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We use synchrotron x-ray diffraction and electrical transport under pressureto probe both the magnetism and the structure of single crystal NiS2 across itsMott-Hubbard transition. In the insulator, the low-temperatureantiferromagnetic order results from superexchange among correlated electronsand couples to a (1/2, 1/2, 1/2) superlattice distortion. Applying pressuresuppresses the insulating state, but enhances the magnetism as thesuperexchange increases with decreasing lattice constant. By comparing ourresults under pressure to previous studies of doped crystals we show that thisdependence of the magnetism on the lattice constant is consistent for both bandbroadening and band filling. In the high pressure metallic phase the latticesymmetry is reduced from cubic to monoclinic, pointing to the primary influenceof charge correlations at the transition. There exists a wide regime of phaseseparation that may be a general characteristic of correlated quantum matter.

Magnetism, structure, and charge correlation at a pressure-induced Mott-Hubbard insulator-metal transition