Magnetic anisotropy and magnetic ordering of transition-metal phosphorus trisulfides

Abstract

Here, a magnetic model with an unprecedentedly large number of parameters was determined from first-principles calculations for transition-metal phosphorus trisulfides (TMPS${}_3$'s), which reproduced the measured magnetic ground states of bulk TMPS${}_3$'s. Our Monte Carlo simulations for the critical temperature, magnetic susceptibility, and specific heat of bulk and few-layer TMPS${}_3$'s agree well with available experimental data and show that the antiferromagnetic order of FePS${}_3$ and NiPS${}_3$ persists down to monolayers. Remarkably, the orbital polarization, which was neglected in recent first-principles studies, dramatically enhances the magnetic anisotropy of FePS${}_3$ by almost two orders of magnitude. A recent Raman study [K. Kim et al., Nat. Commun. 10, 345 (2019)] claimed that magnetic ordering is absent in monolayer NiPS${}_3$ but simultaneously reported a strong two-magnon continuum; we show that the criterion used to judge magnetic ordering there is invalid in monolayer NiPS${}_3$, thus providing an understanding of the two seemingly contradictory experimental results. The rich predictions on the magnetic susceptibility and specific heat of few-layer FePS${}_3$ and NiPS${}_3$ await immediate experimental verifications.

This document is the unedited Author's version of a Submitted Work that was subsequently accepted for publication in Nano Letters, American Chemical Society after peer review. To access the final edited and published work see https://pubs.acs.org/articlesonrequest/AOR-3TCU3CMMVGHMTTRIVWYS

References in corpus (12)

• Ising-Type Magnetic Ordering in Atomically Thin FePS3
• Calculations of Hubbard U from first-principles
• Suppression of magnetic ordering in XXZ-type antiferromagnetic monolayer NiPS3
• Antiferromagnetic ordering in van der Waals two-dimensional magnetic material MnPS3 probed by Raman spectroscopy
• Highly Anisotropic Excitons and Multiple Phonon Bound States in a Van der Waals Antiferromagnetic Insulator
• Evidence of Spin Frustration in Vanadium Diselenide Monolayer Magnet
• Interplay between magnetic properties and Fermi surface nesting in iron pnictides
• Magnetic anisotropy and exchange interactions of two-dimensional FePS${}_3$, NiPS${}_3$ and MnPS${}_3$ from first principles calculations
• Tunneling transport of mono- and few-layers magnetic van der Waals MnPS${}_3$
• Magnetoelastic interaction in the two-dimensional magnetic material MnPS${}_3$ studied by first principles calculations and Raman experiments
• Distinctive magnetic properties of CrI3 and CrBr3 monolayers caused by spin-orbit coupling
• Complete mapping of magnetic anisotropy for prototype Ising van der Waals FePS${}_3$