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在简单玻璃形成体中跳跃和斯托克斯-爱因斯坦关系的破坏。

Hopping and the Stokes-Einstein relation breakdown in simple glass formers.

机构信息

Departments of Chemistry and Physics, Duke University, Durham, NC 27708;

Departments of Chemistry and Dipartimento di Fisica, Sapienza Università di Roma, I-00185 Rome, Italy;

出版信息

Proc Natl Acad Sci U S A. 2014 Oct 21;111(42):15025-30. doi: 10.1073/pnas.1417182111. Epub 2014 Oct 6.

Abstract

One of the most actively debated issues in the study of the glass transition is whether a mean-field description is a reasonable starting point for understanding experimental glass formers. Although the mean-field theory of the glass transition--like that of other statistical systems--is exact when the spatial dimension d → ∞, the evolution of systems properties with d may not be smooth. Finite-dimensional effects could dramatically change what happens in physical dimensions,d = 2, 3. For standard phase transitions finite-dimensional effects are typically captured by renormalization group methods, but for glasses the corrections are much more subtle and only partially understood. Here, we investigate hopping between localized cages formed by neighboring particles in a model that allows to cleanly isolate that effect. By bringing together results from replica theory, cavity reconstruction, void percolation, and molecular dynamics, we obtain insights into how hopping induces a breakdown of the Stokes-Einstein relation and modifies the mean-field scenario in experimental systems. Although hopping is found to supersede the dynamical glass transition, it nonetheless leaves a sizable part of the critical regime untouched. By providing a constructive framework for identifying and quantifying the role of hopping, we thus take an important step toward describing dynamic facilitation in the framework of the mean-field theory of glasses.

摘要

在玻璃化转变的研究中,最具争议的问题之一是均场描述是否是理解实验性玻璃形成物的合理起点。尽管玻璃化转变的均场理论——就像其他统计系统一样——在空间维度 d→∞时是精确的,但系统性质随 d 的演化可能并不平滑。有限维度的影响可能会在物理维度 d=2、3 中产生显著的变化。对于标准相变,有限维度的影响通常可以通过重整化群方法来捕捉,但对于玻璃,修正则更加微妙,并且仅部分被理解。在这里,我们研究了在一个模型中相邻粒子之间形成的局部笼状的跳跃,该模型可以清晰地隔离这种效应。通过结合副本理论、腔重建、空洞渗流和分子动力学的结果,我们深入了解了跳跃如何诱导斯托克斯-爱因斯坦关系的破裂,并在实验系统中改变了均场情景。尽管跳跃被发现超越了动力学玻璃转变,但它仍然没有触及临界区域的很大一部分。通过为识别和量化跳跃的作用提供一个建设性的框架,我们因此朝着在玻璃的均场理论框架中描述动态促进作用迈出了重要的一步。

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