Parasitic Ferromagnetism in Few-Layered Transition-Metal Chalcogenophosphate

Since the rise of two-dimensional (2D) semiconductors, it seems that electronic devices will soon be upgraded with spintronics, in which the manipulation of spin degree of freedom endows it obvious advantages over conventional charge-based electronics. However, as the most crucial prerequisite for the above-mentioned expectation, 2D semiconductors with adjustable magnetic interaction are still rare, which has greatly hampered the promotion of spintronics. Recently, transition metal phosphates have attracted tremendous interest due to their intrinsic antiferromagnetism and potential applications in spintronics. In the work described herein, parasitic ferromagnetism is achieved for the first time by exfoliating an antiferromagnetic chalcogenophosphate to a few layers. Taking the transition metal chalcogenophosphate Mn₂P₂S₆ as an example, the antiferromagnetic transition at the Néel temperature is completely suppressed, and the magnetic behaviors of the as-obtained few-layered Mn₂P₂S₆ are dominated by parasitic ferromagnetism. We experimentally verify an electron redistribution by which part of the Mn 3d electrons migrate and redistribute on P atoms in few-layered Mn₂P₂S₆ due to the introduced Mn vacancies. The results demonstrated here broaden the tunability of the material's magnetic properties and open up a new strategy to rationally design the magnetic behaviors of 2D semiconductors, which could accelerate the applications of spintronics.