Quantum Mechanical Description of Raman Scattering from Molecules in Plasmonic Cavities

Mikolaj K. Schmidt*, Ruben Esteban, Alejandro González-Tudela, Geza Giedke, Javier Aizpurua

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

90 Citations (Scopus)

Abstract

Plasmon-enhanced Raman scattering can push single-molecule vibrational spectroscopy beyond a regime addressable by classical electrodynamics. We employ a quantum electrodynamics (QED) description of the coherent interaction of plasmons and molecular vibrations that reveal the emergence of nonlinearities in the inelastic response of the system. For realistic situations, we predict the onset of phonon-stimulated Raman scattering and a counterintuitive dependence of the anti-Stokes emission on the frequency of excitation. We further show that this QED framework opens a venue to analyze the correlations of photons emitted from a plasmonic cavity.

Original languageEnglish
Pages (from-to)6291-6298
Number of pages8
JournalACS Nano
Volume10
Issue number6
DOIs
Publication statusPublished - 28 Jun 2016
Externally publishedYes

Keywords

  • plasmonics
  • quantum electrodynamics
  • quantum nanooptics
  • Raman scattering
  • SERS
  • Stokes emission

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