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   Polymers exist in the glass state for a wide range of applications. The slow and limited crystallizability of polymers means that solid polymer materials are either wholly or in part glassy, giving them great importance. The glass is a nonequilibrium amorphous state that occurs because the cooperative molecular dynamics become kinetically trapped on cooling as the available thermal energy for molecular motion decreases. This article aims to provide the reader with a molecular picture of what this packing frustration that causes glass formation means for polymers. Experimental considerations for accurately measuring the glass transition temperature 𝑇𝑔 given this nonequilibrium nature will be discussed. Basic concepts underpinning theoretical efforts to model the glass transition will be summarized to provide the reader with a lexicon and paradigm for understanding different approaches used in the field to capture the main characteristics of glasses. Current research areas of interest in polymer glasses will be briefly outlined. Hopefully, this article will provide the beginning investigator a starting point for their own studies. 

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5. Two-step devitrification of ultrastable glasses

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   Herrero, Cecilia; Scalliet, Camille; Ediger, M. D.; Berthier, Ludovic (April 2023, Proceedings of the National Academy of Sciences)

   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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