Magnetic anisotropy and magnetic ordering of transition-metal phosphorus trisulfides

Tae Yun Kim; Cheol-Hwan Park

doi:10.1021/acs.nanolett.1c03992

paper

Magnetic anisotropy and magnetic ordering of transition-metal phosphorus trisulfides

arXiv:2111.14869 · doi:10.1021/acs.nanolett.1c03992

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.

arXiv commentThis 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

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Crucial role of magnetic dipole and anomalous field dependence in $NiP S_{3}$