement with the experiments.

DOI
10.1103/physrevb.69.205318

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Optical coherent manipulation of excitonic polarization is studied in pulse-transmission experiments at medium to high excitation intensities. As a well-defined model system a ZnSe single-quantum well is used. It is found that for constant excitation intensities the dephasing time of the polarization in the sample changes significantly if the cases of coherent amplification and destruction are compared. This effect is explained in terms of an excitation-induced dephasing. The change of the dephasing time of the polarization is quantified. Furthermore, the simultaneous excitation of the exciton and exciton-biexciton resonances is shown to strongly influence the signal of the polarization in the coherent-control experiments. Both the excitation-induced dephasing and the biexcitonic effects are simulated by use of phenomenological models which give a good agreement with the experiments.
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.
The optical coherent-control technique is used to study biexcitonic effects in the four-wave-mixing signal of a ZnSe single quantum well. The signal is analyzed in both directions 2k1 − k2 and 2k2 − k1 which are not equivalent if a pulse pair is applied from direction k1 to achieve coherent control of the induced polarization. It is shown that the coherent control enables a selective enhancement or suppression of the contribution at the exciton and biexciton resonance to the signal, respectively, but only for certain sequences of the excitation pulses. Further, the suppression of exciton-biexciton beats in the signal as a function of tdel by a selective destruction of the biexciton polarization is demonstrated.
Abstract We present results of experimental work in which the coherent‐control technique has been applied to study the coherent manipulation of excitonic polarization in ZnSe quantum‐well samples. We will introduce the linear control of excitonic polarization in pulse‐transmission experiments and afterwards focus on the question if and how the optical transition from the excitonic states to the bound‐biexciton state can be subject to a directed coherent control. The experimental results will be compared to simulations based on a microscopic theory and will also be explained on the base of a phenomenological few‐level model. The overall suitability of coherent control for the investigation of exciton systems in low‐dimensional wide‐gap materials will be discussed. (© 2006 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)
Coherently controlled six-wave-mixing experiments on a ZnSe single quantum well are performed with different polarizations of the excitation pulses to enable or disable the creation of a biexcitonic polarization. A significant contribution of the biexcitonic polarization and other two-pair correlations is observed in the signal which is mainly modulated with the exciton transition frequency. A microscopic theory based on the dynamics controlled truncation scheme including six-point correlations is able to reproduce the experimental results.
Biexcitonic polarization excited in a ZnSe quantum well is coherently controlled with a pair of phase-locked laser pulses. The coherent control of this four-particle correlation is directly verified by observing a spectrally resolved four-wave-mixing signal in direction of the first order of diffraction of the pulse pair. By using polarization selection rules for the generation of biexcitons and changing the interpulse delay of the pulse pair the oscillations of the four-wave-mixing signal are studied at the energetic position of the excitonic as well as the biexcitonic resonance. The excitonic and biexcitonic signals exhibit a phase shift in dependence on the interpulse delay which clearly indicates the separate coherent control of the excitonic and biexcitonic polarization.
The polarization decay of the exciton and bound‐biexciton states in a ZnSe single quantum well was studied as a function of the temperature in real‐time‐resolved pulse‐transmission and spectrally resolved four‐wave‐mixing experiments. Optical and acoustic‐phonon scattering coefficients for both resonances were determined and found to be comparable. Additionally, the impact of the dephasing of the coherent excitonic polarization on coherent‐control experiments was analyzed as a function of the sample temperature.