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 Neel 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.

Automated summary

This study successfully manipulated the magnetism of MnPS3(1-x)Se3x compounds by substituting non-magnetic sulfur atoms with selenium atoms. The anisotropic antiferromagnetic transition of MnPS3(1-x)Se3x compounds were gradually modulated by controlling the selenium concentration, including the monotonic decrease in Neel temperature and Curie-Weiss temperature with increasing selenium concentration, and the selenium concentration dependence of a spin-flop process. Additionally, a magnetic phase diagram was established, revealing an exotic mixed antiferromagnetic state due to the competition between magnetic orderings in parent materials. These findings demonstrate the potential for engineering magnetic properties in magnetic van der Waal materials through chalcogenide ion substitution and provide insights for the design of magnetic devices in two-dimensional magnetic van der Waal materials.