All-optical switching of nonlinear structured light in crystal-engineered van der Waals materials

Abstract

The orbital angular momentum (OAM) of light is a discrete, unbounded degree of freedom that underpins mode-multiplexed communications and high-dimensional quantum photonics. Yet, dynamic OAM control remains dependent on bulky free-space optics or cascaded architectures that separate switching from wavefront shaping, hindering nanoscale integration. Here, we engineer artificial van der Waals crystals from rhombohedrally stacked (3R) MoS$_2$, in which spatial control of the local crystal orientation imprints a nonlinear geometric phase onto the second-harmonic (SH) field, enabling background-free generation of SH vortex beams in an ultrathin (46 nm) van der Waals platform. Leveraging the C$_{3v}$ symmetry of 3R-MoS$_2$, we demonstrate monolithic, all-optical switching with sub-optical-cycle precision between Hermite-Gauss-like and Laguerre-Gaussian vortex SH beams with opposite topological charges ($l=\pm1$). Our results establish artificial 3R-MoS$_2$ crystals as a monolithic platform for the generation and all-optical reconfiguration of nonlinear structured light at the nanoscale, advancing active nanophotonic sources for integrated classical and quantum photonic technologies.