论文标题
粘液粘性聚合物的拥挤溶液中的示踪剂扩散
Tracer diffusion in crowded solutions of sticky polymers
论文作者
论文摘要
在强限的几何形状和拥挤的环境中,大分子扩散在很大程度上仍然是软物质物理和生物学中的开放主题。在本文中,我们采用大规模的langevin动力学模拟来研究示踪剂的扩散如何受到排除体积和弱吸引人的Crowder-Tracer-Tracer相互作用的合并作用的影响。我们考虑了两种示踪剂,这些示踪剂是由几周的chandler-Andersen(WCA)排斥潜力和核心软化(CS)颗粒所描述的,例如,这些颗粒,例如球状蛋白,带电的胶体和纳米颗粒,由聚合物刷覆盖。这些系统的特征是相互作用中存在两个长度尺度,并且由于不同长度尺度之间的固有竞争,可以在扩散中表现出水样异常。在这里,我们报告了这两个示踪剂物种的扩散和结构的全面研究,该环境由聚合物的淬火构型以增加密度的增加而拥挤。我们详细分析了与特定的静态空间相关性的出现相比,示踪剂聚合物亲和力和系统密度如何影响传输。特别是,我们发现,尽管WCA和CS颗粒的扩散特性几乎没有出现任何差异,但对于CS颗粒而言,开发大量拥挤的结构顺序的倾向却非常沮丧。出乎意料的是,对于对拥挤矩阵的足够亲和力,WCA示踪剂的扩散系数显示出非单调趋势,因为与零亲和力方案相比,它们的密度增加。事实证明,这种水样的异常比CS粒子观察到的还要大,并且似乎植根于排除体积和亲和力效应之间的类似竞争。
Macromolecular diffusion in strongly confined geometries and crowded environments is still to a large extent an open subject in soft matter physics and biology. In this paper, we employ large-scale Langevin dynamics simulations to investigate how the diffusion of a tracer is influenced by the combined action of excluded-volume and weak attractive crowder-tracer interactions. We consider two species of tracers, standard hard-core particles described by the Weeks-Chandler-Andersen (WCA) repulsive potential and core-softened (CS) particles, which model, e.g., globular proteins, charged colloids and nanoparticles covered by polymeric brushes. These systems are characterized by the presence of two length scales in the interaction and can show water-like anomalies in their diffusion, stemming from the inherent competition between different length scales. Here we report a comprehensive study of both diffusion and structure of these two tracer species in an environment crowded by quenched configurations of polymers at increasing density. We analyze in detail how the tracer-polymer affinity and the system density affect transport as compared to the emergence of specific static spatial correlations. In particular, we find that, while hardly any differences emerge in the diffusion properties of WCA and CS particles, the propensity to develop structural order for large crowding is strongly frustrated for CS particles. Surprisingly, for large enough affinity for the crowding matrix, the diffusion coefficient of WCA tracers display a non-monotonic trend as their density is increased when compared to the zero affinity scenario. This water-like anomaly turns out to be even larger than what observed for CS particle and appears to be rooted in a similar competition between excluded-volume and affinity effects.