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Three-Pulse Photon Echo Peak Shift Spectroscopy in a Dense Potassium Vapor

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

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 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.

Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)Jun 1, 20070 citations

Three-Pulse Photon Echo in a Dense Potassium Vapor

Virginia O. Lorenz, Steven T. Cundiff, W. Zhuang +1 more

Time-integrated three-pulse photon echo (3PE) and time-resolved 3PE measurements in dense potassium vapor reveal clear signatures of non-Markovian dynamics. We pursue a molecular dynamics simulation to study the many-body effects contributing to the response.

International Conference on Ultrafast PhenomenaJan 1, 20060 citations

Ultrafast Optical Spectroscopy of Spectral Fluctuations in a Dense Atomic Vapor

Virginia O. Lorenz, Shaul Mukamel, W. Zhuang +1 more

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.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 LettersJan 10, 200846 citations

Non-Markovian Dynamics in a Dense Potassium Vapor

Virginia O. Lorenz, Steven T. Cundiff

Transient four-wave mixing experiments on a dense potassium vapor, which has a dephasing time long compared to the collision duration, reveal distinct signatures of non-Markovian dynamics. Theoretical fits assuming stochastic fluctuation of the excited-state frequencies confirm that the two-time correlation function has a finite temporal width.

Physical Review LettersOct 13, 200568 citations

Three-pulse photon echo peak shift measurements in dense potassium vapor

Virginia O. Lorenz, Steven T. Cundiff

Three-pulse photon echo peak shift measurements in dense potassium vapor reveal an exponential peak shift, justifying an exponential two-time correlation function of frequency fluctuations, which is commonly assumed for more complex condensed phase systems.

Conference on Lasers and Electro-OpticsJan 1, 20060 citations

Excitation dependence of non-Markovian dynamics in a dense potassium vapor

Xingcan Dai, Steven T. Cundiff

The transient four-wave mixing signal from a dense potassium vapor, which displays non-Markovian dynamics, depends on the excitation strength. Theoretical fits reveal the excitation dependence of the parameters employ ed in a two-time correlation function.

Conference on Lasers and Electro-OpticsMay 1, 20080 citations

Non-Markovian dynamics in a dense atomic vapor

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Non-Markovian dynamics in a dense atomic vapor

Abstract

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