Tuning Magnetism in Ising-type van der Waals Magnet FePS₃ by Lithium Intercalation

Layered transition metal thiophosphate MPX3 (M = transition metals, X = S or Se) have recently gained significant attention because of their rich magnetic, optical, and electronic properties. Specifically, the diverse magnetic structures and the robust magnetism in the two-dimensional limit have made them a prominent platform to study two-dimensional magnetism. Numerous efforts such as substitutions and interlayer intercalations have been made to tune the magnetic properties of these materials, which has greatly deepened the understanding of the underlying mechanisms that govern the properties. In this work, we focus on modifying the magnetism of Ising-type antiferromagnet FePS₃ using electrochemical lithium intercalation, from which we discovered strong modification of magnetic transition temperature and the rise of spin glass state, providing an efficient approach to modify magnetism in this magnetic van der Waals materials.

Funding acknowledgement: DOE DE-SC0022006 and DE-SC0023412, NSF DMR-1906383