From predicting to correlating the bonding properties of iron sulfide phases

Abstract

Iron sulfides have emerged as a fascinating class of materials in electromagnetics and catalysis areas, which however are challenging in first-principles modeling because of the strongly-correlated interactions between Fe 3d and S 3p electrons. Here, we assess the performances of 14 density functionals on the structural, electronic, and magnetic properties of five iron sulfides. The PBE + U with Ueff = 2.0 eV has the overall best performance. After evaluating functionals and obtaining reliable properties, our final goal is from predicting to correlating in order to do high throughput screening for the systems since the complex structures and phases of iron sulfides, to put it in another way, to hunting a reliable descriptor for predicting their properties. In the work, we demonstrate that the crystal orbital Hamilton population (COHP) and Bader charge of Fe atoms presents a good correlation with the empirical bond valence. Our results open a new avenue to effectively investigate phases and properties for various structures of iron sulfides. Indeed, the correlations between COHP/Bader charge and bond valence can be extended to other systems.