Nonlinear van der Waals Metasurfaces with Resonantly Enhanced Light Generation

Efficient nonlinear wave mixing is of paramount importance for a wide range of applications. However, weak optical nonlinearities pose significant challenges for accessing nonlinear light–matter interaction in compact systems. Here, we experimentally study second harmonic generation in deeply subwavelength 3R-MoS₂ metasurfaces (<λ/13 thick). Our measurements, supported by theoretical analysis, reveal a complex interplay and coupling between geometric resonances, optical extinction, and exciton-driven strong nonlinear susceptibility dispersion. We further demonstrate >150-fold enhancement in second harmonic signal at 740 nm mediated by the A exciton resonance. Additionally, our theoretical studies predict an enhancement of more than 10⁶ in second harmonic generation in <100 nm thick structures exhibiting bound states in the continuum resonance. These findings provide insight into accessing and harnessing the unprecedented 3R-MoS₂ nonlinearities at a subwavelength scale, paving the way to ultracompact nonlinear photonic devices.