Transition metals Fe, Co, and Ni are the canonical systems for studying the effect of external perturbations on ferromagnetism. Among these, Ni stands out as it undergoes no structural phase transition under pressure. Here we have investigated the long-debated issue of the pressure-induced magnetization drop in Ni from first principles. Our calculations confirm an abrupt quenching of magnetization at high pressures not associated with any structural phase transition. We find that the pressure substantially enhances the crystal-field splitting of Ni-$3d$ orbitals, driving the system toward a new metallic phase violating the Stoner Criterion for ferromagnetic (FM) ordering. Analyzing the charge populations in each spin channel, we show that the next-nearest-neighbor interactions play a crucial role in quenching FM ordering in Ni and materials alike.
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