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arXiv · 2608.20536

Reversing strain deformations probe mechanisms for enhanced segmental mobility of polymer glasses

Kelly Hebert·M. D. Ediger
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Abstract

Optical probe reorientation measurements were performed to monitor changes in segmental dynamics resulting from the nonlinear deformation of a polymer glass. Segmental dynamics were monitored in a poly(methyl methacrylate) glass near Tg before and after a series of reversing deformations in which the sample was extended at constant strain rate and then allowed to retract back to zero stress at constant strain rate. Evidence of a rejuvenation mechanism, as quantified by a departure of the segmental dynamics from the quiescent aging dynamics after the reversing deformation, is observed for deformations which reach 60% of the yield strain or greater. By this measure, a saturation of the rejuvenation mechanism is not observed until at least five times the yield strain. For comparison, purely mechanical measurements of rejuvenation, based upon the reduction of the yield stress in a subsequent deformation, were also performed. These purely mechanical experiments show broad qualitative agreement with the probe reorientation experiments, but quantitatively differ in the pre-yield regime. The results are discussed in the context of recent theoretical approaches and simulations which provide a molecular-level description of polymer glass deformation.

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Kelly Hebert, M. D. Ediger. 2026-08-20. Reversing strain deformations probe mechanisms for enhanced segmental mobility of polymer glasses. https://doi.org/10.1021/acs.macromol.6b02490

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