We investigate the sensitive interplay between magnetic, electronic and structural properties in the ferrimagnetic oxide NiFe2O4. Emphasis is placed on the impact of reduced dimensionality in the crossover from bulk-like to ultrathin films. We observed an enhanced saturation magnetization for ultrathin NiFe2O4 films on Nb-SrTiO3 (001) substrates that co-occurs with a reduced out-of-plane lattice constant under compressive in-plane epitaxial strain. We found a bulk-like cationic coordination of the inverse spinel lattice independent of the NiFe2O4 film thickness – thus ruling out a cationic inversion that nominally could account for an enhanced . Our study instead uncovers a reduction of the unit cell volume, i.e. an auxetic behavior in ultrathin NiFe2O4 films, which may result in an enhanced magnetic exchange caused by an increased interatomic electronic localization.

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