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The effects of cobalt incorporation in spherical heterostructured iron oxidenanocrystals (NCs) of sub-critical size have been explored by colloidalchemistry methods. Synchrotron X-ray total scattering methods suggest thatcobalt (Co) substitution in rock salt iron oxide NCs tends to remedy its vacantiron sites, offering a higher degree of resistance to oxidative conversion.Self-passivation still creates a spinel-like shell, but with higher volumefraction of the rock salt Co-containing phase in the core. The higher divalentmetal stoichiometry in the rock salt phase, with increasing Co content, resultsin a population of unoccupied tetrahedral metal sites in the spinel part,likely through oxidative shell creation, involving an ordered defect-clusteringmechanism, directly correlated to the core stabilization. To shed light on theeffects of Co-substitution and atomic-scale defects (vacant sites), Monte Carlosimulations suggest that designed NCs, with desirable, enhanced magneticproperties (cf. exchange bias and coercivity), are developed withmagnetocrystalline anisotropy raised at relatively low content of Co ions inthe lattice. Growth of optimally performing candidates combines also a stronglyexchange-coupled system, secured through a high volumetric ratio rock saltphase, interfaced by a not so defective spinel shell. In view of theserequirements, Specific Absorption Rate (SAR) calculations demonstrate that thesufficiently protected from oxidation rock salt core and preserved over timeheterostructure, play a key role in magnetically-mediated heating efficacies,for potential use of such NCs in magnetic hyperthermia applications.

Tailoring defects and nanocrystal transformation for optimal heating power in bimagnetic $Co_yFe_{1-y}O@Co_xFe_{3-x}O_4$ particles