Fano-like resonances arising from long-lived molecule-plasmon interactions in colloidal nanoantennas

Renee R. Frontiera, Natalie L. Gruenke, Richard P. Van Duyne

Research output: Contribution to journalArticle

43 Scopus citations

Abstract

We examine ultrafast dynamics in a coupled molecule-plasmon system. Using a new ultrafast Raman technique called surface enhanced-femtosecond stimulated Raman spectroscopy (SE-FSRS), we prove that plasmonic nanoparticles and adsorbed molecules are coupled by the appearance of Fano-like lineshapes, which arise from the interaction of narrowband vibrational coherences and the broadband plasmon resonance. We probe the effect of plasmon energy on the vibrational lineshapes and observe changes in the phase of the line shape dispersion. Finally, we examine the effect of plasmon-molecule coupling on the molecular vibrational coherence lifetime. Surprisingly, coupling of the molecular vibration to the plasmon does not significantly shorten the vibrational coherence dephasing time. Better understanding of the ultrafast dynamics of excited vibrational states and vibrational coherences in coupled molecular-plasmonic systems should assist in developing a mechanism-based view of plasmonically enhanced photovoltaic and photocatalytic systems.

Original languageEnglish (US)
Pages (from-to)5989-5994
Number of pages6
JournalNano letters
Volume12
Issue number11
DOIs
StatePublished - Nov 14 2012

Keywords

  • Plasmonics
  • femtosecond stimulated Raman spectroscopy
  • molecule-plasmon interactions
  • surface-enhanced Raman scattering
  • vibrational coherence lifetimes

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