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Breaking the glass ceiling: Configurational entropy measurements in extremely supercooled liquids

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Date
2017-06-01
Authors
Berthier, Ludovic
Charbonneau, Patrick
Coslovich, Daniele
Ninarello, Andrea
Ozawa, M
Yaida, Sho
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Abstract
Liquids relax extremely slowly on approaching the glass state. One explanation is that an entropy crisis, due to 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 found also in simulations even beyond the experimental glass transition. Our numerical results thus open a new observational window into the physics of glasses and reinforce the relevance of an entropy crisis for understanding their formation.
Type
Journal article
Subject
cond-mat.stat-mech
cond-mat.stat-mech
cond-mat.soft
Permalink
https://hdl.handle.net/10161/14610
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Scholars@Duke

Charbonneau

Patrick Charbonneau

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.

Sho Yaida

Postdoctoral Associate
Alphabetical list of authors with Scholars@Duke profiles.
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