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

TL;DR

This study uses first-principles calculations to show that twin-stacked CrSBr bilayers exhibit enhanced interlayer electronic coupling, which significantly affects excitonic and optical properties, depending on twist angle and spin alignment.

Contribution

It reveals the nonlinear and nonmonotonic dependence of interlayer coupling on twist angle and spin configuration in CrSBr bilayers, highlighting twin stacking as a tool for engineering 2D magnetic heterostructures.

Findings

Maximum interlayer coupling at twin-stacking configuration.

Excitons delocalized across layers with polarization sensitive to spin alignment.

Interlayer coupling depends on orbital overlap and spin angle.

Abstract

The degree of electronic coupling between individual layers in few-layer 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 gives rise to excitons delocalized across the two layers with a strong polarization dependence that reflects the details of the interlayer spin alignment. Our results reveal a sensitive interplay between twist angle, magnetism, and excitonic properties in twin-stacked CrSBr bilayers, and they establish twin stacking as an effective route to engineering interlayer coupling and optical response in anisotropic two-dimensional magnets with rectangular lattices.