Optomechanical Effects in Nanocavity-enhanced Resonant Raman Scattering of a Single Molecule
arXiv:2210.02639 · doi:10.1103/PhysRevB.107.075435
Abstract
In this article, we address the optomechanical effects in surface-enhanced resonant Raman scattering (SERRS) from a single molecule in a nano-particle on mirror (NPoM) nanocavity by developing a quantum master equation theory, which combines macroscopic quantum electrodynamics and electron-vibration interaction within the framework of open quantum system theory. We supplement the theory with electromagnetic simulations and time-dependent density functional theory calculations in order to study the SERRS of a methylene blue molecule in a realistic NPoM nanocavity. The simulations allow us not only to identify the conditions to achieve conventional optomechanical effects, such as vibrational pumping, non-linear scaling of Stokes and anti-Stokes scattering, but also to discovery distinct behaviors, such as the saturation of exciton population, the emergence of Mollow triplet side-bands, and higher-order Raman scattering. All in all, our study might guide further investigations of optomechanical effects in resonant Raman scattering.
arXiv comment15 pages; 9 figures
References in corpus (12)
- Cavity Optomechanics
- QuTiP 2: A Python framework for the dynamics of open quantum systems
- QuTiP: An open-source Python framework for the dynamics of open quantum systems
- Optical excitations in electron microscopy
- MNPBEM - A Matlab toolbox for the simulation of plasmonic nanoparticles
- Light-matter interactions with photonic quasiparticles
- Molecular cavity optomechanics: a theory of plasmon-enhanced Raman scattering
- Plasmonics simulations with the MNPBEM toolbox: Consideration of substrates and layer structures
- QED description of Raman scattering from molecules in plasmonic cavities
- Molecular optomechanics in the anharmonic cavity-QED regime using hybrid metal-dielectric cavity modes
- A new signature for strong light-matter coupling using spectroscopic ellipsometry
- Quantum description of surface-enhanced resonant Raman scattering within a hybrid-optomechanical model