Strongly Exchange Coupled Core|Shell Nanoparticles with High Magnetic Anisotropy: A Strategy toward Rare-Earth-Free Permanent Magnets

Antiferromagnetic­(AFM)|ferrimagnetic­(FiM) core|shell (CS) nanoparticles (NPs) of formula Co0.3Fe0.7O|Co0.6Fe2.4O4 with mean diameter from 6 to 18 nm have been synthesized through a one-pot thermal decomposition process. The CS structure has been generated by topotaxial oxidation of the core region, leading to the formation of a highly monodisperse single inverted AFM|FiM CS system with variable AFM-core diameter and constant FiM-shell thickness (∼2 nm). The sharp interface, the high structural matching between both phases, and the good crystallinity of the AFM material have been structurally demonstrated and are corroborated by the robust exchange-coupling between AFM and FiM phases, which gives rise to one among the largest exchange bias (H E) values ever reported for CS NPs (8.6 kOe) and to a strongly enhanced coercive field (H C). In addition, the investigation of the magnetic properties as a function of the AFM-core size (d AFM), revealed a nonmonotonous trend of both H C and H E, which display a maximum value for d AFM = 5 nm (19.3 and 8.6 kOe, respectively). These properties induce a huge improvement of the capability of storing energy of the material, a result which suggests that the combination of highly anisotropic AFM|FiM materials can be an efficient strategy toward the realization of novel rare-earth-free permanent magnets.