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Quantum Electronics and Laser Science Conference

Higher order exciton correlations from six-wave mixing

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

Published May 12, 2000• 0 citations
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Abstract

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).

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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).
Coherently controlled four-wave-mixing (FWM) measurements have turned out to be a very sensitive tool to investigate the microscopic origin of the nonlinear optical response of semiconductor quantum-well structures, in particular if excitons are excited [1-3]. The measured signal oscillates as a function of the phase difference of the two interferometric pulses and is modulated additionally by contributions that oscillate with integer multiples of the excitonic resonance frequency. The influence of these harmonics can be measured in background free directions, i.e., the first (FWM) or second (six-wave mixing, SWM) diffracted order in direction 2k2-k1 or 3k2-2k1, respectively. Their intensity is easily quantified by inspecting the corresponding Fourier transforms (FT). Here, we report on transient interferometric SWM measurements and the influence of biexcitons on the signal.
Summary form only given. Using a full microscopic many-body theory, based on the dynamics-controlled truncation (DCT) formalism, we compute four-wave mixing spectra of thin semiconductor quantum well microcavities within the lowest-order nonlinear regime (/spl chi//sup (3)/-regime). Specifically, we focus on heavy-hole 1s excitons and corresponding two-exciton correlations (coherent biexcitons and two-exciton continuum correlations). Within this approach, the linear optical response corresponding to hh-excitons with given absorption lineshapes are inputs to the calculation of the nonlinear FWM spectra.
This dissertation addresses both fundamental aspects of Coulomb correlations in semiconductor quantum wells and more practical aspects of theoretical analysis of semiconductor optoelectronic devices. After introducing the subject, we present and evaluate a state-of-the-art theory of the third order coherent optical response of a semiconductor quantum well based on the Dynamics Controlled Truncation (DCT) scheme. Already in the third order (the so-called chi (3)) regime, semiconductors exhibit a number of many-body Coulomb correlation effects. Their manifestation in various multi-pulse experimental configurations, customarily used in ultrafast semiconductor spectroscopy, has been an important component of this thesis. Coherent optical effects in a semiconductor 3-band system based on the heavy-hole, light-hole and conduction bands were investigated. The quantum beats in the time-integrated differential transmission signal were analyzed and compared with experimental data obtained at the University of Iowa. Fundamental differences from corresponding quantum beats in atomic 3-level systems were found. Also, the analysis of experimental data (obtained at the University of Arizona) of the coupled heavy-hole-light-hole optical Stark shift revealed evidence of intervalence band coherences, an analog of Raman coherences in atomic 3-levels systems. A scheme for realization of electromagnetically-induced transparency (EIT) based on the interference of excitonic and biexcitonic coherences was proposed. Corresponding experiments performed at the University of Oregon showed indeed a considerable coherent reduction of excitonic absorption. Furthermore, an extension of the chi(3) analysis revealed an energy renormalization of the biexciton, in good agreement with the corresponding experiment. A microscopic analysis of polarization dynamics in time-resolved four-wave mixing signals was performed, revealing interesting implications for the biexciton dephasing in addition to the significance of many-body correlations. In the case of four-wave mixing in semiconductor microcavities, our theoretical analysis in conjunction with experimental data obtained at the University of Tokyo gave us indications for a significant shortcoming of the second Born approximation (2nd BA) applied to two-exciton Coulomb correlations in a thin semiconductor quantum well, in agreement with the general knowledge of the qualitative failure of the 2nd BA in systems with short-range interaction in two dimensions. We also analyzed a novel all-optical switching technique based on the nonlinear polarization rotation. Apart from identifying the many-particle processes relevant for the switch operation in the chi(3) regime, we proposed ways to further optimize the switch.
We report direct investigations of the coherence of four-particle (exciton-exciton) correlations by ultrafast four-wave mixing experiments. We determine the sensitivity of the coherence of the four-particle correlations to temperature and excitation density, comparing it to the coherence of the two-particle correlations. We discuss our results in terms of numerical solutions of the general kinetic equations, treating the four-particle correlations in the second order Born approximation. We introduce a simple model deduced from these kinetic equations that provides an intuitive interpretation of our results.