Departamento de Física Teórica de la Materia Condensada, Universidad Autónoma de Madrid, Campus de Cantoblanco, and Condensed Matter Physics Center (IFIMAC), E-28049, Madrid, Spain.
Soft Matter. 2018 Dec 12;14(48):9937-9949. doi: 10.1039/c8sm01961d.
This work numerically investigates the diffusion of finite inert tracer particles in different types of fixed gels. The mean square displacement (MSD) of the tracers reveals a transition to subdiffusive motion MSD ∼ tα as soon as the accessible volume fraction p in the gel decreases from unity. Individual tracer dynamics reveals two types of particles in the gels: mobile tracers cross the system through percolating pores following subdiffusive dynamics MSDmob ∼ tαmob, while a fraction ptrap(p) of the particles remain trapped in finite pores. Below the void percolation threshold p < pc all the particles get trapped and α → 0. By separately studying both populations we find a simple phenomenological law for the mobile tracers αmob(p) ≈ a ln p + c where c ≈ 1 and a ∼ 0.2 depends on the gel type. On the other hand, a cluster-analysis of the gel accessible volume reveals a power law for the trapping probability ptrap ∼ (p/pc)-γ, with γ ≃ 2.9. This yields a prediction for the ensemble averaged subdiffusion exponent α = αmob(1 - ptrap). Our predictions are successfully validated against the different gels studied here and against numerical and experimental results in the literature (silica gels, polyacrylamide gels, flexible F-actin networks and in different random obstacles). Notably, the parameter a ∼ 0.2 presents small differences amongst all these cases, indicating the robustness of the proposed relation.
这项工作通过数值方法研究了有限惰性示踪粒子在不同类型固定凝胶中的扩散。示踪粒子的平均平方位移(MSD)揭示了一种转变,即一旦凝胶中的可及体积分数 p 从 1 减小,MSD 就会变为亚扩散运动 MSD∼tα。凝胶中的单个示踪剂动力学揭示了两种类型的粒子:可移动示踪剂通过贯穿亚扩散动力学 MSDmob∼tαmob 的渗透孔穿过系统,而一部分分数 ptrap(p)的粒子仍然被困在有限的孔中。在空隙渗流阈值 p<pc 以下,所有粒子都被捕获,并且α→0。通过分别研究这两种粒子,我们发现了一个简单的唯象定律,即可移动示踪剂αmob(p)≈a ln p + c,其中 c≈1,而 a∼0.2 取决于凝胶类型。另一方面,凝胶可及体积的聚类分析揭示了捕获概率 ptrap∼(p/pc)-γ 的幂律关系,其中γ≃2.9。这为系综平均亚扩散指数α=αmob(1-ptrap)提供了一个预测。我们的预测与这里研究的不同凝胶以及文献中的数值和实验结果(二氧化硅凝胶、聚丙烯酰胺凝胶、柔性 F-肌动蛋白网络和不同的随机障碍物)成功吻合。值得注意的是,所有这些情况下的参数 a∼0.2 都有很小的差异,这表明所提出的关系具有很强的稳健性。