文章基本信息

标题：Configurational entropy measurements in extremely supercooled liquids that break the glass ceiling
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作者：Ludovic Berthier ; Patrick Charbonneau ; Daniele Coslovich 等
期刊名称：Proceedings of the National Academy of Sciences
印刷版ISSN：0027-8424
电子版ISSN：1091-6490
出版年度：2017
卷号：114
期号：43
页码：11356-11361
DOI：10.1073/pnas.1706860114
语种：English
出版社：The National Academy of Sciences of the United States of America
摘要：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.
关键词：glass ; relaxation ; entropy ; simulation