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用于连接子介导的不可逆聚集的斯莫卢霍夫斯基方程。

Smoluchowski equations for linker-mediated irreversible aggregation.

作者信息

Tavares J M, Antunes G C, Dias C S, Telo da Gama M M, Araújo N A M

机构信息

Centro de Física Teórica e Computacional, Universidade de Lisboa, 1749-016 Lisboa, Portugal.

出版信息

Soft Matter. 2020 Aug 19;16(32):7513-7523. doi: 10.1039/d0sm00674b.

Abstract

We developed a generalized Smoluchowski framework to study linker-mediated aggregation, where linkers and particles are explicitly taken into account. We assume that the bonds between linkers and particles are irreversible, and that clustering occurs through limited diffusion aggregation. The kernel is chosen by analogy with single-component diffusive aggregation but the clusters are distinguished by their number of particles and linkers. We found that the dynamics depends on three relevant factors, all tunable experimentally: (i) the ratio of the diffusion coefficients of particles and linkers; (ii) the relative number of particles and linkers; and (iii) the maximum number of linkers that may bond to a single particle. To solve the Smoluchoski equations analytically we employ a scaling hypothesis that renders the fraction of bondable sites of a cluster independent of the size of the cluster, at each instant. We perform numerical simulations of the corresponding lattice model to test this hypothesis. We obtain results for the asymptotic limit, and the time evolution of the bonding probabilities and the size distribution of the clusters. These findings are in agreement with experimental results reported in the literature and shed light on unexplained experimental observations.

摘要

我们开发了一个广义的斯莫卢霍夫斯基框架来研究连接体介导的聚集,其中明确考虑了连接体和粒子。我们假设连接体与粒子之间的键是不可逆的,并且聚集是通过有限扩散聚集发生的。内核的选择类似于单组分扩散聚集,但聚集体通过其粒子和连接体的数量来区分。我们发现动力学取决于三个相关因素,所有这些因素都可以通过实验进行调节:(i)粒子和连接体的扩散系数之比;(ii)粒子和连接体的相对数量;以及(iii)可与单个粒子结合的连接体的最大数量。为了解析求解斯莫卢霍夫斯基方程,我们采用了一种标度假设,即在每个时刻,聚集体的可键合位点分数与聚集体大小无关。我们对相应的晶格模型进行了数值模拟以检验这一假设。我们得到了渐近极限、键合概率的时间演化以及聚集体大小分布的结果。这些发现与文献中报道的实验结果一致,并为未解释的实验观察提供了启示。

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