Garcia Gonzalo A, Cohen Samuel I A, Dobson Christopher M, Knowles Tuomas P J
Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, United Kingdom.
Phys Rev E Stat Nonlin Soft Matter Phys. 2014 Mar;89(3):032712. doi: 10.1103/PhysRevE.89.032712. Epub 2014 Mar 24.
The self-assembly of biomolecules, such as peptides and proteins, into filaments is conventionally understood as a nucleated polymerization reaction. However, detailed analysis of experimental observation has revealed recently that nucleation pathways generate growth-competent nuclei via a cascade of metastable intermediate species, which are omitted in conventional models of filamentous growth based on classical nucleation theory. Here we take an analytical approach to generalizing the classical theory of nucleated polymerization to include the formation of these prenucleation clusters, providing a quantitative general classification of the behavior exhibited by these nucleation-conversion-polymerization reactions. A phase diagram is constructed, and analytical predictions are derived for key experimental observables. Using this approach, we delineate the characteristic time scales that determine the nature of biopolymer growth phenomena.
生物分子（如肽和蛋白质）自组装成细丝通常被理解为一种成核聚合反应。然而，最近对实验观察的详细分析表明，成核途径通过一系列亚稳态中间物种产生具有生长能力的核，而基于经典成核理论的丝状生长传统模型中忽略了这些物种。在这里，我们采用一种分析方法，将经典的成核聚合理论推广到包括这些预成核簇的形成，为这些成核-转化-聚合反应所表现出的行为提供定量的一般分类。构建了一个相图，并推导了关键实验可观测量的分析预测。使用这种方法，我们描绘了决定生物聚合物生长现象本质的特征时间尺度。
