Enhanced Interlayer Coupling and Excitons in Twin-Stacked Two-Dimensional Magnetic CrSBr Bilayers

The degree of electronic coupling between individual layers in van der Waals heterostructures offers a route to engineer their magnetic, electronic, and optical functionalities. Using state-of-the-art first-principles calculations, we demonstrate that the electronic coupling between two monolayers of CrSBr─an anisotropic two-dimensional magnetic semiconductor─is highly nonlinear and nonmonotonic with respect to their relative twist angle, exhibiting a pronounced maximum at the twin-stacking configuration. The coupling strength scales with both the degree of overlap of Br orbitals adjacent to the van der Waals gap and the cosine of half of the interlayer spin angle. This enhanced interlayer electronic coupling leads to excitons delocalized across the two layers, with a polarization dependence that reflects the interlayer spin alignment. Our results reveal a sensitive interplay among twist angle, magnetism, and excitonic properties in twin-stacked CrSBr bilayers, suggesting twin stacking as an effective means for engineering interlayer coupling.