Precise Crystal Orientation Identification and Twist-Induced Giant Modulation of Optical Anisotropy in 1T'-ReS₂

The ability to precisely identify crystal orientation as well as to nondestructively modulate optical anisotropy in atomically thin rhenium dichalcogenides is critical for the future development of polarization programmable optoelectronic devices, which remains challenging. Here, we report a modified polarized optical imaging (POI) method capable of simultaneously identifying in-plane (Re chain) and out-of-plane (c-axis) crystal orientations of the monolayer to few-layer ReS₂, meanwhile, propose a nondestructive approach to modulate the optical anisotropy in ReS₂ via twist stacking. The results show that parallel and near-cross POI are effective to independently identify the in-plane and out-of-plane crystal orientations, respectively, while regulating the twist angle allows for giant modulation of in-plane optical anisotropy from highly intrinsic anisotropy to complete optical isotropy in the stacked ReS₂ bilayer (with either the same or opposite c-axes), as well modeled by linear electromagnetic theory. Overall, this study not only develops a simple optical method for precise crystal orientation identification but also offers an efficient light polarization control strategy, which is a big step toward the practical application of anisotropic van der Waals materials in the design of nanophotonic and optoelectronic devices.