Figure 1.

High‐Néel‐temperature metallic spin‐split antiferromagnet CrSb. a) Crystal structure of CrSb along with magnetic moments. Red/blue arrows indicate the spin‐up and ‐down orientations of the Cr atom. b) Spin‐polarized electronic density distribution of CrSb. Black lines indicate the unit cell. Red dash lines indicate the mirror planes. Transpose symmetries [C₂ || M_z ] and [C₂ || C_6zt] are shown. c) Left: the 3D and surface‐projected Brillouin zone (BZ) of CrSb. Blue dots represent high symmetry points; green dots represent the midpoint between two high symmetry points. Right: Schematic for the sign of S_z polarization in the 3D BZ. d) DFT‐calculated spin‐resolved bands with SOC. There is no spin polarization within the ΓMK and ΓKHA plane, whereas a high level of spin polarization is seen in the OBC and ΓMLA plane. e) Core‐level photoemission spectra taken on an in situ cleaved sample at hν = 137 eV. f) Single crystal XRD results and representative Laue X‐ray diffraction pattern of the (001) surface of CrSb. Yellow arrows in the Laue pattern show the orientation indexes of [100] and [110]. Inset: a hexagonally shaped CrSb single crystal with exposed (001) plane against a millimeter gird.