2D‐Material‐Fused High‐Emittance Plasmo–Photonic Metasurfaces

Abstract Transition metal dichalcogenides (TMDC) are a family of atomic‐layer 2D materials (2dMs). Many researches have attempted to reinforce the unique properties by incorporating artificially designed nanostructures. Here, a highly photoluminescence (PL) enhancing platform is reported that is formed by combining high‐emittance plasmo–photonic metasurfaces with a large‐area 2dM, which is a continuous monolayer of TMDC of cm² dimension. It is experimentally demonstrated that the 2dM‐PL intensity at room temperature is enhanced by more than 1030‐fold in comparison with that observed on the flat gold film regions. The enhancement is associated with spectral transformation indicating a resonant effect of the metasurfaces. It is moreover revealed that the confocal PL image originates from a coherent single‐mode emission that forms a photon number distribution obeying the Poisson probability distribution. Thus, the 2dM‐fused metasurfaces function as efficient coherent quantum light sources. PL decay‐time analysis also reveals the coexistence of two components in the enhanced PL. The fast component exhibits a lifetime of 18 ps whereas the slow component decays at 4.4 ns. Both components are most likely to undergo radiative processes, which indicates that metal‐induced PL quenching is suppressed on these 2dM‐fused metasurfaces. The long lifetime component is ascribed to an excitonic intervalley transition.