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Abstract Recent developments in 2D magnetic materials have motivated the search for new van der Waals magnetic materials, especially Ising‐type magnets with strong magnetic anisotropy. Fe‐basedMPX₃(M= transition metal,X= chalcogen) compounds such as FePS₃and FePSe₃both exhibit an Ising‐type magnetic order, but FePSe₃receives 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 toward the 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. 

The presence of partially filled 4f orbitals of cerium regulates heteroanionic CeHaVIO₄to give good infrared nonlinear optical materials with moderate photocurrent response. 

Heteroanionic chalcohalides La₃AsS₅Br₂and La₅As₂S₉Cl₃exhibit a good example of how alignment of lone pair electrons affects the formation of acentric crystal structure.