Evolution of magnetic phase in two-dimensional van der Waals Mn_1−x Ni _x PS₃ single crystals

Abstract

Metal thio(seleno)phosphates MPX3 have attracted considerable attentions with wide spanned band gaps and rich magnetic properties. In this series, two neighboring members MnPS3 and NiPS3 differ in magnetic atoms, magnetic easy axes, spin anisotropies, as well as nearest-neighbor magnetic interactions. The competition between these components may cause intriguing physical phenomena. In this article, the evolution of magnetism of Mn1-xNixPS3 series is reported. Despite the incompatible antiferromagnetic orders of two end members, the antiferromagnetism persists as the ground state in the whole substitution region. The magnetic ordering temperature TN show nonmonotonic V-shape behavior, and the reentrant spin glass phase at x=0.5 is observed. In addition, abnormal bifurcation of TN occurs at x=0.75, which may be due to the temperature-dependent spin reorientation or phase separation. The evolution of magnetism is further confirmed semiquantitatively by our density functional theory calculations. Our study indicates that exotic magnetism can be intrigued when multi-degrees of freedom are involved in these low dimensional systems, which call for more in-depth microscopic studies in future.

Alterferroicity with seesaw-type magnetoelectricity

“…Both magnetic and polar TMTCs have been reported, such as ferroelectric CuInP S ( 16 ) and ferromagnetic CrGeTe ( 17 ). Other antiferromagnets like PS ( = Fe, Mn, Ni) have also been well known ( 18 , 19 ), and recently, a few more ferroelectric candidates were predicted in some TMTC’s monolayers by a high-throughput calculation ( 20 ). In addition, the weak electronegativities of chalcogens and auxiliary ions allow (partial) covalent bonds.…”

MPX3 van der Waals magnets under pressure (M = Mn, Ni, V, Fe, Co, Cd; X = S, Se)

“…Toward this end, researchers are using chemical substitution, doping and intercalation, as well as various external perturbations such as electric field, light, strong magnetic fields, and strain (Wang et al, 2018a;Pei et al, 2022). For instance, chemical substitution on the M and X sites provides the control of d-orbital filling and bandwidth, respectively, which are both important parameters to control Mottness, magnetism, and spin-orbital-lattice coupling (Lu et al, 2022;Peng et al, 2023). Even better, many MPS 3 compounds have both X = S and Se limits as stable systems, which allows continuous tuning of lattice parameters and bandwidth via synthesizing MPS x Se 3−x samples (Basnet et al, 2022b).…”

Ferromagnetism Induced by Magnetic Dilution in Van der Waals Material Metal Thiophosphates

“…Various strategies have been implemented by introducing defects, intercalation, substrate, and chemical doping. Previous attempts focused on Mn 1-x Fe x PSe 3 , [35] Mn 1-x Fe x PS 3 , [36,37] Fe 1-x Ni x PS 3 , [38,39] and Mn 1-x Ni x PS 3 [40,41] solid solutions for which two end members have distinct spin anisotropies, spin directions, and magnetic interactions. Glassy-like states, such as magnetic glass, spin glass/cluster spin glass, are observed with the ordering temperatures falling between the Néel temperatures of two parent compounds.…”