Combined Computational and in Situ Experimental Search for Phases in an Open Ternary system, Ba–Ru–S

Abstract

Rapid materials discovery in inorganic chemistry should combine predictive computational tools with fast experimental syntheses. We apply such a tandem approach to explore the Ba–Ru–S phase space, where no ternary compounds are yet known to exist. Related ternary oxide ruthenates and ternary iron sulfides exhibit interesting electronic properties due to d-electron correlations, such as superconductivity, metamagnetism, and quantum phase transitions. We use a combination of evolutionary algorithms and density functional theory to inform traditional and in situ diffraction methods. In the course of our investigation, we find that convex hull constructions of the binary constituents inform interpretation of the ternary hull, which in this case has two compounds near thermodynamic stability. Our experimental study does not reveal formation of the candidates BaRu2S2 or BaRuS3, but it does provide the structure of a high-temperature polymorph of BaS2. This methodology can be exploited to study other ternary sys...