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NiPSe3 is regarded as a bandwidth-controlled Mott insulator, distinct fromthe widely studied Mott insulating magnetic graphene MPSe3 (M = Mn and Fe)family. By employing high-pressure synchrotron X-ray diffraction, we observetwo structural transitions as a function of pressure. With the help offirst-principles calculations, we discover the antiferromagnetic (AFM) momentdirections of NiPSe3 switch from out-of-plane to in-plane and the honeycomblayers slide relative to each other at the first structural transition. Thein-plane AFM order persists until the second structural transition, whereuponthe two-dimensional (2D) structure assumes a more three-dimensional (3D)character. A bandwidth-controlled Mott insulator-metal transition (IMT) occursbetween the two structural transitions at 8.0 GPa, concomitant with theemergence of superconductivity with 4.8 K. The superconductivity in NiPSe3emerging in the 2D monoclinic phase coexists with the in-plane AFM order andcontinues into the 3D trigonal phase. Our electronic structure calculationsreveal that the Mott IMT and superconductivity in NiPSe3 are both closelyrelated to the enhanced Se2- 4p and Ni2+ 3d electronic hybridizations underpressure. From these results, we construct the temperature-pressure electronicphase diagram of NiPSe3, revealing rich physics and many similarities withcopper oxide and iron-based superconductors.

Coexistence of zigzag antiferromagnetic order and superconductivity in compressed NiPSe3