Probing large viscosities in glass-formers with nonequilibrium simulations.

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.

authors

Jadhao V,Robbins MO

doi

10.1073/pnas.1705978114

subject

Has Abstract

pub_date

2017-07-25 00:00:00

pages

7952-7957

issue

30

eissn

0027-8424

issn

1091-6490

pii

1705978114

journal_volume

114

pub_type

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