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.