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physica status solidi (b)

Coherent control of exciton–biexciton beats: direction selectivity of four‐wave‐mixing signals in experiment and microscopic theory

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

Published Jul 12, 2006• 1 citation
Publisher

Abstract

Abstract In experiments and simulations based on a microscopic theory the optical coherent control of exciton–biexciton beats in coherent four‐wave‐mixing signals from a semiconductor quantum well is demonstrated. It is found that a reduction of the beat amplitude for one four‐wave‐mixing direction may at the same time coincide with a large beat amplitude for the other direction. The results can be understood by considering that at least two‐photon processes are required to coherently excite biexcitonic transitions which are responsible for the occurrence of the beat structure in the four‐wave‐mixing signals. (© 2006 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)

DOI
10.1002/pssb.200668068

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Abstract In experiments and simulations based on a microscopic theory the optical coherent control of exciton–biexciton beats in coherent four‐wave‐mixing signals from a semiconductor quantum well is demonstrated. It is found that a reduction of the beat amplitude for one four‐wave‐mixing direction may at the same time coincide with a large beat amplitude for the other direction. The results can be understood by considering that at least two‐photon processes are required to coherently excite biexcitonic transitions which are responsible for the occurrence of the beat structure in the four‐wave‐mixing signals. (© 2006 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)
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Abstract Four wave mixing signals from single dots and dot ensembles involving excitonic and biexcitonic transitions are discussed. The results have been obtained analytically from a four level dot model coupled to longitudinal acoustic phonons. Time integrated four wave mixing amplitudes for quantum dot ensembles exhibit polarization dependent quantum beats that have already been found in experimental data. In four wave mixing signals of single quantum dots we find that the ground state to exciton transition has two contributions. One is identical to the known solution of the two level quantum dot model and leads to symmetric spectra for longer delay times, while the other comprises phase information from the biexciton and results in asymmetric spectra. (© 2006 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)
By use of an optical coherent-control technique we demonstrate and analyze the control of transitions involved in the generation of four-wave-mixing signals in a semiconductor quantum well for the two different four-wave-mixing directions and for different sequences of the excitation pulses. Results are presented for frequency- as well as for time-resolved signals. A doubling of the coherent switching frequency is found which occurs if the laser pulses performing the control process contribute quadratically to the wave-mixing signal. A direct comparison between experiment and microscopic theory reveals how the coherent-control process acts on the coherent polarization of the exciton-biexciton system in all different configurations. An additional interpretation of the experimental results based on a simplified few-level model is able to provide an intuitive understanding of the relevant processes which govern the coherent control of the excitonic and biexcitonic wave-mixing polarizations.
Systematic measurements and microscopic simulations were performed to study the optical coherent control of the exciton‐biexciton systems in a ZnSe quantum well. Our results show that the spectral components in the four‐wave mixing signal at the exciton and the exciton‐biexciton transition, respectively, can be separately controlled in the coherent regime. This separate control also results in different beat structures on the real‐time transients of the nonlinear wave‐mixing polarization. With respect to all important features experiment and simulation are in excellent agreement.
Two-pair correlations are shown to induce dependences of the nonlinear optical response of semiconductors that can be used for a coherent manipulation of the resulting emission. Influences of biexcitonic transitions as well as transitions to two-pair scattering states are discussed within a microscopic density matrix approach. It is shown that the coherent control of biexciton beats is selective with respect to the propagation direction of the emitted signal, in contrast to the control of beats where all beat partners are generated by single photon processes. Furthermore, it is demonstrated that memory structures induced by exciton?exciton scattering states enable coherent manipulations of the excitonic line shape that allow us to estimate lower bounds for the corresponding memory time from experimentally accessible data.
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.