Predicting Bulk Metallic Glass Forming Ability with the Thermodynamic Density of Competing Crystalline States

Abstract: Despite two decades of studies, the formation of metallic glasses, very promising systems for industrial applications, still remains mostly unexplained. This lack of knowledge hinders the search for new systems, still performed with combinatorial trial and error. In the past, it was speculated that some sort of "confusion" during crystallization could play a key role during their formation. In this article, we propose a heuristic descriptor quantifying such confusion. It is based on the "thermodynamic density of competing crystalline states", parameterized from high-throughput ab-initio calculations. The existence of highly enthalpy-degenerate but geometrically-different phases frustrates the crystallization process and promotes glass formation. Two test beds are considered. A good and a bad glass-former, CuZr and NiZr, are experimentally characterized with high-throughput synthesis. The experimental results corroborate the capability of the heuristic descriptor in predicting glass forming ability through the compositional space. Our analysis is expected to deepen the understanding of the underlying mechanisms and to accelerate the discovery of novel metallic glasses.