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Physical Review Letters

Demonstration of Sixth-Order Coulomb Correlations in a Semiconductor Single Quantum Well

S. R. Bolton, U. Neukirch, Lu Jeu Sham, D. S. Chemla, V. M. Axt

Published Aug 28, 2000• 66 citations
Publisher

Abstract

Six-wave mixing in a ZnSe quantum well is investigated and compared with microscopic theory. We demonstrate that sixth-order Coulomb correlations have a significant qualitative impact on the nonlinear optical response. Six-wave mixing is shown to be a uniquely sensitive tool for investigation of correlations beyond the four-point level.
DOI
10.1103/physrevlett.85.2002

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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.
Summary form only given. The nonlinear optical response in semiconductors has traditionally been treated in a mean field approximation at the 2-particle level. Recent work, in particular comparisons of four-wave mixing (FWM) with microscopic theory, have demonstrated the importance of 4-particle correlations. Such experiments, however, are not optimally sensitive to correlations at the 6-particle level. In order to probe such six-particle correlations we compare the results of six-wave mixing (SWM) measurements with a detailed microscopic theory based on the dynamics controlled truncation scheme (DCT).
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.
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.
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.