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Physical Review Letters

Ultrafast Optical Spectroscopy of Spectral Fluctuations in a Dense Atomic Vapor

Virginia O. Lorenz, Shaul Mukamel, W. Zhuang, Steven T. Cundiff

Published Jan 10, 2008• 46 citations
Publisher

Abstract

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.

DOI
10.1103/physrevlett.100.013603

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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.
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.
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.
A theory for the nonlinear optical response of an assembly of four level atoms representing an s–p transition, with dipole–dipole interactions is developed. Simulation results for two-pulse ultrafast four wave mixing measurements in atomic clusters and in liquids demonstrate that the electronic density of states can be obtained by combining absorption and four wave mixing experiments. We show that a sensitive direct probe for interatomic interactions and correlations is provided by reversing the pulse time ordering in a photon echo sequence. The effect of nuclear motions on the linear absorption spectrum is investigated.