Search

Tuning magnetic properties in layered magnets is an important route to realize novel phenomenon related to two-dimensional (2D) magnetism. Recently, tuning antiferromagnetic (AFM) properties through substitution and intercalation techniques have been widely studied in MPX3 compounds. Interesting phenomena, such as diverse AFM structures and even the signatures of ferrimagnetism, have been reported. However, long-range ferromagnetic (FM) ordering has remained elusive. In this work, we explored the magnetic properties of the previously unreported Cr-substituted NiPS3. We found that Cr substitution is extremely efficient in controlling spin orientation in NiPS3. Our study reveals a field-induced spin polarization in lightly (9%) Cr-substituted NiPS3, which is likely attributed to the attenuation of AFM interactions and magnetic anisotropy due to Cr doping. Our work provides a possible strategy to achieve FM phase in AFM MPX3, which could be useful for investigating 2D magnetism as well as potential device applications.

Recent development in two-dimensional (2D) magnetic materials have motivated the search for new van der Waals magnetic materials, especially Ising-type magnets with strong magnetic anisotropy. Fe-based MPX3 (M = transition metal, X = chalcogen) compounds such as FePS3 and FePSe3 both exhibit an Ising-type magnetic order, but FePSe3 receives much less attention compared to FePS3. This work focuses on establishing the strategy to engineer magnetic anisotropy and exchange interactions in this less-explored compound. Through chalcogen and metal substitutions, the magnetic anisotropy is found to be immune against S substitution for Se whereas tunable only with heavy Mn substitution for Fe. In particular, Mn substitution leads to a continuous rotation of magnetic moments from the out-of-plane direction towards in-plane. Furthermore, the magnetic ordering temperature displays non-monotonic doping dependence for both chalcogen and metal substitutions but due to different mechanisms. These findings provide deeper insight into the Ising-type magnetism in this important van der Waals material, shedding light on the study of other Ising-type magnetic systems as well as discovering novel 2D magnets for potential applications in spintronics.