Efficient DNA-Driven Nanocavities for Approaching Quasi-Deterministic Strong Coupling to a Few Fluorophores

Strong coupling between light and matter is the foundation of promising quantum photonic devices such as deterministic single photon sources, single atom lasers, and photonic quantum gates, which consist of an atom and a photonic cavity. Unlike atom-based systems, a strong coupling unit based on an emitter-plasmonic nanocavity system has the potential to bring these devices to the microchip scale at ambient conditions. However, efficiently and precisely positioning a single or a few emitters into a plasmonic nanocavity is challenging. In addition, placing a strong coupling unit on a designated substrate location is a demanding task. Here, fluorophore-modified DNA strands are utilized to drive the formation of particle-on-film plasmonic nanocavities and simultaneously integrate the fluorophores into the high field region of the nanocavities. High cavity yield and fluorophore coupling yield are demonstrated. This method is then combined with e-beam lithography to position the strong coupling units on designated locations of a substrate. Furthermore, polariton energy under the detuning of fluorophore embedded nanocavities can fit into a model consisting of three sets of two-level systems, implying vibronic modes may be involved in the strong coupling. Our system makes strong coupling units more practical on the microchip scale and at ambient conditions and provides a stable platform for investigating fluorophore-plasmonic nanocavity interaction.