Rediscovering Cr₂S₃ as Half-semiconducting Antiferromagnet

The promises of spintronics have longed for the realization of fully compensated states and full spin polarization. Half metallic/semiconducting and fully compensated materials are suggested as candidates. We use density functional theory to report that the experimentally realized rhombohedral Cr₂S₃ is a promising candidate as a half-semiconducting antiferromagnetic (HS-AFM) material. Our calculations demonstrate that the uniquely layered structure of Cr₂S₃ produces different interlayer and intralayer d-p-d hybridization schemes between Cr atoms. Strong interlayer and weak intralayer AFM coupling between different Cr sites make the overall magnetic state a fully compensated structure state. The origin of half-semiconducting and fully compensated state has been explained by a structural analysis, where magnetic exchange interaction between Cr sites is dependent on bond distance and bond angle of each Cr-centered octahedron. Furthermore, by applying strains perpendicular to the basal plane, distortion of Cr octahedron sites and Cr–Cr distance is altered, resulting in the phase transition of the material both electronically and magnetically from HS-AFM to ferrimagnetic (FiM). These studies enable us to rediscover Cr₂S₃ as one of ideal spintronic materials.