Spin-crossover induced ferromagnetism and layer stacking-order change in pressurized 2D antiferromagnet MnPS$_3$

Abstract: High-pressure properties of MnPS$3$ are investigated by using the hybrid functional, we report a spin-crossover pressure of 35 GPa consisting with experimental observation (30 GPa), less than half of existing report (63 GPa) using the Hubbard U correction. Interestingly, a spin-crossover induced antiferromagnetism-to-ferromagnetism transition combined with stacking-order change from monoclinic to rhombohedral are founded, and the ferromagnetism origins from the partially occupied $t{2g}$ orbitals. Different from previous understanding, the Mott metal-insulator transition of MnPS$_3$ does not occur simultaneously with the spin-crossover but in pressurized low-spin phase.