Probing intensity-field correlations of single-molecule surface-enhanced Raman-scattered light

Abstract

In the context of the quantum-mechanical description of single-molecule surface-enhanced Raman scattering, intensity-field correlation measurements of photons emitted from a plasmonic cavity are explored, theoretically, using the technique of conditional homodyne detection. The inelastic interplay between plasmons and vibrations of a diatomic molecule placed inside the cavity can be manifested in phase-dependent third-order fluctuations of the light recorded by the aforesaid technique, allowing us to reveal signatures of non-classicality (indicatives of squeezing) of the outgoing Raman photons.

Phase-dependent fluctuations of resonance fluorescence near the coherent population trapping condition

“…asymmetry was readily observed for cavity QED systems both numerically [14,19] and experimentally [15], it has been the resonance fluorescence of several 3LA systems that have provided clear theoretical access to the understanding of the asymmetry [21][22][23][24][25][26]. More recent accounts of asymmetric correlations are found in plasmonics [27] and collective cavity QED [28].…”

Phase-dependent fluctuations of resonance fluorescence near the coherent population trapping condition

“…While this asymmetry was readily observed for cavity QED systems both numerically [14,19] and experimentally [15], it has been the resonance fluorescence of several 3LA systems that have provided clear theoretical access to the understanding of the asymmetry [21][22][23][24][25][26]. More recent accounts of asymmetric correlations are found in plasmonics [27] and collective cavity QED [28].…”

A comparison ofg(1)(τ),g(3/2)(τ), andg(2)(τ) for radiation from harmonic oscillators in Brownian motion with a coherent background

“…It would seem that a correlation of three fields would not give any further information, but strictly speaking, there are three fields from the source and one from a local oscillator that cancels out in the normalized definition, giving access to such intensity-field correlation that probes the field quadrature fluctuations. Recent investigations now include the study of Raman scattering of molecules on surfaces [31]. The paper by Xu et al [32] summarizes the motivation for the development of the intensity-field correlation function as a tool to study conditional dynamics in quantum optics.…”