Abstract
Here, a combined experimental and theoretical investigation of the properties of Ni${}_{3}$TeO${}_{6}$ under pressure reveals reduced compressibility near 4 GPa due to the unique behavior of one bond angle. This trend arises from a nearby cavity in the crystal structure that enhances tunability in this and other corrundumlike materials. Analysis of superexchange angles reveals enhanced antiferromagnetic interactions, in line with an increase in ${T}_{N}$ observed in magnetization. Magnetoelectric coupling likely enhances polarization under pressure. This work suggests that incorporating empty cavities into crystal structures provides a new route for control of multiferroic properties.
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