Ultrasmall Mode Volumes in Plasmonic Cavities of Nanoparticle‐On‐Mirror Structures

The mode volume and Purcell factor are two important parameters to assess the performance of optical nanocavities. Achieving small mode volumes and high Purcell factors for nanocavity structures while simplifying their fabrication has been a major task to realize high‐performance and large‐scale photonic devices and systems. Different optical resonators based on nanoparticle‐on‐mirror (NPoM) structures are systematically analyzed, which are easy to fabricate and flexible to use. Direct comparison of these optical resonators is made through finite‐difference time‐domain (FDTD) simulations. The achievement of ultrasmall mode volumes below 10^?7 based on the NPoM structure through FDTD simulations is demonstrated by rationally selecting the structural parameters. Such NPoM structures provide a decent Purcell factor on the order of 10⁷, which can effectively enhance spontaneous emission and facilitate a number of photonic applications. The simulation results are confirmed by dark field scattering and second‐harmonic generation measurements. This work is scientifically important and offers practical guidelines for the design of optical resonators for state‐of‐the‐art optical and photonic devices.