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Journal of the Optical Society of America B

Influence of higher Coulomb correlations on optical coherent-control signals from a ZnSe quantum well

Hans Georg Breunig, T. Voss, Ilja Rückmann, J. Gutowski, V. M. Axt, T. Kühn

Published Aug 1, 2003• 14 citations
Publisher

Abstract

The manipulation of the coherent optical polarization in a quantum well with a pair of phase-locked laser pulses is investigated by using wave-mixing signals. The measurements are performed in four- and six-wave-mixing geometries with different polarization states of the excitation pulses. Even at moderate excitation densities, the signals are modulated by higher harmonics that correspond to high-order optical nonlinearities. A significant effect of higher Coulomb correlations on the coherent-control signals is demonstrated by comparing the experiments with calculations based on a microscopic density-matrix theory. The theoretical approach makes use of the dynamics-controlled truncation scheme. The corresponding numerical results are in good agreement with the experiment.

DOI
10.1364/josab.20.001769

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The manipulation of the coherent optical polarization in a quantum well with a pair of phase-locked laser pulses is investigated by using wave-mixing signals. The measurements are performed in four- and six-wave-mixing geometries with different polarization states of the excitation pulses. Even at moderate excitation densities, the signals are modulated by higher harmonics that correspond to high-order optical nonlinearities. A significant effect of higher Coulomb correlations on the coherent-control signals is demonstrated by comparing the experiments with calculations based on a microscopic density-matrix theory. The theoretical approach makes use of the dynamics-controlled truncation scheme. The corresponding numerical results are in good agreement with the experiment.
Six-wave-mixing signals from a ZnSe quantum well are analyzed experimentally and with a microscopic density-matrix description using the dynamics-controlled-truncation scheme. For each physically distinct combination of polarizations of the exciting pulses, the spectrum of six-wave-mixing emission is measured as a function of time delay. The experimental results are compared with calculations performed at different levels of approximation. Although the leading order contributions to six-wave-mixing signals are of fifth order in the laser field, we show that there are significant signal components that are due to at least ${\ensuremath{\chi}}^{(7)}$ processes. The sensitivity of six-wave-mixing signals to high-order Coulomb correlations is demonstrated. Six-point density matrices are found to be indispensable for the interpretation of our experiments, while some details seem to indicate the involvement of even higher-order correlation functions. Furthermore, we find a remarkable dynamical decoupling of spectral signatures and the delay-time behavior after excitation with linearly polarized pulses.
The optical phase of four-wave-mixing (FWM) signals from a ZnSe single quantum well is analyzed experimentally and theoretically. The focus is on excitation conditions where the polarization state of the emitted light is dynamically changing rather than being fixed by selection rules, a case known to be sensitive to high-order Coulomb correlations. The phase is measured using an iterative procedure taking as input FWM signals with real-time resolution as well as frequency regime data. The results are compared with a microscopical density-matrix description using the dynamics controlled truncation (DCT) scheme. Mean-field Coulomb interactions, Pauli blocking and transitions to biexcitons and the two-pair scattering continuum are accounted for. Calculations in the coherent limit are able to reproduce the measured phases. The correlated two-pair scattering continuum is shown to have a significant impact on the phase.
The optical phase of four-wave-mixing (FWM) signals from a ZnSe single quantum well is analyzed experimentally and theoretically. The focus is on excitation conditions where the polarization state of the emitted light is dynamically changing rather than being fixed by selection rules, a case known to be sensitive to high-order Coulomb correlations. The phase is measured using an iterative procedure taking as input FWM signals with real-time resolution as well as frequency regime data. The results are compared with a microscopical density-matrix description using the dynamics controlled truncation (DCT) scheme. Mean-field Coulomb interactions, Pauli blocking and transitions to biexcitons and the two-pair scattering continuum are accounted for. Calculations in the coherent limit are able to reproduce the measured phases. The correlated two-pair scattering continuum is shown to have a significant impact on the phase.
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.
Correlations due to biexcitons as well as to two-pair scattering states are direct manifestations of Coulomb quantum kinetics. Effects resulting from the memory structure of the corresponding contributions to the optical interband polarization are analyzed taking a ZnSe single-quantum well as model system. Our calculations are based on a microscopic density matrix description using the dynamics controlled truncation scheme for closing the hierarchy of higher-order density matrices. A detailed comparison between experiment and theory allows for the identification of numerous effects directly reflecting different aspects of pair-correlations. In particular, we demonstrate various influences of the two-pair scattering continuum on four-wave-mixing signals. Furthermore, we show that signals with a dynamically changing polarization sensitively monitor a competition between coherent parts of the dynamics and signal components induced by incoherent exciton densities. Surprisingly, the phase of these signals is found to be almost unaffected by the presence of incoherent densities. This result can be traced back to a compensation of the influences on the phases resulting from different incoherent parts of the dynamics. Six-particle correlations representing transitions from incoherent densities to two-pair correlations turn out to be indispensable for a proper description of this effect.© (2001) COPYRIGHT SPIE--The International Society for Optical Engineering. Downloading of the abstract is permitted for personal use only.
A three-beam configuration is used to investigate the spectrally resolved wave-mixing signal of a ZnSe single quantum well. The spectrum recorded in direction 2 k2–k1 shows coherent oscillations induced by a delayed third pulse with direction k3. Intensity and polarization-dependent measurements indicate that the signal is generated by a combination of four- and six-wave mixing. The origin of the oscillations can be explained qualitatively by a two-level model. The polarization-dependent experimental results require the treatment of many-body correlations and are well explained by microscopic calculations including four-particle correlations up to fifth order in the fields.