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对玻璃形成液体活化能的快速贡献。

Fast contribution to the activation energy of a glass-forming liquid.

作者信息

Hecksher Tina, Olsen Niels Boye, Dyre Jeppe C

机构信息

Glass and Time, IMFUFA, Department of Science and Environment, Roskilde University, DK-4000 Roskilde, Denmark

Glass and Time, IMFUFA, Department of Science and Environment, Roskilde University, DK-4000 Roskilde, Denmark.

出版信息

Proc Natl Acad Sci U S A. 2019 Aug 20;116(34):16736-16741. doi: 10.1073/pnas.1904809116. Epub 2019 Aug 7.

DOI:10.1073/pnas.1904809116
PMID:31391307
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6708330/
Abstract

This paper presents physical-aging data for the silicone oil tetramethyl-tetraphenyl trisiloxane. The density and the high-frequency plateau shear modulus [Formula: see text] were monitored following temperature jumps starting from fully equilibrated conditions. Both quantities exhibit a fast change immediately after a temperature jump. Adopting the material-time formalism of Narayanaswamy, we determine from the dielectric loss at 0.178 Hz the time evolution of the aging-rate activation energy. The relative magnitude of the fast change of the activation energy differs from that of the density, but is identical to that of [Formula: see text] In fact, the activation energy is proportional to [Formula: see text] throughout the aging process, with minor deviations at the shortest times. This shows that for the silicone oil in question the dynamics are determined by [Formula: see text] in-as well as out of-equilibrium.

摘要

本文给出了硅油四甲基-四苯基三硅氧烷的物理老化数据。从完全平衡的条件开始,在温度跃升后监测密度和高频平台剪切模量[公式:见正文]。这两个量在温度跃升后立即呈现快速变化。采用纳拉亚纳斯瓦米的材料-时间形式理论,我们从0.178赫兹的介电损耗确定老化速率活化能的时间演化。活化能快速变化的相对幅度与密度的不同,但与[公式:见正文]的相同。实际上,在整个老化过程中,活化能与[公式:见正文]成正比,在最短时间时有微小偏差。这表明对于所讨论的硅油,其动力学在平衡态和非平衡态下均由[公式:见正文]决定。

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本文引用的文献

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On the Physics Required for Prediction of Long Term Performance of Polymers and Their Composites.论预测聚合物及其复合材料长期性能所需的物理学原理。
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Does the Adam-Gibbs relation hold in simulated supercooled liquids?亚当-吉布斯关系在模拟过冷液体中成立吗?
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Phys Rev Lett. 2017 Sep 15;119(11):115703. doi: 10.1103/PhysRevLett.119.115703.
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Real space renormalization group theory of disordered models of glasses.玻璃无序模型的实空间重整化群理论
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Adam-Gibbs Formulation of Enthalpy Relaxation Near the Glass Transition.玻璃化转变附近焓松弛的亚当-吉布斯公式
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