Magnetic anisotropy and exchange interactions of two-dimensional FePS$_3$, NiPS$_3$ and MnPS$_3$ from first principles calculations

TL;DR

This study uses first-principles calculations to analyze the magnetic anisotropy and exchange interactions in 2D FePS$_3$, NiPS$_3$, and MnPS$_3$, highlighting the importance of Hubbard U and comparing results with experimental data.

Contribution

It provides a detailed first-principles analysis of magnetic interactions in 2D transition metal phosphorous trichalcogenides, emphasizing the U-dependence and comparing with experimental spectra.

Findings

Exchange constants agree with experiments when U is properly chosen

Néel temperature varies significantly with U for FePS$_3$

DFT underestimates magnetic anisotropy parameters

Abstract

The van der Waals bonded transition metal phosphorous trichalcogenides FePS$_3$, NiPS$_3$ and MnPS$_3$ have recently attracted renewed attention due to the possibility of exfoliating them into their monolayers. Although the three compounds have similar electronic structure, the magnetic structure differs due to subtle differences in exchange and magnetic anisotropy and the materials thus comprise a unique playground for studying different aspects of magnetism in 2D. Here we calculate the exchange and anisotropy parameters of the three materials from first principles paying special attention to the choice of Hubbard parameter U. We find a strong dependence of the choice of U and show that the calculated N\'eel temperature of FePS$_3$ varies by an order of magnitude over commonly applied values of U for the Fe $d$-orbitals. The results are compared with parameters fitted to experimental spin-wave spectra of the bulk materials and we find excellent agreement between the exchange constants when a proper value of U is chosen. However, the anisotropy parameters are severely underestimated by DFT and we discuss possible origins of this discrepancy.