title: Quantum Mechanical Description of Raman Scattering from Molecules in Plasmonic Cavities.
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.
authors.affiliation: Materials Physics Center CSIC-UPV/EHU, Paseo Manuel de Lardizabal 5, 20018 Donostia-San Sebastián, Spain.|Donostia International Physics Center DIPC, Paseo Manuel de Lardizabal 4, 20018 Donostia-San Sebastián, Spain.
authors.forename: Mikolaj K
authors.initials: MK
authors.lastname: Schmidt
authors.affiliation: Donostia International Physics Center DIPC, Paseo Manuel de Lardizabal 4, 20018 Donostia-San Sebastián, Spain.
authors.forename: Ruben
authors.initials: R
authors.lastname: Esteban
authors.affiliation: Max-Planck-Institut für Quantenoptik, Hans-Kopfermann-Strauße 1, 85748 Garching, Germany.
authors.forename: Alejandro
authors.initials: A
authors.lastname: González-Tudela
authors.affiliation: Donostia International Physics Center DIPC, Paseo Manuel de Lardizabal 4, 20018 Donostia-San Sebastián, Spain.|IKERBASQUE, Basque Foundation for Science, Maria Diaz de Haro 3, 48013 Bilbao, Spain.
authors.forename: Geza
authors.initials: G
authors.lastname: Giedke
authors.affiliation: Materials Physics Center CSIC-UPV/EHU, Paseo Manuel de Lardizabal 5, 20018 Donostia-San Sebastián, Spain.|Donostia International Physics Center DIPC, Paseo Manuel de Lardizabal 4, 20018 Donostia-San Sebastián, Spain.
authors.forename: Javier
authors.initials: J
authors.lastname: Aizpurua
keywords: Raman scattering; SERS; Stokes emission; plasmonics; quantum electrodynamics; quantum nanooptics