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Experimental Determinations of Coherent Multidimensional Vibrational Spectroscopy
Experimental Determinations of Coherent Multidimensional Vibrational Spectroscopy
Bulletin of the Korean Chemical Society. 2003. Aug, 24(8): 1119-1125
  • Published : August 20, 2003
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Besemann Daniel
Condon Nicholas
Meyer Kent
Zhao Wei
Wright John C.

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 <TEX>$(��^{(3)})$</TEX> for the nonlinear processes. We show that the DOVE <TEX>$��^{(3)}$</TEX> values are directly related to the molar absorptivities and Raman <TEX>$��^{(3)}$</TEX>. We then use these relationships to obtain estimates for the <TEX>$��^{(3)}$</TEX> of the stimulated photon echo and <TEX>$��^{(5)}$</TEX> 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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