Plasmonic dimer cavities can induce extreme electric-field hot spots that allow one to access ultrastrong coupling regimes using Raman-type spectroscopy on single vibrating molecules. Using a generalized master equation, we study resonant Raman scattering in the strong coupling regime of cavity quantum electrodynamics, when also in the vibrational ultrastrong coupling regime, leading to “phonon-dressed polaritons.” The master equation rigorously includes spectral baths for the cavity and vibrational degrees of freedom, as well as a pure dephasing bath for the resonant two-level system, which play a significant role. Employing realistic parameters for gold dimer cavity modes, we investigate the emission spectra in several characteristic strong coupling regimes, leading to extremely rich spectral resonances due to an interplay of phonon-modified polariton states and bath-induced resonances. We also show explicitly the failure of the standard master equation in these quantum nonlinear regimes.

Resonant Raman scattering of single molecules under simultaneous strong cavity coupling and ultrastrong optomechanical coupling in plasmonic resonators: Phonon-dressed polaritons

Settineri A.;Savasta S.;
2021

Abstract

Plasmonic dimer cavities can induce extreme electric-field hot spots that allow one to access ultrastrong coupling regimes using Raman-type spectroscopy on single vibrating molecules. Using a generalized master equation, we study resonant Raman scattering in the strong coupling regime of cavity quantum electrodynamics, when also in the vibrational ultrastrong coupling regime, leading to “phonon-dressed polaritons.” The master equation rigorously includes spectral baths for the cavity and vibrational degrees of freedom, as well as a pure dephasing bath for the resonant two-level system, which play a significant role. Employing realistic parameters for gold dimer cavity modes, we investigate the emission spectra in several characteristic strong coupling regimes, leading to extremely rich spectral resonances due to an interplay of phonon-modified polariton states and bath-induced resonances. We also show explicitly the failure of the standard master equation in these quantum nonlinear regimes.
File in questo prodotto:
Non ci sono file associati a questo prodotto.
Pubblicazioni consigliate

Caricamento pubblicazioni consigliate

I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/11570/3212288
 Attenzione

Attenzione! I dati visualizzati non sono stati sottoposti a validazione da parte dell'ateneo

Citazioni
  • ???jsp.display-item.citation.pmc??? ND
  • Scopus 1
  • ???jsp.display-item.citation.isi??? 0
social impact