Issue 16, 2021

Spin-crossover induced ferromagnetism and layer stacking-order change in pressurized 2D antiferromagnet MnPS3

Abstract

Spin-crossover combined with metal–insulator transition and superconductivity has been found in 2D transition-metal phosphorous trichalcogenides when tuning them by high pressure. Simulation of such intriguing spin-crossover behaviors is crucial to understanding the mechanism. The Hubbard U correction is widely used to describe the strong on-site Coulomb interaction in the d electrons of transition-metal compounds, while the U values are sensitive to the crystal field and spin state varying greatly with pressure. In this work, we show that taking MnPS3 as an example and based on a uniform parameter set, the hybrid functional calculations give a spin-crossover pressure of 35 GPa consistent with experimental observation (30 GPa), which is less than half of the existing reported value (63 GPa) using the Hubbard U correction. Notably, we find a spin-crossover induced transition from an antiferromagnetic semiconductor with monoclinic stacking-order to a ferromagnetic semiconductor with rhombohedral stacking-order, and the ferromagnetism originates from the partially occupied t2g orbitals. Different from previous understanding, the Mott metal–insulator transition of MnPS3 does not occur simultaneously with the spin-crossover but in a pressurized low-spin phase.

Graphical abstract: Spin-crossover induced ferromagnetism and layer stacking-order change in pressurized 2D antiferromagnet MnPS3

Article information

Article type
Paper
Submitted
17 Sep 2020
Accepted
08 Feb 2021
First published
09 Feb 2021

Phys. Chem. Chem. Phys., 2021,23, 9679-9685

Spin-crossover induced ferromagnetism and layer stacking-order change in pressurized 2D antiferromagnet MnPS3

H. Zhang, C. Niu, J. Zhang, L. Zou, Z. Zeng and X. Wang, Phys. Chem. Chem. Phys., 2021, 23, 9679 DOI: 10.1039/D0CP04917D

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