Probing large viscosities in glass-formers with nonequilibrium simulations [Physics]
For decades, scientists have debated whether supercooled liquids stop flowing below a glass transition temperature
Tg0 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
ηN over a range of pressures and temperatures that change
ηN 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
ηN. 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 (
⋅s). Possible experimental tests of our results are outlined.
Publisher URL: http://feedproxy.google.com/~r/Pnas-RssFeedOfEarlyEditionArticles/~3/DNiQxIF6qCk/1705978114.short
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