Magnetic pair distribution function analysis of the 2D layered material CrPS₄

Two-dimensional layered materials, characterized by weak van der Waals bonds between the layers in the bulk material, showcase the potential for distinct quantum behaviors and hold promise for applications in spintronics. Among these 2D materials, CrPS₄ is gaining considerable attention in the scientific community due to its magnetic and semiconducting properties. The 2D layers in CrPS₄ are weakly bound with van der Waals forces, suggesting possibilities for exfoliating it to monolayer or few-layer structures. CrPS₄ is an antiferromagnet with a Néel temperature of 36 K and an unusual two-stage magnetic transition. Within the 2D layers, the Cr spins couple ferromagnetically and these 2D layers are antiferromagnetically arranged along the c- direction. In this study, we performed detailed neutron total scattering measurements to access the magnetic and structural behavior. Specifically, we adopted the atomic and magnetic pair distribution function (mPDF) technique to undertake an analysis of the local structural and magnetic behavior of CrPS₄. We will discuss these results that follow the magnetism from the long-range ordered phase through to the short-range ordering above the Néel temperature.