Anion correlation induced nonrelativistic spin splitting in rutile antiferromagnets

Abstract

Many studies of non-relativistic spin-splitting (NRSS), or altermagnetism, have focused on idealized, perfectly ordered crystals, relying on symmetry-based approaches to identify candidate materials. Here, we theoretically investigate how local short-range ordering (SRO) influences NRSS of energy bands in partially ordered collinear antiferromagnetic iron oxyfluoride (FeOF). Using the cluster expansion method, we identify four nearly degenerate structures (energy difference $\le 8$ meV per formula unit) that represent distinct snapshots of local plane-to-plane O/F correlations. Our density functional theory (DFT) results show robust NRSS along the $\Gamma$-M direction in all four structures, despite the absence of long-range order. The magnitude and character of the splitting depend sensitively on the specific direction of anion correlations, effects that are not fully captured in high-symmetry average structures. Notably, two configurations ($Pmc{2}_1$ and $Pm$) exhibit $\Gamma$-point spin splitting absent in ordered FeF${}_2$ and a virtual crystal approximation model of FeOF. We further predict distinct magneto-optical Kerr effect (MOKE) signatures, enabling experimental detection of SRO-driven electronic structure changes. These results highlight heteroanionic compounds as a promising design space for NRSS antiferromagnets, with experimentally synthesized FeOF already exhibiting a substantially higher Néel temperature (315\,K) than FeF${}_2$ (79\,K).

13 pages, 5 main figures, 4 appendix figures