Repository logo

Infoscience

  • English
  • French
Log In
Logo EPFL, École polytechnique fédérale de Lausanne

Infoscience

  • English
  • French
Log In
  1. Home
  2. Academic and Research Output
  3. Journal articles
  4. Molecular cavity optomechanics as a theory of plasmon-enhanced Raman scattering
 
research article

Molecular cavity optomechanics as a theory of plasmon-enhanced Raman scattering

Roelli, Philippe  
•
Galland, Christophe  
•
Piro, Nicolas  
Show more
2015
Nature Nanotechnology

The exceptional enhancement of Raman scattering by localized plasmonic resonances in the near field of metallic nanoparticles, surfaces or tips (SERS, TERS) has enabled spectroscopic fingerprinting down to the single molecule level. The conventional explanation attributes the enhancement to the subwavelength confinement of the electromagnetic field near nanoantennas. Here, we introduce a new model that also accounts for the dynamical nature of the plasmon-molecule interaction. We thereby reveal an enhancement mechanism not considered before: dynamical backaction amplification of molecular vibrations. We first map the system onto the canonical Hamiltonian of cavity optomechanics, in which the molecular vibration and the plasmon are parametrically coupled. We express the vacuum optomechanical coupling rate for individual molecules in plasmonic 'hot -spots' in terms of the vibrational mode's Raman activity and find it to be orders of magnitude larger than for microfabricated optomechanical systems. Remarkably, the frequency of commonly studied molecular vibrations can be comparable to or larger than the plasmon's decay rate. Together, these considerations predict that an excitation laser blue-detuned from the plasmon resonance can parametrically amplify the molecular vibration, leading to a nonlinear enhancement of Raman emission that is not predicted by the conventional theory. Our optomechanical approach recovers known results, provides a quantitative framework for the calculation of cross -sections, and enables the design of novel systems that leverage dynamical backaction to achieve additional, mode -selective enhancements. It also provides a quantum mechanical framework to analyse plasmon-vibrational interactions in terms of molecular quantum optomechanics.

  • Details
  • Metrics
Type
research article
DOI
10.1038/nnano.2015.264
Web of Science ID

WOS:000370769600014

Author(s)
Roelli, Philippe  
Galland, Christophe  
Piro, Nicolas  
Kippenberg, Tobias J.  
Date Issued

2015

Publisher

Nature Publishing Group

Published in
Nature Nanotechnology
Volume

11

Issue

2

Start page

164

End page

169

Editorial or Peer reviewed

NON-REVIEWED

Written at

EPFL

EPFL units
LPQM  
GR-GA  
Available on Infoscience
March 11, 2016
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/124831
Logo EPFL, École polytechnique fédérale de Lausanne
  • Contact
  • infoscience@epfl.ch

  • Follow us on Facebook
  • Follow us on Instagram
  • Follow us on LinkedIn
  • Follow us on X
  • Follow us on Youtube
AccessibilityLegal noticePrivacy policyCookie settingsEnd User AgreementGet helpFeedback

Infoscience is a service managed and provided by the Library and IT Services of EPFL. © EPFL, tous droits réservés