2026/06/18 by William A. Schaarman, Sophie F. Weber
#cond-mat.mtrl-sci #physics.comp-ph
We use density functional theory and model Hamiltonians to reveal large spin splitting of bands localized at ferromagnetic surfaces of bulk antiferromagnets (AFMs). There is great interest in material platforms combining the robustness and ultrafast dynamics of AFMs with large, functional spin splitting which is often restricted to ferromagnets (FMs). Here, we show that a subset of AFM surfaces which have symmetry-allowed magnetization can host large spin splitting via bulk degeneracy lifting of sublattice-resolved exchange splittings. We find that the spin splitting is maximized for two ferromagnetic surface motifs: terminations with single uncompensated magnetic sublattices, and two-sublattice surfaces whose sublattices are magnetically compensated in the bulk, but acquire distinct crystal field environments via surface truncation. The latter case can yield FM-like spin splitting magnitudes while also having small uncompensated magnetization. We confirm these predictions with first-principles calculations of Cr2O3 and FeF2, finding splittings as large as 1~eV depending on the surface in question. Our findings point to intrinsic surface symmetry breaking as a route to large, functional spin splitting in an expanded range of AFM materials.