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In contrast to bulk materials, nanoscale crystal growth is criticallyinfluenced by size- and shape-dependent properties. However, it is challengingto decipher how stoichiometry, in the realm of mixed-valence elements, can actto control physical properties, especially when complex bonding is implicatedby short and long-range ordering of structural defects. Here, solution-growniron-oxide nanocrystals (NCs) of the pilot wustite system are found to convertinto iron-deficient rock-salt and ferro-spinel sub-domains, but attain asurprising tetragonally distorted local structure. Cationic vacancies withinchemically uniform NCs are portrayed as the parameter to tweak the underlyingproperties. These lattice imperfections are shown to produce localexchange-anisotropy fields that reinforce the nanoparticles magnetization andovercome the influence of finite-size effects. The concept of atomic-scaledefect control in subcritical size NCs, aspires to become a pathway totailor-made properties with improved performance for hyperthermia heating overdefect-free NCs.

Vacancy-driven non-cubic local structure and magnetic anisotropy tailoring in Fe$_x$O-Fe$_{3-\delta}$O$_4$ nanocrystals