Breaking the glass ceiling: Configurational entropy measurements in extremely supercooled liquids
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 articlePermalink
https://hdl.handle.net/10161/14610Collections
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Show full item recordScholars@Duke
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
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