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胶体动力学自洽广义朗之万方程中的动态阻滞

Dynamic arrest within the self-consistent generalized Langevin equation of colloid dynamics.

作者信息

Yeomans-Reyna L, Chávez-Rojo M A, Ramírez-González P E, Juárez-Maldonado R, Chávez-Páez M, Medina-Noyola M

机构信息

Departamento de Física, Universidad de Sonora, Boulevard Luis Encinas y Rosales, 83000, Hermosillo, Sonora, Mexico.

出版信息

Phys Rev E Stat Nonlin Soft Matter Phys. 2007 Oct;76(4 Pt 1):041504. doi: 10.1103/PhysRevE.76.041504. Epub 2007 Oct 22.

Abstract

This paper presents a recently developed theory of colloid dynamics as an alternative approach to the description of phenomena of dynamic arrest in monodisperse colloidal systems. Such theory, referred to as the self-consistent generalized Langevin equation (SCGLE) theory, was devised to describe the tracer and collective diffusion properties of colloidal dispersions in the short- and intermediate-time regimes. Its self-consistent character, however, introduces a nonlinear dynamic feedback, leading to the prediction of dynamic arrest in these systems, similar to that exhibited by the well-established mode coupling theory of the ideal glass transition. The full numerical solution of this self-consistent theory provides in principle a route to the location of the fluid-glass transition in the space of macroscopic parameters of the system, given the interparticle forces (i.e., a nonequilibrium analog of the statistical-thermodynamic prediction of an equilibrium phase diagram). In this paper we focus on the derivation from the same self-consistent theory of the more straightforward route to the location of the fluid-glass transition boundary, consisting of the equation for the nonergodic parameters, whose nonzero values are the signature of the glass state. This allows us to decide if a system, at given macroscopic conditions, is in an ergodic or in a dynamically arrested state, given the microscopic interactions, which enter only through the static structure factor. We present a selection of results that illustrate the concrete application of our theory to model colloidal systems. This involves the comparison of the predictions of our theory with available experimental data for the nonergodic parameters of model dispersions with hard-sphere and with screened Coulomb interactions.

摘要

本文提出了一种最近发展起来的胶体动力学理论,作为描述单分散胶体系统中动态阻滞现象的另一种方法。这种理论,称为自洽广义朗之万方程(SCGLE)理论,旨在描述胶体分散体在短时间和中间时间范围内的示踪剂扩散和集体扩散特性。然而,其自洽特性引入了非线性动态反馈,导致预测这些系统中会出现动态阻滞,这与成熟的理想玻璃化转变模式耦合理论所表现出的情况类似。给定粒子间作用力(即平衡相图统计热力学预测的非平衡类似物),该自洽理论的完整数值解原则上提供了一条在系统宏观参数空间中确定流体 - 玻璃转变位置的途径。在本文中,我们专注于从同一自洽理论推导出确定流体 - 玻璃转变边界的更直接途径,该途径由非遍历参数方程组成,其非零值是玻璃态的标志。这使我们能够在给定微观相互作用(仅通过静态结构因子进入)的情况下,判断在给定宏观条件下系统处于遍历态还是动态阻滞态。我们展示了一系列结果,这些结果说明了我们的理论在模拟胶体系统中的具体应用。这涉及将我们理论的预测与具有硬球和屏蔽库仑相互作用的模型分散体非遍历参数的现有实验数据进行比较。

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