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Frustrated antiferromagnets offer a captivating platform to study the intricate relationship of magnetic interactions, geometric constraints, and emergent phenomena. By controlling spin orientations, these materials can be tailored for applications in spintronics and quantum information processing. The research focuses on the interplay of magnetic and exchange anisotropy effects in artificial heterostructures based on a canonical frustrated antiferromagnet, UO 2 . The potential to manipulate the spin directions in this material and switch between distinct antiferromagnetic (AFM) states is investigated using substrate‐induced strain. The phenomenon is probed using exchange bias effects in stoichiometric UO 2 /Fe 3 O 4  bilayers. By employing many‐body first‐principles calculations magnetic configurations in the UO 2  layers are identified. Even a minor tetragonal distortion triggers a transition between AFM states of different symmetries, driven by a robust alteration of single‐ion anisotropy due to the distortion. Consequently, this change influences the arrangement of magnetic moments at the UO 2 /Fe 3 O 4  interface, affecting the magnitude of exchange bias. The findings showcase how epitaxial strain can effectively manipulate the AFM states in frustrated antiferromagnets by controlling single‐site anisotropy.

Strain‐driven Switching Between Antiferromagnetic States in Frustrated Antiferromagnet UO 2 Probed by Exchange Bias Effect