Suppressed Quenching and Strong-Coupling of Purcell-Enhanced Single-Molecule Emission in Plasmonic Nanocavities

An emitter in the vicinity of a metal nanostructure is quenched by its decay through nonradiative channels, leading to the belief in a zone of inactivity for emitters placed within <10 nm of a plasmonic nanostructure. Here we demonstrate and explain why in tightly coupled plasmonic resonators forming nanocavities “quenching is quenched” due to plasmon mixing. Unlike isolated nanoparticles, such plasmonic nanocavities show mode hybridization, which can massively enhance emitter excitation and decay via radiative channels, here experimentally confirmed by laterally dependent emitter placement through DNA-origami. We explain why this enhancement of excitation and radiative decay can be strong enough to facilitate single-molecule strong coupling, as evident in dynamic Rabi-oscillations.