First-principles based study of magnetic states and high-pressure enthalpy landscape of manganese sulfide polymorphs

TL;DR

This study uses first-principles calculations to explore magnetic states and pressure-induced structural transformations in manganese sulfide polymorphs, revealing a phase transition around 21 GPa consistent with experimental findings.

Contribution

The paper introduces a combined computational approach that accurately predicts magnetic properties and phase transitions in MnS under pressure, aligning well with experimental data.

Findings

Identification of a structural transition at ~21 GPa from rock-salt to MnP-type phase.

Accurate prediction of magnetic moments and band gaps in MnS.

Correlation of computational results with experimental phase behavior.

Abstract

Using first-principles calculations in combination with special quasirandom structure and occupation control matrix methods, we study the magnetic ordering and the effect of pressure on manganese sulfide polymorphs. At ambient conditions, MnS is commonly observed in paramagnetic rock-salt structure, but as temperature decreases at constant pressure it becomes antiferromagnetic. On the other hand, at room temperature MnS has shown to undergo structural transformations as pressure increases. Here, we show that our approach involving the ordering/disordering of the local magnetic moments in addition to the explicit dealing with the localization of the Mn $d$-electrons produces energy band gaps and local magnetic moments in excellent agreement with those observed experimentally, particularly for paramagnetic MnS. Finally, we focus on how MnS evolves under pressure and from its enthalpy landscape we identify at about 21~GPa, the structural transformation from rock-salt to orthorhombic MnP-type. This structural transformation resembles closely experimental results in which a new stable but unidentified MnS phase was previously reported.