Novel ways to tune magnetism in metal thiophosphates MPX₃

Recent discoveries in two-dimensional magnetism have intensively motivated the search of new van der Waals magnetic materials and further engineer their magnetic properties for potential use in spintronics applications. Tunable magnetism has been widely studied in antiferromagnetic metal thiophosphates MPX₃. Substitution of metal ions M has been adopted as a common technique to manipulate their magnetism. Here, we present other approaches to tune magnetism in MPX₃: chalcogen X substitution and lithium intercalation. Our studies reveal the effective control of magnetic exchanges and anisotropies upon chalcogen substitution. In addition, we found the signature of ferrimagnetism up on Li intercalation in van der Waals-type MPX₃, which provides alternative route to achieve various magnetic phases in MPX₃ that are not accessible through metal substitution.