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Journal Articles Proceedings of the National Academy of Sciences of the United States of America Year : 2023

Two-step devitrification of ultrastable glasses


The discovery of ultrastable glasses raises novel challenges about glassy systems. Recent experiments studied the macroscopic devitrification of ultrastable glasses into liquids upon heating but lacked microscopic resolution. We use molecular dynamics simulations to analyze the kinetics of this transformation. In the most stable systems, devitrification occurs after a very large time, but the liquid emerges in two steps. At short times, we observe the rare nucleation and slow growth of isolated droplets containing a liquid maintained under pressure by the rigidity of the surrounding glass. At large times, pressure is released after the droplets coalesce into large domains, which accelerates devitrification. This two-step process produces pronounced deviations from the classical Avrami kinetics and explains the emergence of a giant lengthscale characterizing the devitrification of bulk ultrastable glasses. Our study elucidates the nonequilibrium kinetics of glasses following a large temperature jump, which differs from both equilibrium relaxation and aging dynamics, and will guide future experimental studies.
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hal-04117704 , version 1 (05-06-2023)



Cecilia Herrero, Camille Scalliet, M. Ediger, Ludovic Berthier. Two-step devitrification of ultrastable glasses. Proceedings of the National Academy of Sciences of the United States of America, 2023, 120 (16), ⟨10.1073/pnas.2220824120⟩. ⟨hal-04117704⟩
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