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We report a metadynamics simulation study of crystallization in a deepundercooled metallic glass-forming liquid by developing appropriate collectivevariables. Through a combined analysis of free energy surface (FES) andatomic-level behaviors, a picture of an abnormal-endothermic crystallizationprocess is revealed: rejuvenated disorder states with less localfivefold-symmetry and fast dynamics form firstly by changing the local chemicalorder around Cu atoms, which then act as the precursor for the nucleation ofwell-ordered crystallites. This process reflects a complex energy landscapewith well-separated glassy and crystal basins, giving rise to the directevidence of intrinsic frustration against crystallization in deep undercooledmetallic glass forming liquids. Moreover, the rejuvenated disorder states withdistinct physical behaviors offer great opportunities to tailor theperformances of metallic glass by controlling the thermal history of a metallicmelt.

Revealing Rejuvenated Disorder States towards Crystallization in a Supercooled Metallic Glass-Forming Liquid