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A light beam can be spatially structured in the complex amplitude to possessorbital angular momentum (OAM), which introduces a new degree of freedomalongside the intrinsic spin angular momentum (SAM) associated with circularpolarization. Moreover, super-imposing two twisted lights with distinct SAM andOAM produces a vector vortex beam (VVB) in non-separable states where not onlycomplex amplitude but also polarization are spatially structured and entangledwith each other. In addition to the non-separability, the SAM and OAM in a VVBare intrinsically coupled by the optical spin-orbit interaction and constitutethe profound spin-orbit physics in photonics. In this work, we present acomprehensive theoretical investigation, implemented on the first-principlesbase, of the intriguing light-matter interaction between VVBs and WSe$_{2}$monolayers (WSe$_{2}$-MLs), one of the best-known and promising two-dimensional(2D) materials in optoelectronics dictated by excitons, encompassing brightexciton (BX) as well as various dark excitons (DXs). One of the key findings ofour study is the substantial enhancement of the photo-excitation of grayexcitons (GXs), a type of spin-forbidden dark exciton, in a WSe$_2$-ML throughthe utilization of a twisted light that possesses a longitudinal fieldassociated with the optical spin-orbit interaction. Our research demonstratesthat a spin-orbit-coupled VVB surprisingly allows for the imprinting of thecarried optical information onto gray excitons in 2D materials, which is robustagainst the decoherence mechanisms in materials. This observation suggests apromising method for deciphering the transferred angular momentum fromstructured lights to excitons.

Enhanced photo-excitation and angular-momentum imprint of gray excitons in WSe$_{2}$ monolayers by spin-orbit-coupled vector vortex beams