Robust Spin Splitting and Fermiology in the Layered Altermagnet CoNb4Se8

ABSTRACT Altermagnetism defies conventional classifications of collinear magnetic phases, combining compensated magnetization with momentum‐dependent, nonrelativistic spin splitting. While altermagnetic band splitting has been established in three‐dimensional compounds such as MnTe and CrSb, layered altermagnets remain far less explored spectroscopically. Here, combining termination‐resolved micro‐ARPES, fine photon‐energy mapping, spin‐ARPES, and density functional theory, we map the three‐dimensional fermiology of the layered g ‐wave altermagnet , obtained by ordered Co intercalation of 2H‐. We resolve the spin–split branches of the altermagnetic pairs directly in the raw photoemission spectra and, with spin‐ARPES at these experimentally identified momenta, show the reversal of the spin polarization at opposite momenta and between two regions of the sample, consistent with opposite time‐reversal domains, and its absence along the symmetry‐protected nodal –K direction. We further report a weak low‐temperature anomaly near T 0 ≈ 50–60 K, detected by magnetometry, temperature‐dependent micro‐ARPES, and ultrafast reflectivity, whose microscopic origin remains open. These results provide a momentum‐resolved benchmark of the electronic structure of a layered altermagnet.