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

Proceedings of the National Academy of Sciences of the United States of America
Ludovic BerthierSho Yaida

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.

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Citations

Feb 21, 2018·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Daniele CoslovichLudovic Berthier
Dec 24, 2017·The Journal of Chemical Physics·Harukuni IkedaAtsushi Ikeda
Jan 18, 2018·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Ian WilliamsC Patrick Royall
Jul 5, 2018·Journal of Physics. Condensed Matter : an Institute of Physics Journal·C Patrick RoyallJoshua Robinson
Nov 14, 2019·Soft Matter·Luca CipellettiLaurence Ramos
Jan 4, 2019·Nature Communications·Lijin WangElijah Flenner
Jan 27, 2019·Scientific Reports·Douglas M Reitz, Estela Blaisten-Barojas
Apr 20, 2019·Physical Review. E·Ludovic BerthierJoyjit Kundu
Sep 1, 2019·The Journal of Chemical Physics·Misaki OzawaLudovic Berthier
Sep 11, 2020·Physical Review Letters·Anshul D S ParmarLudovic Berthier
Oct 22, 2018·The Journal of Chemical Physics·Misaki OzawaLudovic Berthier
Jan 3, 2019·The Journal of Chemical Physics·Guillaume Bareigts, Christophe Labbez
Mar 10, 2019·The Journal of Chemical Physics·Ludovic BerthierGilles Tarjus
Sep 7, 2020·The Journal of Chemical Physics·C Patrick RoyallThomas Speck
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Jan 24, 2019·Proceedings of the National Academy of Sciences of the United States of America·Elijah Flenner, Grzegorz Szamel
Jan 10, 2019·Nature Communications·Erin G TeichSharon C Glotzer
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Oct 10, 2020·The Journal of Chemical Physics·Anshul D S ParmarLudovic Berthier
Nov 21, 2020·Physical Review. E·Benjamin GuiselinGilles Tarjus
Dec 16, 2020·The Journal of Chemical Physics·Benjamin GuiselinLudovic Berthier
Apr 3, 2021·Proceedings of the National Academy of Sciences of the United States of America·Yuliang Jin, Hajime Yoshino
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Jul 5, 2019·The Journal of Physical Chemistry Letters·M S BeasleyM D Ediger
Sep 4, 2021·Physical Review Letters·Ludovic Berthier

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