Ferromagnetic correlations in the layered van der Waals sulfide FeAl2S4.

Transition metal-based layered compounds with van der Waals gaps between the adjacent layers are a source of two-dimensional (2D) nanomaterials with nontrivial transport and magnetic properties. 2D ferromagnets, both metals and semiconductors, can be leveraged to produce spin-polarized current in spintronic devices with tailored functionalities. Here, we report on the synthesis, crystal growth, crystal and electronic structure, and magnetic properties of the Fe-based FeAl2S4 layered sulfide. In the crystal structure, Fe and Al atoms mix on octahedral and tetrahedral sites between hexagonal layers of S atoms, which are terminated by the van der Waals gaps. Band structure calculations reveal strong electronic correlations within the semiconducting ground state, which induce ferromagnetism with the magnetic moment of 0.12µB per formula unit for a Hubbard interaction U = 5 eV and Hund's rule coupling J = 0.8 eV. Crystal growth employing chemical vapor transport reactions results in bulk cleavable crystals, which show paramagnetic Curie-Weiss behavior at high temperatures with the Fe2+ magnetic centers. At low temperatures, an anomaly is observed on the magnetic susceptibility curve, below which the magnetization shows ferromagnetic hysteresis, indicating the presence of ferromagnetic correlations in FeAl2S4.