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Chemical Physics

Ultrafast spectroscopy of a dense potassium vapor

Virginia O. Lorenz, Steven T. Cundiff

Published Jul 18, 2007• 5 citations
Publisher
DOI
10.1016/j.chemphys.2007.07.008

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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.

Physical Review Letters•Jan 10, 2008•46 citations
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.
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.