Magnetic anisotropy and exchange interactions of two-dimensional FePS3, NiPS3 and MnPS3 from first principles calculations

The van der Waals bonded transition metal phosphorous trichalcogenides FePS3, NiPS3 and MnPS3 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 Neel temperature of FePS3 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 density functional theory and we discuss possible origins of this discrepancy.

Automated summary

FePS3, NiPS3, and MnPS3 are van der Waals bonded transition metal phosphorous trichalcogenides that have attracted attention for their potential exfoliation into monolayers. Despite similar electronic structures, subtle differences in exchange and magnetic anisotropy result in different magnetic structures, making them ideal for studying various aspects of 2D magnetism. The study highlights the significant impact of the Hubbard parameter U choice on calculations and reveals the underestimation of anisotropy parameters by density functional theory.