SearcharxivSearch

arXiv subjects

Enran Xing

Publications and source records attributed to Enran Xing.

4 recordsLinked to original sources

Rejuvenation versus overaging: The effect of cyclic loading/unloading on the segmental dynamics of PMMA glasses

The acceleration of structural relaxation or physical aging by deformation, known as overaging, has been reported in experiments and simulations of polymer and colloid glasses, and correctly accounting for overaging is important for the prediction of the long-term behavior of polymer glasses in engineering applications. Here the effects of cyclic loading/unloading on the segmental dynamics and mechanical properties of PMMA glasses are investigated using a probe reorientation technique and time-aging time superposition of the mechanical response, respectively. Sets of 5000 tensile loading/unloading cycles were performed at temperatures between Tg - 10 K and Tg - 25 K with cycle extension strains ranging from 0.003 to 0.007. After cycling, the segmental dynamics measured with the probe reorientation technique either remained unchanged or were faster relative to an undeformed sample. The relaxation times of cycled glasses recovered with a common time scale on the order of their aging time, indicating that they retain a memory of their original age, as opposed to a full erasure of their thermal and mechanical history. Surprisingly, changes as a result of cycling were more obvious in probe reorientation measurements than in the mechanical properties, suggesting that the probe reorientation technique can sensitively detect nonlinear effects of deformation. No evidence of overaging was observed in the optical or mechanical measurements as a result of these cyclic loading/unloading experiments.

cond-mat.soft

Multi-step deformation experiment and development of a model for the mechanical behavior of polymeric glasses

Traditional models for stress-strain behavior of glassy polymers are based on the assumption that the critical features of the stress-strain response can be explained by changes in the molecular mobility. The four-step deformation experiments consisting of (i) an initial constant strain rate loading, (ii) unloading to specified stress, (iii) creep under that stress and (iv) second constant strain rate loading, challenges that assumption. Specifically, existing models fail to predict the experimentally observed large second stress overshoot in case of a slight unloading. Until now there has remained a possibility that the mobility was actually lower in case of a partial rather than complete unloading, which would preserve the main assumption, if not particular details, of these specific constitutive models. By performing direct optical experiments using the photobleaching technique simultaneously with the mechanical four-step experiments it is shown that a lower molecular mobility upon partial unloading does not take place. As traditional models cannot account for these experimental results, a new model has been developed where the changes of molecular structure manifest not in the relaxation time, but in the shear modulus, which is function of an internal variable that is the fraction of the efficiently packed material. This fraction obeys a population balance equation, where the steady-state fraction is controlled by the applied stress. In the absence of deformation, the efficiently packed fraction increases, which explains the increase in the modulus in the course of physical aging below Tg. The model qualitatively describes the four-step experiment as well as single step loading experiments.

cond-mat.soft

Overaging with stress in polymer glasses? Faster segmental dynamics despite larger yield stress!

It is well known that physical aging of polymer glasses increases their yield stress and affects their failure behavior. Studies indicate that application of moderate levels of stress during aging results in higher yield stress compared to aging in the absence of stress (quiescent aging). This has been interpreted to indicate that stress accelerates physical aging, and has been described as overaging. In this study, we age PMMA glasses under stress, and carry out direct measurement of segmental dynamics during and after aging by using a probe reorientation technique. We observe that samples aged under stress, despite having higher yield stress, have faster segmental dynamics after stress release than quiescently aged samples. This contradicts the overaging interpretation, for the range of conditions explored here. Our results indicate that yield stress is not a simple function of structural relaxation time and theoretical models based on this understanding need to be revised.

cond-mat.soft

Segmental Dynamics in the Strain-hardening Regime for Poly(methyl methacrylate) Glasses with and without Melt-stretching

Strain-hardening is a feature of polymer glasses during large deformation, which helps to stabilize the glasses against breakage. Experimentally, little is known about the segmental dynamics during strain-hardening, and such data is important for building a molecular-level theory of polymer glasses deformed in this regime. Here, using a photobleaching technique, we measured the segmental dynamics of lightly-crosslinked poly(methyl methacrylate) (PMMA) glasses with and without melt-stretching, which were deformed into the strain-hardening regime with local engineering strain rates from 10^-4.6 s^-1 to 10^-4 s^-1 at Tg-23K and Tg-33K. We find that melt-stretched PMMA glasses show a more prominent strain-hardening feature and faster segmental dynamics by a factor of about 15% compared to PMMA without melt-stretching. At a given true strain rate, the segmental dynamics of PMMA without melt-stretching are accelerated in the deep strain-hardening regime from the value just beyond yield, by up to 40% at 0.8 true strain. Our observations are in agreement with previously published simulation results.

cond-mat.soft