Steering Nonlinear Twisted Valley Photons of Monolayer WS₂ by Vector Beams

Monolayer transition metal dichalcogenides have intrinsic spin-valley degrees of freedom, drawing broad interests due to their potential applications in information storage and processing. Here, we demonstrate the possibility of using cylindrical vector pumped beams, which are nonseparable in their polarization and spatial modes, to manipulate nonlinear valley-locked twisted-vortex emissions in monolayer tungsten disulfide (WS₂). The second-harmonic (SH) photons from K and K' valleys are encoded with opposite optical vortices, thus allowing the SH beams to emerge as cylindrical vector beams with doubled topological orders compared to the fundamental beams. The conically refracted pumped beams allow us to generate the first-order SH cylindrical vector and full Poincaré beams via tuning the valley-locked emitted light field profiles. With fanshaped WS₂ films breaking the axial symmetry of SH beams, the SH valley photons are routed to opposite directions. Our results pave the way to develop atomically thin nonlinear photonic devices and valleytronic nanodevices.