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Journal of the Physical Society of Japan

Four-Wave Mixing Theory at the Excitonic Resonance: Weakly Interacting Boson Model

Yuri P. Svirko, Masayuki Shirane, Hidekatsu Suzuura, Makoto Kuwata‐Gonokami

Published Feb 15, 1999• 27 citations
Publisher

Abstract

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.

DOI
10.1143/jpsj.68.674

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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.
A microscopic semi-classical theory for the self-consistent calculation of the nonlinear response field is applied to the exciton–microcavity coupled systems. Our results show that the respective spectral features of the degenerated four wave mixing (DFWM) signal in both the weak (Ω ≤ Γ) and the strong coupling (Ω ≫ Γ) regimes, where Ω is the Rabi splitting and Γ is the width of the modes, can be clearly described with a single framework. In the weak coupling regime, the nonlinear signal is strongest at the bare excitonic resonance, and its enhancement due to cavity effect is remarkable. In the strong coupling regime, our framework very well reproduces the polarization dependent DFWM spectra in a recent experiment.
The nonlinear optical responses of a strongly coupled exciton-photon system in a semiconductor microcavity structure under weak excitation can be explained by a weak exciton-exciton interaction due to the nonideal bosonic (weakly interacting bosons) nature of the excitons. The exciton-exciton interaction leads to an attractive interaction between excitons with opposite spin, and a repulsive interaction between excitons with the same spin and a phase space filling. Earlier, we have reported the ratio of these interaction energies from the polarization-sensitive degenerate four-wave mixing on a strongly coupled GaAs quantum well (QW) microcavity under weak excitation density. In order to quantitatively determine the exciton-exciton polarization interaction energy, we have proposed a pump-probe nonlinear polarization rotation scheme. In the paper, we report the quantitative measurement of the exciton-exciton polarization interaction energy in the above mentioned system under strict weak excitation density using the pump-probe nonlinear polarization rotation (PR) technique. In the technique, the change of polarization state of a weak linearly polarized probe due to the anisotropy induced by a strong, circularly polarized pump is monitored in reflection geometry.
Summary form only given. Four-particle correlation mediated by the Coulomb interaction has been found to play a major role in the nonlinear optical response at the semiconductor band edge at low excitation density. The attractive interaction of the excitons with opposite spins result in the formation of bound (bi-exciton) and unbound (scattered) two-exciton states. In this paper we report on the first to our knowledge, comparison of the contributions to the coherent nonlinearity from the bound and unbound two-exciton states. The polarization-sensitive four wave mixing experiment is performed in the high-Q semiconductor microcavity, in which the incoherent effects are suppressed due to strong exciton-photon coupling. The semiconductor microcavity has a single 12-nm-thick GaAs quantum well.