Enhanced Photo-excitation and Angular-Momentum Imprint of Gray Excitons in WSe2 Monolayers by Spin–Orbit-Coupled Vector Vortex Beams

A light beam can be spatially structured in the complex amplitude to possess orbital angular momentum (OAM), which introduces an extra degree of freedom alongside the intrinsic spin angular momentum (SAM) associated with circular polarization. Furthermore, superimposing two such twisted light (TL) beams with distinct SAM and OAM produces a vector vortex beam (VVB) in nonseparable states where not only complex amplitude but also polarization is spatially structured and entangled with each other. In addition to the nonseparability, the SAM and OAM in a VVB are intrinsically coupled by the optical spin–orbit interaction and constitute the profound spin–orbit physics in photonics. In this work, we present a comprehensive theoretical investigation, implemented on the first-principles base, of the intriguing light–matter interaction between VVBs and WSe2 monolayers (WSe2-MLs), one of the best-known and promising two-dimensional (2D) materials in optoelectronics dictated by excitons, encompassing bright exciton (BX) as well as various dark excitons (DXs). One of the key findings of our study is that a substantial enhancement of the photoexcitation of gray excitons (GXs), a type of spin-forbidden DX, in a WSe2-ML can be achieved through the utilization of a 3D-structured TL with the optical spin–orbit interaction. Moreover, we show that a spin–orbit-coupled VVB surprisingly allows for the imprinting of the carried optical information onto GXs in 2D materials, which is robust against the decoherence mechanisms in the materials. This suggests a promising method for deciphering the transferred angular momentum from structured light to excitons.