Evolution of magnetic phase in two-dimensional van der Waals Mn_1-NiPS₃single 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 Mn_1-NiPS₃series 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 temperatureT_Nshow nonmonotonic V-shape behavior, and the reentrant spin glass phase atx= 0.5 is observed. In addition, abnormal bifurcation ofT_Noccurs 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.