Configurational entropy measurements in extremely supercooled liquids that break the glass ceiling.
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Liquids relax extremely slowly on approaching the glass state. One explanation is that an entropy crisis, because of the rarefaction of available states, makes it increasingly arduous to reach equilibrium in that regime. Validating this scenario is challenging, because experiments offer limited resolution, while numerical studies lag more than eight orders of magnitude behind experimentally relevant timescales. In this work, we not only close the colossal gap between experiments and simulations but manage to create in silico configurations that have no experimental analog yet. Deploying a range of computational tools, we obtain four estimates of their configurational entropy. These measurements consistently confirm that the steep entropy decrease observed in experiments is also found in simulations, even beyond the experimental glass transition. Our numerical results thus extend the observational window into the physics of glasses and reinforce the relevance of an entropy crisis for understanding their formation.
Published Version (Please cite this version)10.1073/pnas.1706860114
Publication InfoBerthier, Ludovic; Charbonneau, Patrick; Coslovich, Daniele; Ninarello, Andrea; Ozawa, Misaki; & Yaida, Sho (2017). Configurational entropy measurements in extremely supercooled liquids that break the glass ceiling. Proceedings of the National Academy of Sciences of the United States of America, 114(43). 10.1073/pnas.1706860114. Retrieved from https://hdl.handle.net/10161/17093.
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Professor of Chemistry
Professor Charbonneau studies soft matter. His work combines theory and simulation to understand the glass problem, protein crystallization, microphase formation, and colloidal assembly in external fields.