Optomechanical Effects in Nanocavity-enhanced Resonant Raman Scattering of a Single Molecule

分类： 光学 >> 量子光学 提交时间： 2023-02-19

Xuan-Ming Shen Yuan Zhang Shunping Zhang Yao Zhang Qiu-Shi Meng Guangchao Zheng Siyuan Lv Luxia Wang Roberto A. Boto Chongxin Shan Javier Aizpurua

摘要： 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.

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