Enhanced second‐harmonic generation in monolayer MoS 2 on suspended metallic nanostructures by plasmonic resonances

Monolayer transition metal dichalcogenides (TMDs) possess large second‐order nonlinear responses due to the broken inversion symmetry, which can extend their intriguing applications in nonlinear nanophotonics and optoelectronics. However, the atomic thickness of monolayer TMDs severely decreases the interaction length with free light with respect to bulk materials, leading to rather low second‐harmonic generation (SHG) conversion efficiency. Here, we demonstrate a hybrid structure consisting of a monolayer MoS 2 on a suspended perforated silver film, on which the SHG signal emitted from the monolayer MoS 2 is enhanced by more than three orders of magnitude at room temperature. The pronounced SHG enhancement is attributed to the distinct electric field amplification nearby the nanoholes, which is induced by the symmetric surface plasmon polaritons (SPPs) existing in the ultrathin suspended silver grating. Our results reported here may establish the substrate‐free engineering of nonlinear optical effects via plasmonic nanostructures on demand.