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

Journal Article

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.

Full Text

Duke Authors

Cited Authors

  • Berthier, L; Charbonneau, P; Coslovich, D; Ninarello, A; Ozawa, M; Yaida, S

Published Date

  • October 10, 2017

Published In

Volume / Issue

  • 114 / 43

Start / End Page

  • 11356 - 11361

PubMed ID

  • 29073056

Electronic International Standard Serial Number (EISSN)

  • 1091-6490

International Standard Serial Number (ISSN)

  • 0027-8424

Digital Object Identifier (DOI)

  • 10.1073/pnas.1706860114

Language

  • eng