Design strategy for Al-containing metallic glasses by entropy engineering and covalent attribute

Traditional approaches to the composition design of metallic glasses often disregard the distinct nature of metallic and covalent interactions, leading to challenges in accurately incorporating specific elements that are more covalent and understanding their interactions. This limitation complicates the quantitative design process and hinders the development of a comprehensive theoretical framework. To address this, we propose a novel design strategy based on entropy engineering to tune metallic bonds using melting entropy, while the covalent interactions is guided by mixing enthalpy. Applying this method, we successfully designed the metallic glasses La 60.6 Ni 22.9 Al 17.5 and La 62.2 Ni 11.8 Cu 12.7 Al 13.2 whose GFA is highly consistent with the reported components. • Introduced a phase-based approach for glass design. • Applied mixing ehthalpy to achieve low entropy in a covalent glass forming system. • Demonstrated that melting entropy is a versatile criterion applicable across simple force system. • Provided new guidelines and strategies for designing glass systems with covalent elements.