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Physical review. B, Condensed matter

Spectroscopy of four-particle correlations in semiconductor microcavities

Salvatore Savasta, Omar Di Stefano, R. Girlanda

Published Jul 31, 2001• 24 citations
Publisher

Abstract

We present a theory of ultrafast time-resolved pump and probe spectroscopy in semiconductor microcavities. The numerical solutions are in excellent agreement with experimental data. An analytical study based on the Weisskopf-Wigner approximation gives physical insight into the transient optical nonlinearities of semiconductor microcavites. It is able to explain the physical origin of the unusual transient shifts and asymmetric-excitation-induced dephasing observed experimentally. This theory demonstrates that the nonperturbative regime provides a unique tool for measuring the spectrum of four-particle correlations.

DOI
10.1103/physrevb.64.073306

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We present a theory of ultrafast time-resolved pump and probe spectroscopy in semiconductor microcavities. The numerical solutions are in excellent agreement with experimental data. An analytical study based on the Weisskopf-Wigner approximation gives physical insight into the transient optical nonlinearities of semiconductor microcavites. It is able to explain the physical origin of the unusual transient shifts and asymmetric-excitation-induced dephasing observed experimentally. This theory demonstrates that the nonperturbative regime provides a unique tool for measuring the spectrum of four-particle correlations.
Summary form only given. Optical interactions in semiconductor microcavities embedded with quantum wells enter a nonperturbative regime when the dipole coupling rate between the exciton and the cavity mode exceeds relevant decay rates. In this regime, coherent energy exchange between the exciton and the cavity mode, i.e. normal mode oscillation (NMO), takes place when the cavity mode is excited impulsively by a short laser pulse. Similar coherent oscillations have also been observed in transient four-wave mixing (FWM) responses. In this paper, we present experimental and theoretical studies on the nature of oscillations in these transient FWM responses. We show that, in contrast to earlier beliefs, oscillations in time-integrated transient FWM do not correspond to NMO of the exciton or photon populations. Theoretical studies further reveal that FWM arising from different physical mechanisms including band filling, excitation-induced dephasing, and renormalized electric fields is characterized by highly distinct coherent dynamics. Oscillations in transient FWM reflect interference between these coherent optical processes and can be used as a unique probe for exciton many-body interactions in the nonperturbative regime.
We report experimental and theoretical studies of the transient nonlinear response from semiconductor microcavities. We show that, in the nonperturbative regime, oscillations in time-integrated transient four-wave mixing do not correspond to normal mode oscillations of either the exciton or photon population in the cavity. Coherent nonlinear responses arising from band filling, excitation-induced dephasing, and renormalized electric fields feature highly distinctive dynamical behaviors. Coherent dynamics in transient four-wave mixing reflects interference between these nonlinear processes.
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.
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.