Coherent Molecular Vibrational Motion Observed in the Time Domain Through Impulsive Stimulated Raman Scattering

S. Ruhman, A. G. Joly, K. A. Nelson

Research output: Contribution to journalArticlepeer-review

202 Scopus citations

Abstract

Femtosecond time-resolved observations of coherent molecular vibrations are carried out through impulsive stimulated Raman scattering (ISRS). Individual cycles of vibrational oscillation, as well as vibrational dephasing, are time resolved. ISRS therefore provides a means through which time-resolved spectroscopy of vibrationally distorted molecules can be carried out. Several experimental configurations involving either crossed excitation pulses or a single excitation pulse are discussed theoretically and demonstrated experimentally. The experiments with a single excitation pulse show that ISRS occurs whenever a sufficiently short pulse passes through a Raman-active medium. In some configurations, the ISRS experiment is strictly analogous to polarized or depolarized light scattering spectroscopy, and ISRS data contain in the time domain the full information content of the corresponding frequency-domain Raman (and Rayleigh) spectra. In molecular liquids, ISRS therefore probes both vibrational and orientational dynamics.

Original languageEnglish
Pages (from-to)460-469
Number of pages10
JournalIEEE Journal of Quantum Electronics
Volume24
Issue number2
DOIs
StatePublished - Feb 1988
Externally publishedYes

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