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 journalArticle

12 Citations (Scopus)

Abstract

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
Article number094106
JournalJournal of Chemical Physics
Volume145
Issue number9
DOIs
Publication statusPublished - Sep 7 2016

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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