Evolution of magnetic phase in two dimensional van der Waals Mn${}_{1-x}$Ni${}_x$PS${}_3$ single crystals

Abstract

Metal thio(seleno)phosphates MPX${}_3$ have attracted considerable attentions with wide spanned band gaps and rich magnetic properties. In this series, two neighboring members MnPS${}_3$ and NiPS${}_3$ differ in magnetic atoms, magnetic easy axes, spin anisotropy, 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 Mn${}_{1-x}$Ni${}_x$PS${}_3$ 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 $T_{\mathrm{N}}$ show nonmonotonic V-shape behavior, and the reentrant spin glass phase at x=0.5 is observed. In addition, abnormal bifurcation of $T_{\mathrm{N}}$ 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 semi-quantitatively 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.

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• Magnetic anisotropy and low-energy spin dynamics in the van der Waals compounds Mn${}_2$P${}_2$S${}_6$ and MnNiP${}_2$S${}_6$
• Electron Spin Resonance Spectroscopy on Magnetic Van der Waals Compounds
• Evolution of the spin dynamics in the van der Waals system $M_{\text{2}}$P${}_{\text{2}}$S${}_{\text{6}}$ (${\mathbf{M}}_{\text{2}}$ = Mn${}_{\text{2}}$, MnNi, Ni${}_{\text{2}}$) series probed by electron spin resonance spectroscopy