QED 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 \textit{phonon-stimulated Raman scattering} and an counter-intuitive dependence of the anti-Stokes emission on the frequency of excitation. We further show that this novel QED framework opens a venue to analyze the correlations of photons emitted at a plasmonic cavity
Keywords
Cite
@article{arxiv.1509.03851,
title = {QED description of Raman scattering from molecules in plasmonic cavities},
author = {Mikolaj K. Schmidt and Ruben Esteban and Alejandro Gonzalez-Tudela and Geza Giedke and Javier Aizpurua},
journal= {arXiv preprint arXiv:1509.03851},
year = {2016}
}
Comments
We add the discussion of the quantum noise treatment to the main text, correct equations in the SI and amend the discussion of the processes yield strong Stokes/anti-Stokes correlations