Literature DB >> 28696320

Probing large viscosities in glass-formers with nonequilibrium simulations.

Vikram Jadhao1,2, Mark O Robbins3.   

Abstract

For decades, scientists have debated whether supercooled liquids stop flowing below a glass transition temperature [Formula: see text] or whether motion continues to slow gradually down to zero temperature. Answering this question is challenging because human time scales set a limit on the largest measurable viscosity, and available data are equally well fit to models with opposite conclusions. Here, we use short simulations to determine the nonequilibrium shear response of a typical glass-former, squalane. Fits of the data to an Eyring model allow us to extrapolate predictions for the equilibrium Newtonian viscosity [Formula: see text] over a range of pressures and temperatures that change [Formula: see text] by 25 orders of magnitude. The results agree with the unusually large set of equilibrium and nonequilibrium experiments on squalane and extend them to higher [Formula: see text] Studies at different pressures and temperatures are inconsistent with a diverging viscosity at finite temperature. At all pressures, the predicted viscosity becomes Arrhenius with a single temperature-independent activation barrier at low temperatures and high viscosities ([Formula: see text] Pa[Formula: see text]s). Possible experimental tests of our results are outlined.

Entities:  

Keywords:  glass transition; molecular dynamics simulations; nonequilibrium systems; rheology; supercooled liquids

Year:  2017        PMID: 28696320      PMCID: PMC5544323          DOI: 10.1073/pnas.1705978114

Source DB:  PubMed          Journal:  Proc Natl Acad Sci U S A        ISSN: 0027-8424            Impact factor:   11.205


  17 in total

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Authors:  G Tarjus; D Kivelson; S Mossa; C Alba-Simionesco
Journal:  J Chem Phys       Date:  2004-04-01       Impact factor: 3.488

2.  Direct experimental evidence of a growing length scale accompanying the glass transition.

Authors:  L Berthier; G Biroli; J-P Bouchaud; L Cipelletti; D El Masri; D L'Hôte; F Ladieu; M Pierno
Journal:  Science       Date:  2005-12-16       Impact factor: 47.728

Review 3.  Theory of structural glasses and supercooled liquids.

Authors:  Vassiliy Lubchenko; Peter G Wolynes
Journal:  Annu Rev Phys Chem       Date:  2007       Impact factor: 12.703

4.  Corresponding states of structural glass formers.

Authors:  Yael S Elmatad; David Chandler; Juan P Garrahan
Journal:  J Phys Chem B       Date:  2009-04-23       Impact factor: 2.991

5.  Formation of glasses from liquids and biopolymers.

Authors:  C A Angell
Journal:  Science       Date:  1995-03-31       Impact factor: 47.728

6.  In search of a theory of supercooled liquids.

Authors:  Steven A Kivelson; Gilles Tarjus
Journal:  Nat Mater       Date:  2008-11       Impact factor: 43.841

7.  AIREBO-M: a reactive model for hydrocarbons at extreme pressures.

Authors:  Thomas C O'Connor; Jan Andzelm; Mark O Robbins
Journal:  J Chem Phys       Date:  2015-01-14       Impact factor: 3.488

8.  Using 20-million-year-old amber to test the super-Arrhenius behaviour of glass-forming systems.

Authors:  Jing Zhao; Sindee L Simon; Gregory B McKenna
Journal:  Nat Commun       Date:  2013       Impact factor: 14.919

9.  Novel approach to numerical measurements of the configurational entropy in supercooled liquids.

Authors:  Ludovic Berthier; Daniele Coslovich
Journal:  Proc Natl Acad Sci U S A       Date:  2014-07-28       Impact factor: 11.205

10.  Growth rate of crystalline ice and the diffusivity of supercooled water from 126 to 262 K.

Authors:  Yuntao Xu; Nikolay G Petrik; R Scott Smith; Bruce D Kay; Greg A Kimmel
Journal:  Proc Natl Acad Sci U S A       Date:  2016-12-12       Impact factor: 11.205

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  3 in total

1.  Purported fragile-to-Arrhenius crossover in squalane.

Authors:  Scott Bair
Journal:  Proc Natl Acad Sci U S A       Date:  2017-10-03       Impact factor: 11.205

2.  Reply to Bair: Crossover to Arrhenius behavior at high viscosities in squalane.

Authors:  Vikram Jadhao; Mark O Robbins
Journal:  Proc Natl Acad Sci U S A       Date:  2017-10-03       Impact factor: 11.205

3.  Effect of lubricants on the rotational transmission between solid-state gears.

Authors:  Huang-Hsiang Lin; Jonathan Heinze; Alexander Croy; Rafael Gutiérrez; Gianaurelio Cuniberti
Journal:  Beilstein J Nanotechnol       Date:  2022-01-05       Impact factor: 3.649

  3 in total

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