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In this article, we address fluorescence of single molecule inside aplasmonic picocavity by proposing a semi-classical theory via combining themacroscopic 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 classicalelectromagnetic simulation of the pico-cavity, formed by single atom decoratedsilver STM tip and a silver substrate, and the time-dependent densityfunctional theory calculation of zinc phthalocyanine molecule. Our simulationsnot only reproduce the fluorescence spectrum as measured in the experiment,confirming the influence of extreme field confinement afforded by thepicocavity, but also reveal Rabi oscillation dynamics and Mollow tripletsspectrum for moderate laser excitation. Thus, our study highlights thepossibility of coherently manipulating the molecular state and exploringnon-linear optical phenomena with the plasmonic picocavity.

Picocavity-controlled Sub-nanometer Resolved Single Molecule Non-linear Fluorescence