Defect-mediated ferromagnetism in correlated two-dimensional transition metal phosphorus trisulfides

Controlling the magnetic spin states of two-dimensional (2D) van der Waals (vdW) materials with strong electronic or magnetic correlation is important for spintronic applications but challenging. Crystal defects that are often present in 2D materials such as transition metal phosphorus trisulfides (MPS3) could influence their physical properties. Here, we report the effect of sulfur vacancies on the magnetic exchange interactions and spin ordering of few-layered vdW magnetic Ni1-xCoxPS3 nanosheets. Magnetic and structural characterization in corroboration with theoretical calculations reveal that sulfur vacancies effectively suppress the strong intralayer antiferromagnetic correlation, giving rise to a weak ferromagnetic ground state in Ni1-xCoxPS3 nanosheets. Notably, the magnetic field required to tune this ferromagnetic state (<300 Oe) is much lower than the value needed to tune a typical vdW antiferromagnet (> several thousand oersted). These findings provide a previously unexplored route for controlling competing correlated states and magnetic ordering by defect engineering in vdW materials.

Automated summary

This study investigates the influence of sulfur vacancies on the spin states of Ni1-xCoxPS3 nanosheets, finding that the vacancies effectively suppress strong intralayer antiferromagnetic correlation, leading to a weak ferromagnetic ground state. Additionally, the magnetic field required to tune this ferromagnetic state is much lower compared to typical antiferromagnetic materials, providing a new route for controlling spin states through defect engineering in vdW materials.