Emergent mixed antiferromagnetic state in MnPS3(1-x)Se3x

The discovery of magnetism in van der Waal (vdW) materials has aroused substantial interest in the exploration of magnetic interactions toward a two-dimensional (2D) limit. Here, we report the engineering of magnetic properties in MnPS3(1-x)Se3x compounds by substituting the non-magnetic chalcogenide S atoms with Se atoms. The anisotropic antiferromagnetic transition of MnPS3(1-x)Se3x compounds is gradually modulated by controlling the Se concentration, including the monotonic decrease in the Néel temperature and Curie–Weiss temperature with increasing Se concentration, and the Se concentration dependence of a spin-flop process. In addition, the magnetic phase diagram is established, in which an exotic mixed antiferromagnetic state appears due to the competition between the magnetic orderings in parent materials of MnPS3 and MnPSe3. Our findings validate the possibility of the manipulation of magnetic properties in magnetic vdW materials through the substitution of chalcogenide ions and pave the way toward the engineering of magnetic interactions and the designing of magnetic devices in two-dimensional magnetic vdW materials.