分类: 光学 >> 量子光学 提交时间: 2023-02-19
摘要: In this article, we address fluorescence of single molecule inside a plasmonic picocavity by proposing a semi-classical theory via combining the macroscopic quantum electrodynamics theory and the open quantum system theory. To gain insights into the experimental results [Nat. Photonics, 14, 693 (2020)], we have further equipped this theory with the classical electromagnetic simulation of the pico-cavity, formed by single atom decorated silver STM tip and a silver substrate, and the time-dependent density functional theory calculation of zinc phthalocyanine molecule. Our simulations not only reproduce the fluorescence spectrum as measured in the experiment, confirming the influence of extreme field confinement afforded by the picocavity, but also reveal Rabi oscillation dynamics and Mollow triplets spectrum for moderate laser excitation. Thus, our study highlights the possibility of coherently manipulating the molecular state and exploring non-linear optical phenomena with the plasmonic picocavity.
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.
分类: 光学 >> 量子光学 提交时间: 2023-02-19
摘要: Free-space optical communication (FSO) can achieve fast, secure and license-free communication without need for physical cables, making it a cost-effective, energy-efficient and flexible solution when the fiber connection is absent. To establish FSO connection on-demand, it is essential to build portable FSO devices with compact structure and light weight. Here, we develop a miniaturized FSO system and realize 9.16 Gbps FSO between two nodes that is 1 km apart, using a commercial fiber-coupled optical transceiver module with no optical amplification. Basing on the home-made compact 90 mm-diameter acquisition, pointing and tracking (APT) system with four-stage close-loop feedback, the link tracking error is controlled at 3 {\mu}rad and results an average coupling loss of 13.7 dB. Such loss is within the tolerance of the commercial optical communication modules, and without the need of optical amplifiers, which contributes to the low system weight and power consumption. As a result, a single FSO device weighs only about 12 kg, making it compact and portable for potential application in high-speed wireless communication. Our FSO link has been tested up to 4 km, with link loss of 18 dB in the foggy weather in Nanjing, that shows longer distances can be covered with optical amplification.