Anisotropic Electron-Hole Excitation and Large Linear Dichroism in Two-Dimensional Ferromagnet CrSBr with In-Plane Magnetization

Abstract

The observation of magnetic ordering in atomically thin CrI${}_3$ and Cr${}_2$Ge${}_2$Te${}_6$ 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 CrI${}_3$ and CrBr${}_3$ monolayers have expanded the understanding of exciton physics in 2D materials. Unlike CrI${}_3$ and CrBr${}_3$ 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. Strongly bounded exciton has been identified with the first bright exciton located at 1.35 eV, in good agreement with an experiment of photoluminescence (Nat. Mater. \textbf{20}, 1657 (2021)). 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 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 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.

47 pages, 24 figures

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• Doping-control of excitons and magnetism in few-layer CrSBr
• Raman Polarization Switching in CrSBr
• Distinct Magneto-Optical Response of Frenkel and Wannier Excitons in CrSBr
• Magnetic Correlation Spectroscopy in CrSBr
• Excitonic optical absorption in strained monolayer CrSBr