Bulletin of the Korean Chemical Society

Korean Chemical Society (대한화학회)
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Two-color Transient Grating Spectroscopy of a Two-level System

  • Kwak, Kyoung-Won (Department of Chemistry and Center for Multidimensional Spectroscopy, Korea University) ;
  • Cho, Min-Haeng (Department of Chemistry and Center for Multidimensional Spectroscopy, Korea University) ;
  • Fleming, Graham R. (Department of Chemistry and Center for Multidimensional Spectroscopy, Korea University) ;
  • Agarwal, Ritesh (Department of Chemistry, University of California, Berkeley and Physical Biosciences Division,Lawrence Berkeley National Laboratory) ;
  • Prall, Bradley S. (Department of Chemistry, University of California, Berkeley and Physical Biosciences Division,Lawrence Berkeley National Laboratory)
  • Published : 2003.08.20
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Abstract

A theoretical description and experimental demonstration of homodyne-detected two-color transient grating (2-C TG) signal are presented. By treating the coupled bath degrees of freedom as a collection of harmonic oscillators and using a short-time expansion method, approximated nonlinear response functions were obtained. An analytic expression for the two-color transient grating signal was obtained by carrying out relevant Gaussian integrals. The initial rising and decaying parts of the 2-C TG signal is shown to be critically dependent on the ultrafast inertial component of the solvation correlation function. The experimental results confirm the predictions of the theoretical model.

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References

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