Giant enhancement of optical nonlinearity from monolayer MoS₂ using plasmonic nanocavity

The particle-on-mirror nanocavity, supporting multiple plasmonic resonances, provides an ideal platform to efficiently boost the nonlinear optical processes at the nanoscale. Here, we report on the enhancement of the second (SHG) and third-harmonic generations (THG) from the monolayer MoS2 using a multi-resonant Au nanosphere dimer-on-mirror nanocavity (DoMN). The strong plasmon hybridization between the dimer and underlying Au substrate leads to the emergence of two distinct cavity modes, which are intentionally aligned with the SH and TH frequencies, rendering a 15- and 68-fold enhancement for the SHG and THG of the monolayer MoS2, respectively. Further theoretical analysis yields that these remarkable nonlinearity enhancements are also ascribed to the amplification of nonlinear source because of the excellent spatial mode overlap and the high directivity of nonlinear emission enabled by the cavity modes. Our results pave the way for the implementation of low-cost, and highly efficient nonlinear photonics devices integrated with plasmonic nanocavities.