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Physical Review B

Echo peak-shift spectroscopy of non-Markovian exciton dynamics in quantum wells

Sam Carter, Z. Chen, Steven T. Cundiff

Published Sep 28, 2007• 22 citations
Publisher

Abstract

Three-pulse four-wave mixing is used to observe the loss of system memory for excitons confined in quantum wells. By measuring the photon echo peak shift with pulse delay, we obtain the two-time exciton frequency fluctuation correlation function. Spectral diffusion of localized excitons gives rise to exponential decay of the correlation function, while static inhomogeneity gives an offset. Nonmonotonic behavior during the first few picoseconds indicates complex memory effects due to the interaction of excitons with acoustic phonons.

DOI
10.1103/physrevb.76.121303

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Physical Review Letters•Jan 10, 2008•46 citations
Three-pulse four-wave mixing is used to observe the loss of system memory for excitons confined in quantum wells. By measuring the photon echo peak shift with pulse delay, we obtain the two-time exciton frequency fluctuation correlation function. Spectral diffusion of localized excitons gives rise to exponential decay of the correlation function, while static inhomogeneity gives an offset. Nonmonotonic behavior during the first few picoseconds indicates complex memory effects due to the interaction of excitons with acoustic phonons.
The three-pulse photon echo technique has provided significant insight into ultrafast dynamics in a variety of condensed phase systems1. Clear signatures of non-Markovian dynamics in a dense potassium vapor2 provide the opportunity to gain further insight into the correlation function of frequency fluctuations both experimentally and theoretically. Here, experimental three-pulse photon echo peak shifts are compared to calculated peak shifts that include the long-range resonant interactions in a dense atomic vapor within an exciton formalism3. A slow exponential decay in the peak shifts is attributed to long-range resonant interactions.
The polarization dependence of the ultrafast nonlinear response of localized excitons in GaAs/AlGaAs quantum wells has been investigated by spectrally resolved, transient four-wave mixing. The role of the excitation-induced dephasing in the delay dependence of the signal is discussed in detail. In particular, we show experimentally that the excitation-induced dephasing gives rise to a photon echo in inhomogeneous systems. We develop a simple analytical model for the delay dependence of the signal, which enables us to deduce the dephasing time from the four-wave mixing decay.
Transient four-wave mixing experiments with 100 fs pulses in a dense potassium vapor probe the electronic energy fluctuations that lead to optical decoherence. Echo-peak shift experiments yield a biexponential two-time correlation function of energy level fluctuations. Molecular dynamics simulations show that the slow component is a many-body excitonic contribution arising from long-range resonant interactions. The decay of the correlation function occurs on comparable time scales in theory and experiment.