Lutsko James F, Durán-Olivencia Miguel A
Center for Nonlinear Phenomena and Complex Systems, Code Postal 231, Université Libre de Bruxelles, Blvd. du Triomphe, 1050 Brussels, Belgium.
J Phys Condens Matter. 2015 Jun 17;27(23):235101. doi: 10.1088/0953-8984/27/23/235101. Epub 2015 May 20.
A two-variable stochastic model for diffusion-limited nucleation is developed using a formalism derived from fluctuating hydrodynamics. The model is a direct generalization of the standard classical nucleation theory (CNT). The nucleation rate and pathway are calculated in the weak-noise approximation and are shown to be in good agreement with direct numerical simulations for the weak-solution/strong-solution transition in globular proteins. We find that CNT underestimates the time needed for the formation of a critical cluster by two orders of magnitude and that this discrepancy is due to the more complex dynamics of the two variable model and not, as often is assumed, a result of errors in the estimation of the free energy barrier.
利用从涨落流体动力学推导出来的一种形式体系，开发了一种用于扩散限制成核的双变量随机模型。该模型是标准经典成核理论（CNT）的直接推广。在弱噪声近似下计算了成核速率和路径，结果表明它们与球状蛋白质中弱溶液/强溶液转变的直接数值模拟结果高度吻合。我们发现，经典成核理论低估了形成临界团簇所需时间达两个数量级，并且这种差异是由于双变量模型的动力学更为复杂，而并非如通常所认为的那样，是自由能垒估计误差的结果。
