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Journal of the Physical Society of Japan

Quantitative Study of Exciton-Exciton Interaction in a GaAs Microcavity

C. Ramkumar, Takao Aoki, Ryo Shimano, Yuri P. Svirko, Tomofumi Kise, Takao Someya, H. Sakaki, Makoto Kuwata‐Gonokami

Published Aug 15, 2000• 2 citations
Publisher

Abstract

We employ a pump-induced polarization rotation scheme for the quantitative study of four-particle (exciton-exciton) correlations in a strongly coupled semiconductor microcavity. From the measured rotation angle in the χ (3) -regime, in which the nonlinear response is linearly proportional to pump intensity ( I p u m p ), we evaluate the absolute value of anharmonicity of two-dimensional excitons. Deviation from the χ (3) -regime is observed beyond I p u m p =0.2 kW/cm 2 .

DOI
10.1143/jpsj.69.2439

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We employ a pump-induced polarization rotation scheme for the quantitative study of four-particle (exciton-exciton) correlations in a strongly coupled semiconductor microcavity. From the measured rotation angle in the χ (3) -regime, in which the nonlinear response is linearly proportional to pump intensity ( I p u m p ), we evaluate the absolute value of anharmonicity of two-dimensional excitons. Deviation from the χ (3) -regime is observed beyond I p u m p =0.2 kW/cm 2 .
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.
Summary form only given. The ultrafast nonlinear optical response of semiconductor-microcavities (SMCs) in the nonperturbative regime is attracting growing interest for exploring fundamental light-matter interactions in many-particle quantum systems, as well as for the future implementations of ultrafast photonic devices. In spite of many investigations, the coherent dynamics of excitonic nonlinear-response in the nonperturbative regime has not been fully understood. Open questions are how strong exciton-cavity coupling affects exciton-exciton (X-X) interactions, and how in turn the X-X correlation influences the nonlinear response of SmCs. We investigate these open questions and show that the nonperturbative regime provides an unprecedented tool for investigating four-particle correlations.We start from the equations for the third order exciton polarization and cavity field describing quantum optical effects and coherent nonlinear optics in SMCs, perform the semiclassical factorization and include multiple scattering processes.
We show that the exciton–exciton scattering continuum has a significant influence on the transient non-linear optical response of semiconductor microcavities. Comparison between transient shifts observed in pump and probe experiments and calculations demonstrates almost complete cancellation between mean-field and two-exciton continuum contributions. Moreover, we show that suppression of non-linear absorption of the lower polariton observed in many experiments is determined by the specific spectral shape of these correlations. In particular, we find that the pump induced dephasing of polariton resonances is proportional to the spectrum of four-particle correlations calculated at the energy sum of the pumped and probed polaritons.
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.
We report on the optical response of a semiconductor microcavity featuring a strong exciton–photon coupling. The weak excitation regime is investigated experimentally by means of time-resolved transmission and four-wave mixing experiments. The influence of electronic disorder on the coherent exciton–photon dynamics is discussed in terms of the solutions of the Maxwell-Bloch equations. The high excitation regime is investigated by using transient sub-picosecond pump–probe experiments. Optical amplification of the probe beam (up to a factor of five), as well as a fundamental change of the optical spectra, have been found close to and above the exciton saturation density. The observed oscillations are corresponding to the Rabi frequency of the excitons in the pump field.