Engineering magnetism in a 2D magnet from first principles

Among the family of two-dimensional (2D) materials, 2D van der Waals (vdW) magnetic semiconductors exhibit many novel properties resulting from the weak yet tunable interlayer magnetic interaction, which adds an entirely new magnetic degree of freedom to vdW interfacial engineering. As a prototypical 2D vdW magnetic semiconductor, layered CrSBr is ferromagnetic within each layer, and antiferromagnetically coupled between neighboring layers. In this talk, we demonstrate using first-principles calculations that a variety of tuning knobs, such as external magnetic field, strain, pressure, doping, and stacking configurations, can act as control knobs to engineer electronic and excitonic properties by changing the underlying magnetism in this material. We further map these tuning knobs onto a high-dimensional parameter space, in which the variables can be continuous or categorical. Our work establishes a systematic approach to engineer magnetic phases in layered magnetic semiconductors, which opens up opportunities for spintronic and memory devices based on 2D magnetic materials.