Anisotropic electron-hole excitation and large linear dichroism in the two-dimensional ferromagnet CrSBr with in-plane magnetization

The observation of magnetic ordering in atomically thin CrI3 and Cr2Ge2Te6 monolayers has aroused intense interest in condensed-matter physics and material science. Studies of van de Waals two-dimensional (2D) magnetic materials are of both fundamental importance and application interest. In particular, exciton-enhanced magneto-optical properties revealed in CrI3 and CrBr3 monolayers have expanded the understanding of exciton physics in 2D materials. Unlike CrI3 and CrBr3, with out-of-plane magnetization, CrSBr has an in-plane magnetic moment, therefore providing a good opportunity to study the magnetic linear dichroism and high-order magneto-optical effects. Here, based on the many-body perturbation method within density-functional theory, we have studied quasiparticle electronic structure, exciton, and optical properties in CrSBr monolayer. A strongly bounded exciton has been identified with the first bright exciton located at 1.35 eV, in good agreement with an experiment of photoluminescence [Wilson, Nat. Mater. 20, 1657 (2021)1476-112210.1038/s41563-021-01070-8]. Strong contrast in the optical absorption is found between the electric fields lying along the in-plane two orthogonal directions. In accordance with a typical and realistic experimental setup, we show that the rotation angle of linear polarized light, either reflected or transmitted, could be comparable with those revealed in black phosphorene. Such large linear dichroism arises mainly from the anisotropic in-plane crystal structure. The magnetic contribution from the off-diagonal component of dielectric function to the linear dichroism in CrSBr is negligible. Our findings not only have revealed the excitonic effect on the optical and magneto-optical properties in 2D ferromagnet CrSBr, but also have shown its potential applications in 2D optics and optoelectronics. © 2023 authors. Published by the American Physical Society. Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.