Mixed Enthalpy–Entropy Descriptor for the Rational Design of Synthesizable High-Entropy Materials

As the exploration of novel materials composed of just two or three elements reaches its combinatorial limits, high-entropy materials (HEMs) have emerged as a promising platform for functional materials design and discovery. Over the past two decades, extensive research efforts have been directed toward developing new functional HEMs and identifying predictive composition-structure-synthesis relationships. However, progress in this area remains slow and limited, largely due to the lack of effective methods for distinguishing the relative synthesizability of HEMs among different polymorphs and element combinations. In this talk, we will introduce the mixed enthalpy-entropy descriptor (MEED), a 2D vector descriptor for predicting polymorph-dependent synthesizability. MEED can be easily and rapidly computed entirely from first principles and is adaptable for high-throughput screening of synthesizable HEMs across large chemical spaces. It also enables the simultaneous exploration of synthesizability trends across various polymorphs and compositions. We demonstrate the efficacy of MEED through two material systems: cubic high-entropy metal carbides and 2D high-entropy transition metal chalcogenides (2D-HETMCs) in three distinct polymorphs—2H, 1T, and 1T'. From thousands of element combinations screened, we identified dozens of highly synthesizable HEMs in each system. These new HEMs will be presented alongside experimental validations. Emerging insights into the intricate relationships between composition, structure, and synthesis will also be discussed.