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

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 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-x Ni (x) PS3 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 (N) show nonmonotonic V-shape behavior, and the reentrant spin glass phase at x= 0.5 is observed. In addition, abnormal bifurcation of T (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.