Ultrafast all-optical switching in nonlinear 3R-MoS${}_2$ van der Waals metasurfaces

Second-order nonlinear optical processes are fundamental to photonics, spectroscopy, and information technologies, with material platforms playing a pivotal role in advancing these applications. Here, we demonstrate the exceptional nonlinear optical properties of the van der Waals crystal 3R-MoS${}_2$, a rhombohedral polymorph exhibiting high second-order optical susceptibility (${\chi }^{(2)}$) and remarkable second-harmonic generation (SHG) capabilities. By designing high quality factor resonances in 3R-MoS${}_2$ metasurfaces supporting quasi-bound states in the continuum (qBIC), we first demonstrate SHG efficiency enhancement exceeding 10${}^2$. Additionally, by using degenerate pump-probe spectroscopy, we harness the C${}_{3v}$ system’s symmetry to realize ultrafast SHG polarization switching with near-unity modulation depth. The operation speeds are limited only by the excitation pulse duration, allowing its characterization via the nonlinear autocorrelation function. These findings establish 3R-MoS${}_2$ as a transformative platform for nanoscale nonlinear optics, offering large conversion efficiencies and ultrafast response times for advanced pulse measurement devices, integrated photonics, and quantum technologies.