Configurational entropy measurements in extremely supercooled liquids that break the glass ceiling.

dc.contributor.author

Berthier, Ludovic

dc.contributor.author

Charbonneau, Patrick

dc.contributor.author

Coslovich, Daniele

dc.contributor.author

Ninarello, Andrea

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Ozawa, Misaki

dc.contributor.author

Yaida, Sho

dc.date.accessioned

2018-06-01T17:35:35Z

dc.date.available

2018-06-01T17:35:35Z

dc.date.issued

2017-10-10

dc.date.updated

2018-06-01T17:35:34Z

dc.description.abstract

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.

dc.identifier.issn

0027-8424

dc.identifier.issn

1091-6490

dc.identifier.uri

https://hdl.handle.net/10161/17093

dc.language

eng

dc.publisher

Proceedings of the National Academy of Sciences

dc.relation.ispartof

Proceedings of the National Academy of Sciences of the United States of America

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10.1073/pnas.1706860114

dc.subject

entropy

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glass

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relaxation

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simulation

dc.title

Configurational entropy measurements in extremely supercooled liquids that break the glass ceiling.

dc.type

Journal article

duke.contributor.orcid

Charbonneau, Patrick|0000-0001-7174-0821

pubs.issue

43

pubs.organisational-group

Trinity College of Arts & Sciences

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Duke

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Chemistry

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Physics

pubs.publication-status

Published

pubs.volume

114

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