Core-shell nanoparticles of MnO|Mn3O4 with average particle sizes of 5-60 nm, composed of an antiferromagnetic (AFM) core and a ferrimagnetic (FiM) shell, have been synthesized and their magnetic properties investigated. The core-shell structure has been generated by the passivation of the MnO cores, yielding an inverted AFM-core|FiM-shell system, as opposed to the typical FM-core|AFM-shell. The exchange-coupling between AFM and FiM gives rise to an enhanced coercivity of approximately 8 kOe and a loop shift of approximately 2 kOe at 10 K, i.e., exchange bias. The coercivity and loop shift show a non-monotonic variation with the core diameter. The large coercivity and the loop shift are ascribed to the highly anisotropic Mn3O4 and size effects of the AFM (i.e., uncompensated spins, AFM domains, and size-dependent transition temperature).

The growing miniaturization demand of magnetic devices is fuelling the recent interest in bi-magnetic nanoparticles as ultimate small components. One of the main goals has been to reproduce practical magnetic properties observed so far in layered systems. In this context, although useful effects such as exchange bias or spring magnets have been demonstrated in core/shell nanoparticles, other interesting key properties for devices remain elusive. Here we show a robust antiferromagnetic (AFM) coupling in core/shell nanoparticles which, in turn, leads to the foremost elucidation of positive exchange bias in bi-magnetic hard-soft systems and the remarkable regulation of the resonance field and amplitude. The AFM coupling in iron oxide-manganese oxide based, soft/hard and hard/soft, core/shell nanoparticles is demonstrated by magnetometry, ferromagnetic resonance and X-ray magnetic circular dichroism. Monte Carlo simulations prove the consistency of the AFM coupling. This unique coupling could give rise to more advanced applications of bi-magnetic core/shell nanoparticles.

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