Short and long-range magnetic ordering and emergent topological transition in (Mn1−xNix)2P2S6

Two-dimensional magnetic materials with tunable physical parameters are emerging as potential candidates for topological phenomena as well as applications in spintronics. The famous Mermin-Wagner theorem states that spontaneous spin symmetry cannot be broken at finite temperature in low dimensional magnetic systems which forbids the possibility of a transition to a long-range ordered state in a two-dimensional magnetic system at finite temperature. Though, there are some exceptions to Mermin-Wagner theorem in particular low dimensional magnetic systems with topologically ordered phase transitions. Here, we present an in-depth temperature dependent analysis for the bulk single crystals of two-dimensional (Mn_1-xNi_x)₂P₂S₆ with x = 1, 0.7, 0.3, 0 using the Raman spectroscopy supported by first-principles calculations of the phonon frequencies. We observed multiple phase transitions with tunability as a function of doping associated with the short and long-range spin-spin correlations. First transition at ~ 150 K to ~ 170 K for x = 0 to x = 0.7, and second one from ~ 60 K to ~ 153 K. Quite interestingly, a third transition is observed at low temperature (much below their respective T_N) ~ 24 K to ~ 60 K and is attributed to the potential topological phase transition. These transitions are marked by the distinct changes observed in the temperature evolution of the phonon self-energy parameters, modes intensity and dynamic Raman susceptibility.