Strong coupling with directional scattering features of metal nanoshells with monolayer WS2 heterostructures

Realizing and manipulating strong light–matter coupling in 2D monolayer semiconductors are of the utmost importance in the development of photonic devices. Hollow nanostructures of noble metals are particularly interesting because of their stronger local electromagnetic field compared with solid nanoparticles, which facilitate the strong coupling of single metal nanostructures. Here, the tunable single nanocavity plasmon–exciton coupling was demonstrated at room temperature in hybrid systems consisting of Ag@Au hollow nanocubes (HNCs) and monolayer WS2 underneath, where a large vacuum Rabi splitting of 131.3 meV was observed. Mode splitting can be clearly observed from the dark-field scattering spectrum of the single hybrid nanocavity, which is ascribed to the strong coupling between the nanocavity mode and the excitonic mode. Then, we used the finite difference time domain method to simulate these hybrid systems. By changing the thickness of the shell of the Ag@Au HNC, we can tune the surface plasmon resonance peak position of HNCs to match the exciton energy of the monolayer WS2. The strong couplings were realized via the calculated scattering spectra. The calculated results were consistent with the experimental results. Furthermore, the mode volume of different nanostructures was discussed, and the mode volume of HNCs is smaller than other solid ones at the same plasmonic resonance wavelength, which also indicates that its ability to restrict an electromagnetic field is stronger. This study provides an ideal platform for the strong coupling of a single nanocavity at room temperature and has broad application prospects in the field of single-photon devices.