Augmenting photoluminescence of monolayer MoS₂ using high order modes in a metal dimer-on-film nanocavity

Plasmonic particle-on-film nanocavities, supporting gap modes with ultra-small volume, provide a great solution to boost light–matter interactions at the nanoscale. In this work, we report on the photoluminescence (PL) enhancement of monolayer MoS₂ using high order modes of an Au nanosphere dimer-on-film nanocavity (DoFN). The high order plasmon modes, consisting of two bonding quadrupoles in the dimer and their images in the Au film, are revealed by combining the polarization-resolved scattering spectra with the numerical simulations. Further integrating the monolayer MoS₂ into the DoFN, these high order modes are used to enhance PL intensity through simultaneously boosting the absorption and emission processes, producing a 1350-fold enhancement factor. It opens an avenue to enhance the light–matter interaction with high order plasmon modes and may find applications in future optoelectronics and nanophotonics devices.