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Experimental Determinations of Coherent Multidimensional Vibrational Spectroscopy

  • Besemann, Daniel (Department of Chemistry, University of Wisconsin-Madison) ;
  • Condon, Nicholas (Department of Chemistry, University of Wisconsin-Madison) ;
  • Meyer, Kent (Department of Chemistry, University of Wisconsin-Madison) ;
  • Zhao, Wei (Department of Chemistry, University of Wisconsin-Madison) ;
  • Wright, John C. (Department of Chemistry, University of Wisconsin-Madison)
  • Published : 2003.08.20
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Abstract

Coherent multidimensional vibrational spectroscopy is a new technique for establishing correlations between features in vibrational spectra that are caused by intra- and intermolecular interactions. These interactions cause cross-peaks between vibrational transitions that reflect the coupling. In this paper, we use Doubly Vibrationally Enhanced Infrared Spectroscopy (DOVE-IR) and DOVE-Raman processes to obtain coherent two dimensional vibrational spectra. The spectra are fitted to obtain the dephasing rates and third order susceptibilities $(χ^{(3)})$ for the nonlinear processes. We show that the DOVE $χ^{(3)}$ values are directly related to the molar absorptivities and Raman $χ^{(3)}$. We then use these relationships to obtain estimates for the $χ^{(3)}$ of the stimulated photon echo and $χ^{(5)}$ of the six wave mixing spectroscopies, respectively. We also predict the ratio of the cascaded four wave mixing signal to the six wave mixing signal.

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