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Experimental Investigation of Quantum Effects in Time-Resolved Resonant Rayleigh Scattering from Quantum Well Excitons

D. Birkedal, Jagdeep Shah, Andrei V. Shchegrov, Loren N. Pfeiffer

Published Mar 1, 2000• 3 citations
Publisher

Abstract

Resonant Rayleigh scattering from quantum well excitons is investigated using ultrafast spectral interferometry. We isolate the coherent Rayleigh scattering from incoherent luminescence in a single speckle. Averaging the resonant Rayleigh intensity over several speckles allows us to identify features in support of quantum corrections to the classical description of the underlying scattering process.

DOI
10.1002/1521-396x(200003)178:1<5::aid-pssa5>3.0.co;2-h

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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. After the first observation of resonance scattering from excitons in quantum wells about 1980, this topic has received much interest and has given rise to a hot debate on the origin of this scattering process. Recently, the determination of the temporal behaviour and the coherence properties of this scattering has initiated revival of interferometric techniques in semiconductor optics. Finally, the observation of speckles in the angular distribution proved that this scattering indeed originates from exciton states localized by disorder. However, complementary information on the nature of the excitons and the interplay between scattering and luminescence can be obtained from high resolution cw spectroscopy, having the advantage that only a small fraction of the states within the homogeneous linewidth is excited. However yhe polarization behaviour is quite different for the coherent Rayleigh component and the luminescence, depending on the orientation, splitting and relaxation of the localized states. The experimental results for a 20 nm wide GaAs quantum well clearly confirm this prediction.
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.
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.
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.