Dimension‐ and Facet‐Dependent Altermagnetic Biferroics and Ferromagnetic Biferroics and Triferroics in CrSb

Abstract Altermagnets have recently garnered significant interest due to their vanishing net magnetic moment and non‐relativistic momentum‐dependent spin splitting. However, altermagnetic (AM) multiferroics especially triferroics remain scarce. The experimentally synthesized non‐van der Waals CrSb as a model system is investigated to explore the effects of dimensionality and facet orientation on its ferroic properties. NiAs, MnP, wurtzite (WZ), zincblende (ZB), and rocksalt (RS) phases are considered. Using first‐principles calculations, the altermagnetism of CrSb is predicted in MnP phase, which has comparable stability with experimental NiAs phase. Both NiAs‐ and MnP‐phase (110) facets exhibit AM–ferroelastic (FC) biferroics, while the WZ‐phase bulk and (001) facets host ferromagnetic (FM)–ferroelectric (FE) biferroics. Notably, the WZ‐phase (110) facets are identified as FM–FE–FC triferroics, with moderate energy barriers of 0.129 and 0.363 eV atom −1 for FE and FC switching, respectively. Both FE and FC switching can reverse the AM spin splitting in antiferromagnetic (AFM) configurations while preserving the high spin polarization in FM states. The magnetic anisotropy is highly tunable, exhibiting either uniaxial or in‐plane behavior depending on the phase, dimension, and facet. This work establishes a framework for designing AM multiferroics through polymorphic, dimensional, and facet engineering, offering promising avenues for multifunctional spintronic applications.