Defect-Informed Figure of Merit for the High-Throughput Screening of New High-Entropy Materials

Single-phase high-entropy materials (HEM) consisting of at least five elements in nearly equiatomic ratios constitute an enormously large but least explored compositional space. Over recent years, these materials have gained significant and increasing interest due to their potential applications and remarkable functional properties. Despite considerable progress has been made in understanding the salient features of these materials, predictive composition-structure-property relationships are rare, and the prediction of new HEM remains a grand challenge. In this work, we propose a new physical descriptor or figure of merit that can enable high-throughput screening of single-phase HEM. Based on the energy distribution spectrum of various defect configurations, this descriptor measures the relative propensity of forming random chemical disorders in a single phase. Applying this descriptor to disordered refectory five-metal carbides, all experimentally synthesized ones in single phase have been successfully identified and separated from specific elemental combinations that are formed as multiple phases. This method can also be extended to the search for new higher-order (six or more metal elements) high-entropy systems without increasing computational costs.<br/>This is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award Number DE-SC0021127.