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玻璃形成液体的“内部时钟”。

"Inner clocks" of glass-forming liquids.

作者信息

Peredo-Ortiz Ricardo, Medina-Noyola Magdaleno, Voigtmann Thomas, Elizondo-Aguilera Luis F

机构信息

Instituto de Física, Universidad Autónoma de San Luis Potosí, Av. Manuel Nava 6, Zona Universitaria, 78290 San Luis Potosí, Mexico.

Institut für Materialphysik im Weltraum, Deutsches Zentrum für Luft-und Raumfahrt (DLR), 51170 Köln, Germany and Department of Physics, Heinrich-Heine-Universität Düsseldorf, Universitätsstraße 1, 40225 Düsseldorf, Germany.

出版信息

J Chem Phys. 2022 Jun 28;156(24):244506. doi: 10.1063/5.0087649.

Abstract

Providing a physically sound explanation of aging phenomena in non-equilibrium amorphous materials is a challenging problem in modern statistical thermodynamics. The slow evolution of physical properties after quenches of control parameters is empirically well interpreted via the concept of material time (or internal clock) based on the Tool-Narayanaswamy-Moynihan model. Yet, the fundamental reasons of its striking success remain unclear. We propose a microscopic rationale behind the material time on the basis of the linear laws of irreversible thermodynamics and its extension that treats the corresponding kinetic coefficients as state functions of a slowly evolving material state. Our interpretation is based on the recognition that the same mathematical structure governs both the Tool model and the recently developed non-equilibrium extension of the self-consistent generalized Langevin equation theory, guided by the universal principles of Onsager's theory of irreversible processes. This identification opens the way for a generalization of the material-time concept to aging systems where several relaxation modes with very different equilibration processes must be considered, and partially frozen glasses manifest the appearance of partial ergodicity breaking and, hence, materials with multiple very distinct inner clocks.

摘要

在非平衡无定形材料中,对老化现象给出一个符合物理原理的解释是现代统计热力学中一个具有挑战性的问题。基于Tool-Narayanaswamy-Moynihan模型,通过材料时间(或内部时钟)的概念,淬火控制参数后物理性质的缓慢演变在经验上得到了很好的解释。然而,其显著成功的根本原因仍不清楚。我们基于不可逆热力学的线性定律及其扩展(将相应的动力学系数视为缓慢演化的材料状态的状态函数),提出了材料时间背后的微观原理。我们的解释基于这样的认识:在昂萨格不可逆过程理论的普遍原理指导下,相同的数学结构支配着Tool模型和最近发展的自洽广义朗之万方程理论的非平衡扩展。这种识别为将材料时间概念推广到老化系统开辟了道路,在这些老化系统中,必须考虑具有非常不同平衡过程的几种弛豫模式,部分冻结的玻璃表现出部分遍历性破坏的出现,因此,材料具有多个非常不同的内部时钟。

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