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Comparison of phenomenological models with a microscopic theory for semiconductor optical nonlinearities

I. Rumyantsev, N. H. Kwong, Ryu Takayama, Rolf H. Binder

Published Jun 23, 2000• 0 citations
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Abstract

A microscopic theory of the third order coherent semiconductor optical response is used for the investigation of four-wave mixing signals. The theory is based on the dynamics-controlled truncation formalism and evaluated for the case of resonant excitation of heavy-hole excitons. This approach allows for a direct comparison with other theories (microscopic or phenomenological). and yields a detailed understanding of important many-body effects such as excitation-induced dephasing.

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Journal of the Optical Society of America B•Dec 1, 2004•6 citations
A microscopic theory of the third order coherent semiconductor optical response is used for the investigation of four-wave mixing signals. The theory is based on the dynamics-controlled truncation formalism and evaluated for the case of resonant excitation of heavy-hole excitons. This approach allows for a direct comparison with other theories (microscopic or phenomenological). and yields a detailed understanding of important many-body effects such as excitation-induced dephasing.
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.
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 theory of degenerate four-wave mixing (DFWM) in the low density excitation limit at the semiconductor band edge is developed on the basis of the bosonic representation of the electron-hole Hamiltonian. By accounting for the exciton-exciton interactions of the lowest order we arrive at the practical few-level density matrix description of the third-order excitonic nonlinearity. The developed theory accounts phenomenologically for the phase space filling, and excitation induced dephasing effects and well reproduces the results of the recent DFWM experiments in high- and low-fineness microcavity. We show that polarization-sensitive four-wave mixing measurements enable to discriminate the contributions to the DFWM signal from the exciton-exciton interactions of different symmetry.
In order to optimize opto-electronic applications of semiconductor nanostructures, a deep understanding of optical nonlinearities is essential.One fundamental method currently used within this field of research is ultrafast optical spectroscopy.This work presents a theoretical study of optical nonlinearities in semiconductor quantum wells in the coherent time regime.The theory is based on the equations of motion for the coherent exciton and biexciton transition amplitudes.These equations are derived using two different ways: Heisenberg equations of motion in combination with the dynamics-controlled truncation theory and alternatively the non-equilibrium Green´s function technique. For the coherent regime both approaches are equivalent and can be used to formulate a coupled set of equations for the coherent excitation dynamics that is correct up to the third order in the optical field.In contrast to the dynamics-controlled truncation theory the non-equilibrium Green´s function technique allows the inclusion of incoherent scattering processes into the description.The theory is evaluated to describe pump and probe as well as four-wave-mixing experiments with ZnSe quantum wells.Numerical calculations for the coherent control of the macroscopic polarization andthe dependence of transient four-wave-mixing on the light-polarization and intensity are both in good agreement with experiments.In order to correctly describe elevated excitation conditions for the latter investigation, the theory is self-consistently extended such that the included excitonic and biexcitonic nonlinearities contribute up to arbitrary order in the optical field.
We analyze a generic atomic few-level model for the third-order $({\ensuremath{\chi}}^{(3)})$ optical response of semiconductor quantum wells. The purpose is to seek a good understanding of the physical nature of the model's parameters in terms of the material's microscopic constituents and their motions. The strategy is to bring the algebraic expression of the ${\ensuremath{\chi}}^{(3)}$ interband polarization in the few-level model to a form similar to that derived in microscopic theories. Most importantly, in the coherent limit, we make the ``time evolution structure'' of the interband polarization in the few-level and microscopic formalisms coincide, whereby the atomic model's parameters can be interpreted microscopically through a comparison of terms of similar structure in the two formalisms. We also discuss how the conclusion of this comparison can be changed by the introduction of phenomenological dephasing and decay into both theories.
A detailed numerical study of the third-order nonlinear optical susceptibilities (χ(3)) of semiconductor quantum wells is presented. The dependence of χ(3) on material parameters (electron-hole mass ratio and exciton linewidths), on the light polarization configuration (co- and countercircularly polarized) and on the spectral configuration is discussed. The goal of this study is to map out the nonlinear phase shift per quantum well and a related figure of merit caused by quasi-resonant excitonic and biexcitonic nonlinearities induced by picosecond light pulses. The study is based on the dynamics-controlled truncation formalism and evaluated under the assumption that only 1s-heavy-hole excitons contribute to the nonlinearities. It includes all correlation effects (exciton–exciton scattering in the singlet and triplet channels and coherent biexciton formation in the singlet channel) that contribute within the coherent excitonic χ(3) regime.