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 0.12μ_B 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.