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Physical Review Letters

Monte Carlo Simulations of Ultrafast Resonant Rayleigh Scattering from Quantum Well Excitons: Beyond Ensemble Averaging

Andrei V. Shchegrov, D. Birkedal, Jagdeep Shah

Published Aug 16, 1999• 24 citations
Publisher

Abstract

We develop and experimentally verify novel Monte Carlo simulations of ultrafast resonant Rayleigh scattering from quantum well excitons. In contrast to existing theories, these simulations can study the dynamics and spectrum of resonant Rayleigh scattering from a single realization of disorder, and allow direct comparison to experimental data. We find excellent agreement between our experiments and simulations. Our studies demonstrate the high sensitivity of scattering dynamics to a particular realization of disorder, and provide new insights into the nature of spatial correlations of excitons.

DOI
10.1103/physrevlett.83.1391

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We develop and experimentally verify novel Monte Carlo simulations of ultrafast resonant Rayleigh scattering from quantum well excitons. In contrast to existing theories, these simulations can study the dynamics and spectrum of resonant Rayleigh scattering from a single realization of disorder, and allow direct comparison to experimental data. We find excellent agreement between our experiments and simulations. Our studies demonstrate the high sensitivity of scattering dynamics to a particular realization of disorder, and provide new insights into the nature of spatial correlations of excitons.
We report the first investigation of resonant secondary emission from quantum well excitons using ultrafast spectral interferometry. Observation of high-contrast spectral fringes demonstrates a significant phase correlation of the spectral components of the Rayleigh scattered light and allows us to determine the temporal dynamics of the coherent emission. The results contradict the present theories for resonant Rayleigh scattering based on ensemble averaging, and show the nonergodic nature of resonance Rayleigh scattering from semiconductor quantum wells.
Summary form only given. We present the first direct investigation of the coherence properties of resonant secondary emission (RSE) from quantum well excitons. Using ultrafast spectral interferometry, or TADPOLE, we measure spectral fringes that are resonantly enhanced at the exciton transitions. The fringe formation is due to the coherent Rayleigh component of the RSE, and allows us to investigate the dynamics of resonant Rayleigh scattering independent from incoherent luminescence. Our observation of high-contrast spectral fringes is in contradiction with current theories of time resolved resonant Rayleigh scattering from excitons and shows for the first time the non-ergodic nature of the RSE.
Coherent Rayleigh scattering and incoherent luminescence are studied by femtosecond upconversion under resonant excitation as a function of exciton density in GaAs quantum wells. Comparing samples with different well widths allows to establish the relation between inhomogeneous broadening and the shape of resonant Rayleigh scattering. We find an excellent agreement between experiment and a classical model. In samples with moderate inhomogeneous broadening we provide evidence for the transition from coherent to incoherent emission. The comparison with excitonic dephasing times T2 obtained from four-wave-mixing experiments demonstrates that the incoherent exciton population rises within T2/2, at any exciton density when changed by more than an orders of magnitude. The experimental results confirm very clearly the concept predicting that the coherent polarization made up by localized excitons decays into an incoherent exciton population under conservation of the number of excited quanta.
We report on the observation of coherent secondary emission from resonantly excited bound and unbound two-exciton states in quantum wells. The emission is intrinsic, in contrast to the well-known Rayleigh scattering from excitons that requires disorder. We measure the spectral amplitude and the phase (and, hence, the femtosecond dynamics) of this coherent emission using ultrafast spectral interferometry, and obtain direct information on the contributions to the nonlinear susceptibility from exciton-exciton correlations beyond the mean-field approximation.
We have performed spectral interferometry with Rayleigh scattered light coming from a single speckle and emitted after resonant creation of excitons in GaAs quantum wells. The experiment confirms the coherence of the secondary emission at early times, regardless of sample parameters, but underlines the stochastic nature of a single speckle. The scattered electric field is calculated, correctly accounting for the center-of-mass quantization in the disordered potential. We find that the amplitudes of the electric fields emitted by different excitons are uncorrelated, so that the well-known Poisson distribution for speckle intensities applies.