Статья

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

David A. BlankDepartment of Chemistry, University of California, and Physical Biosciences Division, Ernest Orlando Lawrence Berkeley National Laboratory, Berkeley, California 94720Laura J. KaufmanDepartment of Chemistry, University of California, and Physical Biosciences Division, Ernest Orlando Lawrence Berkeley National Laboratory, Berkeley, California 94720Graham R. FlemingDepartment of Chemistry, University of California, and Physical Biosciences Division, Ernest Orlando Lawrence Berkeley National Laboratory, Berkeley, California 94720

1999en

ABI

Аннотация

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.

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Идентификаторы

DOI: 10.1063/1.479591

Цитирования и источники

Цитирований: 3Использованных источников: 0

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