Real-Space Observation of Ripple-Induced Symmetry Crossover in Ultrathin MnPS₃

Stacking order is expected to have a significant impact on the properties of van der Waals layered magnets, as it determines the crystallographic and magnetic symmetry. Recent synchrotron-based optical studies on antiferromagnetic MnPS₃ have revealed a thickness-dependent symmetry crossover, suggesting possible different stackings in few-layer crystals from the bulk, which, however, has not been explicitly identified. Here, by using a combination of atomic-scale electron microscopy and theoretical calculations, we show that despite the bulk monoclinic stacking persists macroscopically down to bilayer, additional local rippling effect lifts the monoclinic symmetry of the few layers while preserving the trigonal symmetry of individual monolayers, leading to possible monolayer-like behavior in ultrathin MnPS₃ samples. This finding reveals the profound impact of rippling on the microscopic symmetry of two-dimensional materials with weak interlayer interactions and raises the possibility of approaching the paradigmatic two-dimensional Néel antiferromagnetic honeycomb lattice in MnPS₃ without reaching monolayer thickness.