Plexciton Photoluminescence in Strongly Coupled 2D Semiconductor–Plasmonic Nanocavity Hybrid

Strong plasmon-exciton interaction between two-dimensional transition metal dichalcogenides and a plasmonic nanocavity under ambient conditions has been reported extensively. But the suspicion on whether it has reached a true "strong coupling" is always there because the commonly used dark-field scattering spectroscopy shows a larger spectral splitting and the splitting in the photoluminescence spectra is absent. Here, by using a nanobipyramid-over-mirror to enhance the in-plane vacuum field, we achieve spectral Rabi splitting in both scattering and differential reflection spectra and observe a clear photoluminescence emission of the lower plexciton branch. The established nanocavity offers two polarization-dependent gap plasmon resonances to provide excitation and quantum yield enhancement simultaneously, yielding a total photoluminescence enhancement of 2.1 × 104 times. This allows the acquisition of emission spectra from an individual coupled system regardless of the presence of an uncoupled emitting background in the collection area. The sharp tips of the nanobipyramid lead to a large single-exciton coupling strength up to a few meV. Correlated scattering, differential reflection, and photoluminescence spectra reveal the similarity between the scattering and normalized photoluminescence spectra. These correlative measurements on a single coupled system clear up the suspicions of strong plasmon-exciton interactions and will promote the development of light-emitting plexcitonic devices at room temperature.