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Bulletin of the Korean Chemical Society (BKCS)

ISSN 0253-2964(Print)
ISSN 1229-5949(Online)
Volume 24, Number 8
BKCSDE 24(8)
August 20, 2003 

Experimental Determinations of Coherent Multidimensional Vibrational Spectroscopy
Daniel Besemann, Nicholas Condon, Kent Meyer, Wei Zhao, John C. Wright
Nonlinear, Vibrational, Two dimensional, Coherent, Infrared
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 ( c(3)) for the nonlinear processes. We show that the DOVE c(3) values are directly related to the molar absorptivities and Raman c(3). We then use these relationships to obtain estimates for the c(3) of the stimulated photon echo and c(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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