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不可逆凝胶化模型中的静态和动态非均质性。

Static and dynamic heterogeneities in a model for irreversible gelation.

作者信息

Abete T, de Candia A, Del Gado E, Fierro A, Coniglio A

机构信息

Dipartimento di Scienze Fisiche, Università degli Studi di Napoli Federico II, INFN, CNR-INFM Coherentia and CNISM, via Cinthia, 80126 Naples, Italy.

出版信息

Phys Rev Lett. 2007 Feb 23;98(8):088301. doi: 10.1103/PhysRevLett.98.088301. Epub 2007 Feb 22.

Abstract

We study the structure and the dynamics in the formation of irreversible gels by means of molecular dynamics simulation of a model system where the gelation transition is due to the random percolation of permanent bonds between neighboring particles. We analyze the heterogeneities of the dynamics in terms of the fluctuations of the self-intermediate scattering functions: in the sol phase close to the percolation threshold, we find that this dynamic susceptibility increases with the time until it reaches a plateau. At the gelation threshold this plateau scales as a function of the wave vector k as k(eta-2), with eta being related to the decay of the percolation pair connectedness function. At the lowest wave vector, approaching the gelation threshold it diverges with the same exponent gamma as the mean cluster size. These findings suggest an alternative way of measuring critical exponents in a system undergoing chemical gelation.

摘要

我们通过对一个模型系统进行分子动力学模拟,研究不可逆凝胶形成过程中的结构和动力学。在该模型系统中,凝胶化转变是由于相邻粒子之间永久键的随机渗流所致。我们根据自中间散射函数的涨落来分析动力学的不均匀性:在接近渗流阈值的溶胶相中,我们发现这种动态磁化率随时间增加,直至达到一个平稳期。在凝胶化阈值处,这个平稳期作为波矢k的函数按k(η - 2)缩放,其中η与渗流对连通函数的衰减有关。在最低波矢处,接近凝胶化阈值时,它以与平均簇尺寸相同的指数γ发散。这些发现提出了一种在经历化学凝胶化的系统中测量临界指数的替代方法。

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