Evolution of magnetic phase in two-dimensional van der Waals Mn1−x Ni x PS3 single crystals

Metal thio(seleno)phosphatesMPX3have attracted considerable attentions with wide spanned band gaps and rich magnetic properties. In this series, two neighboring members MnPS3and NiPS3differ 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 Mn1-xNixPS3series 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 temperatureTNshow nonmonotonic V-shape behavior, and the reentrant spin glass phase atx= 0.5 is observed. In addition, abnormal bifurcation ofTNoccurs atx= 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.