Coupled wave equations theory of surface-enhanced femtosecond stimulated Raman scattering

Michael O. McAnally, Jeffrey M. McMahon, Richard P. Van Duyne, George C. Schatz

Research output: Contribution to journalArticlepeer-review

19 Scopus citations


We present a coupled wave semiclassical theory to describe plasmonic enhancement effects in surface-enhanced femtosecond stimulated Raman scattering (SE-FSRS). A key result is that the plasmon enhanced fields which drive the vibrational equation of motion for each normal mode results in dispersive lineshapes in the SE-FSRS spectrum. This result, which reproduces experimental lineshapes, demonstrates that plasmon-enhanced stimulated Raman methods provide unique sensitivity to a plasmonic response. Our derived SE-FSRS theory shows a plasmonic enhancement of |gpu|2ImχR(ω)gst2/ImχR(ω), where |gpu|2 is the absolute square of the plasmonic enhancement from the Raman pump, χR(ω) is the Raman susceptibility, and gst is the plasmonic enhancement of the Stokes field in SE-FSRS. We conclude with a discussion on potential future experimental and theoretical directions for the field of plasmonically enhanced coherent Raman scattering.

Original languageEnglish (US)
Article number094106
JournalJournal of Chemical Physics
Issue number9
StatePublished - Sep 7 2016

ASJC Scopus subject areas

  • General Physics and Astronomy
  • Physical and Theoretical Chemistry


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