Predicting nonlinear physical aging of glasses from equilibrium relaxation via the material time

Abstract

The noncrystalline glassy state of matter plays a role in virtually all fields of materials science and offers complementary properties to those of the crystalline counterpart. The caveat of the glassy state is that it is out of equilibrium and therefore exhibits physical aging, i.e., material properties change over time. For half a century, the physical aging of glasses has been known to be described well by the material-time concept, although the existence of a material time has never been directly validated. We do this here by successfully predicting the aging of the molecular glass 4-vinyl-1,3-dioxolan-2-one from its linear relaxation behavior. This establishes the defining property of the material time. Via the fluctuation-dissipation theorem, our results imply that physical aging can be predicted from thermal-equilibrium fluctuation data, which is confirmed by computer simulations of a binary liquid mixture.

Published in Science Advances

References in corpus (5)

• Glassy Aging Dynamics
• Temperature development of glassy alpha-relaxation dynamics determined by broadband dielectric spectroscopy
• Microscopic origin of excess wings in relaxation spectra of supercooled liquids
• Aging in thermal active glasses
• A molecular perspective on the yield and flow of polymer glasses: The role of enhanced segmental dynamics during active deformation

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• Non-linear physical aging of supercooled glycerol induced by large upward ideal temperature steps monitored through cooling experiments
• Single parameter aging and density scaling
• Clever algorithms for glasses work by time reparametrization
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• Initial Stages of Rejuvenation of Vapor-Deposited Glasses during Isothermal Annealing: Contrast Between Experiment and Simulation
• Linear-limit aging times of three monoalcohols
• Large temperature-up-jump simulations of a binary Lennard-Jones system
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