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

TL;DR

This study reveals a pressure-induced spin-crossover in MnPS$_3$ at 35 GPa, leading to a transition from antiferromagnetism to ferromagnetism and a stacking-order change, with the Mott transition occurring separately in the low-spin phase.

Contribution

It demonstrates a lower spin-crossover pressure using hybrid functional calculations and uncovers the separate occurrence of Mott transition and spin-crossover in MnPS$_3$.

Findings

Spin-crossover occurs at 35 GPa, matching experimental data.

A transition from antiferromagnetism to ferromagnetism is induced by pressure.

Stacking order changes from monoclinic to rhombohedral during the transition.

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.