Designing magnetic properties in CrSBr through hydrostatic pressure and ligand substitution

The ability to control magnetic material properties is crucial for fundamental research and underpins many information technologies. Two-dimensional materials are a particularly exciting platform due to their high degree of tunability and ease of implementation into nanoscale devices. Here we report two approaches for manipulating the A-type antiferromagnetic properties of the layered semiconductor CrSBr through hydrostatic pressure and ligand substitution. Hydrostatic pressure compresses the unit cell, continuously decreasing the Néel temperature and increasing all saturation fields. Ligand substitution, realized synthetically through Cl alloying, decreases the Néel temperature and all saturation fields, and also decreases the magnetocrystalline anisotropy energy. A detailed structural analysis combined with first-principles calculations reveal alterations in magnetic properties are intricately related to changes in Cr-Cr distances and the Cr-halogen superexchange pathway. Our work demonstrates opportunities for pre- and post-synthetic design of magnetism in this class of ternary layered magnetic semiconductors and suggests routes for enhancing magnetic order.