Ferromagnetism Induced by Magnetic Dilution in Van der Waals Material Metal Thiophosphates.

Metal thio(seleno) phosphates MPX3 attract considerable attention with potential application in spintronics and other types of devices. Here, ferromagnetism in an Ising type diluted magnetic semiconductor Fe1‐xZnxPS3 is reported. Bulk single crystals of Fe1‐xZnxPS3 have been synthesized via chemical vapor transport method and characterized by X‐ray diffraction. The weak ferromagnetism associated with spin/cluster spin glass emerges at 30% Zn doping. A nearly static ferromagnetic order is observed in the highly diluted magnets Fe0.1Zn0.9PS3. X‐ray photoemission measurements indicate introduction of holes and associated Fe3+ in samples with ferromagnetic order. Density functional theory calculations confirm the Ising‐type ferromagnetic state in highly diluted compounds with hole doping. The interplay between bound magnetic polarons induces impurity‐band‐exchange and superexchange interactions can explain the evolution of magnetism with Zn doping. The findings suggest that the magnetic diluted FePS3 system is a candidate for potential applications in magnetic devices, and its quantum mechanism should be explored by using microscopic techniques in the near future. [ABSTRACT FROM AUTHOR]