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ACS Nano. 2016 Jun 28;10(6):6291-8. doi: 10.1021/acsnano.6b02484. Epub 2016 May 31.

Quantum Mechanical Description of Raman Scattering from Molecules in Plasmonic Cavities.

Author information

1
Materials Physics Center CSIC-UPV/EHU, Paseo Manuel de Lardizabal 5, 20018 Donostia-San Sebastián, Spain.
2
Donostia International Physics Center DIPC, Paseo Manuel de Lardizabal 4, 20018 Donostia-San Sebastián, Spain.
3
Max-Planck-Institut für Quantenoptik, Hans-Kopfermann-Strauße 1, 85748 Garching, Germany.
4
IKERBASQUE, Basque Foundation for Science, Maria Diaz de Haro 3, 48013 Bilbao, Spain.

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.

KEYWORDS:

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

PMID:
27203727
DOI:
10.1021/acsnano.6b02484

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