Charge transfer and asymmetric coupling of MoSe${}_2$ valleys to the magnetic order of CrSBr

Abstract

Van der Waals (vdW) heterostructures composed of two-dimensional (2D) transition metal dichalcogenides (TMD) and vdW magnetic materials offer an intriguing platform to functionalize valley and excitonic properties in non-magnetic TMDs. Here, we report magneto-photoluminescence (PL) investigations of monolayer (ML) MoSe${}_2$ on the layered A-type antiferromagnetic (AFM) semiconductor CrSBr under different magnetic field orientations. Our results reveal a clear influence of the CrSBr magnetic order on the optical properties of MoSe${}_2$, such as an anomalous linear-polarization dependence, changes of the exciton/trion energies, a magnetic-field dependence of the PL intensities, and a valley $g$-factor with signatures of an asymmetric magnetic proximity interaction. Furthermore, first principles calculations suggest that MoSe${}_2$/CrSBr forms a broken-gap (type-III) band alignment, facilitating charge transfer processes. The work establishes that antiferromagnetic-nonmagnetic interfaces can be used to control the valley and excitonic properties of TMDs, relevant for the development of opto-spintronics devices.

14 pages, 4 figures

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• Magnetic Anisotropy in Two-dimensional van der Waals Magnetic Materials and Their Heterostructures: Importance, Mechanisms, and Opportunities
• Engineering robust strain transmission in van der Waals heterostructure devices
• Interplay of energy and charge transfer in WSe2/CrSBr heterostructures
• Symmetry Classification for Alternating Excitons in Two-Dimensional Altermagnets
• Tunable resonant s-p mixing of excitons in van der Waals heterostructures
• Effect of spin-dependent tunneling and intervalley scattering in magnetic-semiconductor van der Waals heterostructures on exciton and trion polarization