Unique Energy‐Storage Behavior Driven by High Entropy in Metallic Glasses

Abstract The rejuvenation or energy‐storage behavior in metallic glasses (MGs) has been extensively explored for its theoretical and practical significance. However, very limited research focuses on the rejuvenation of high entropy metallic glasses (HEMGs), leaving uncertainties about how configurational entropy influences this process. In this study, cryogenic temperature cycling (CTC) is utilized to unlock the rejuvenation potential of a series of La‐based MGs with different entropy values. Comparative analysis of these MGs reveals that increased entropy boosts the maximum rejuvenation degree from 37% to 65% and widens the range of energy states where rejuvenation occurs. The changed rejuvenation behavior induced by entropy increase, which has never been reported other studies, are related to glass's structures, fragility and coupling degree between β and α relaxations. Besides, a new rejuvenation mechanism is revealed in HEMGs, which differs significantly from unrestricted growth and interconnection of flow units observed in most MGs. The atomic motion in HEMGs is confined within the icosahedral backbone network during CTC. Surprisingly, this local motion can propagate through strong interactions between adjacent atoms, facilitating the activation of α relaxation. These discoveries offer novel approaches to tune energy‐storage behavior of MGs by modulating icosahedral network structures through entropy control.