Termination-Dependent Surface Fermiology in the Intercalated Altermagnet CoNb4Se8

Abstract Altermagnets have recently gained attention for hosting symmetry-enforced spin-split bands despite zero net magnetization. Angle-resolved photoelectron spectroscopy (ARPES) offers direct access to their electronic structure. However, the intrinsic surface sensitivity of this technique complicates the identification of the observed features: Surface states can be misinterpreted as the spin-split counterpart of bulk bands. This issue becomes particularly relevant for layered intercalated systems, where micrometer-sized domains with distinct terminations often coexist on a cleaved surface. We discuss this scenario for CoNb4Se8, one of the first established layered altermagnets. Supported by density functional theory calculations, we employ micro-ARPES to probe individual domains and reveal two contrasting surface terminations. We identify Co- and Se-terminated domains with characteristic surface states arising from bulk-surface connectivity of the material. Our work shows that termination-dependent surface contributions are essential for the reliable spectroscopic identification of altermagnetism and for assessing its presence across the family of layered materials.