Optical Introduction and Manipulation of Plasmon-Exciton-Trion Coupling in a Si/WS2/Au Nanocavity.

Strong plasmon-exciton coupling, which has potential applications in nanophotonics, plasmonics, and quantum electrodynamics, has been successfully demonstrated by using metallic nanocavities and two-dimensional materials. Dynamical control of plasmon-exciton coupling strength, especially by using optical methods, remains a big challenge although it is highly desirable. Here, we report the optical introduction and manipulation of plasmon-exciton-trion coupling realized in a dielectric-metal hybrid nanocavity, which is composed of a silicon (Si) nanoparticle and a thin gold (Au) film, with an embedded tungsten disulfide (WS2) monolayer. We employ scattering and photoluminescence spectra to characterize the coupling strength between plasmons and excitons in Si/WS2/Au nanocavities constructed by using Si nanoparticles with different diameters. We enhance the plasmon-exciton and plasmon-trion coupling strength by injecting excitons and trions into the WS2 monolayer with a 488 nm laser beam. It is revealed that the emission intensities of excitons and trions with respect to the reference WS2 monolayer can be modified through the change in the coupling strength induced by the laser light. Interestingly, the coupling strength between the plasmons and the excitons/trions can be manipulated from weak to strong coupling regime by simply increasing the laser power, which is clearly resolved in the scattering spectra of Si/WS2/Au nanocavities. More importantly, the plasmon-exciton-trion coupling induced by the laser light is confirmed by the energy exchange between excitons and trions. Our findings indicate the possibility for optically manipulating plasmon-exciton interaction and suggest the practical applications of dielectric-metal hybrid nanocavities in nanoscale plasmonic devices.