分类: 光学 >> 量子光学 提交时间: 2023-02-19
摘要: Plasmon-mediated superradiance for molecules around metallic nanospheres was proposed ten years ago. However, its demonstration has not been achieved yet due to the experimental difficulty of positioning molecules, and the theoretical limitation to the enhanced collective rate of low excited molecules. In this Letter, we propose that the ultrafast plasmon-mediated superradiant pulses can be observed with strongly excited methylene blue molecules standing vertically inside gold nanoparticle-on-mirror nanocavities. Our simulations indicate that in this system the molecules could interact with each other via plasmon- and free-space mediated coherent and dissipative coupling. More importantly, the coherent coupling mediated by short-ranged propagating surface plasmons cancel largely the direct dipole-dipole coupling mediated by the free-space field, and the dominated dissipative coupling mediated by relatively long-ranged gap plasmons enables the ultrafast superradiant pulses within picosecond scale. Our study opens up the possibility of studying the rich superradiant effects from the quantum emitters in a sub-wavelength volumn by engineering the plasmonic environments.
分类: 光学 >> 量子光学 提交时间: 2023-02-19
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.