Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, United Kingdom.
J Chem Phys. 2011 Aug 14;135(6):065106. doi: 10.1063/1.3608917.
Nucleated polymerisation processes are involved in many growth phenomena in nature, including the formation of cytoskeletal filaments and the assembly of sickle hemoglobin and amyloid fibrils. Closed form rate equations have, however, been challenging to derive for these growth phenomena in cases where secondary nucleation processes are active, a difficulty exemplified by the highly non-linear nature of the equation systems that describe monomer dependent secondary nucleation pathways. We explore here the use of fixed point analysis to provide self-consistent solutions to such growth problems. We present iterative solutions and discuss their convergence behaviour. We establish a range of closed form results for linear growth processes, including the scaling behaviours of the maximum growth rate and of the reaction end-point. We further show that a self-consistent approach applied to the master equation of filamentous growth allows the determination of the evolution of the shape of the length distribution including the mean, the standard deviation, and the mode. Our results highlight the power of fixed-point approaches in finding closed form self-consistent solutions to growth problems characterised by the highly non-linear master equations.
成核聚合过程涉及自然界中的许多生长现象,包括细胞骨架丝的形成以及镰刀状血红蛋白和淀粉样纤维的组装。然而,在二次成核过程活跃的情况下,对于这些生长现象,很难推导出闭式速率方程,这一难题的一个例子是描述单体依赖性二次成核途径的方程组具有高度非线性的性质。我们在这里探讨使用不动点分析来为这些生长问题提供自洽解。我们提出了迭代解,并讨论了它们的收敛行为。我们为线性生长过程建立了一系列闭式结果,包括最大增长率和反应终点的标度行为。我们进一步表明,将自洽方法应用于丝状生长的主方程可以确定长度分布形状的演化,包括平均值、标准差和模式。我们的结果强调了不动点方法在寻找高度非线性主方程所描述的生长问题的闭式自洽解方面的强大功能。