Fifth-order two-dimensional Raman spectra of CS2 are dominated by third-order cascades

David A. Blank, Laura J. Kaufman, Graham R. Fleming

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194 Scopus citations

Abstract

We have demonstrated that fifth-order stimulated Raman spectra of the intermolecular modes in CS2 are dominated by cascading third-order processes. Previous studies have successfully discriminated against a sequential cascading process, but did not account for parallel third-order cascades. All of our measured spectra were successfully simulated considering only cascades built directly from our measured third-order spectra. Using an appropriately chosen phase matching geometry we also measured the sequential cascade, which should exist with equal probability to the parallel cascade. When employing a phase matching geometry that provided substantial discrimination against all of the third-order cascades we were not able to measure any signal. We assign an upper limit for the true fifth-order signal of 2% of the cascaded signal.

Original languageEnglish (US)
Pages (from-to)3105-3114
Number of pages10
JournalJournal of Chemical Physics
Volume111
Issue number7
DOIs
StatePublished - Aug 15 1999

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