GPM, UMR CNRS 6634 BP 12, Université de Rouen, Avenue de l'Université 76801 Saint Etienne de Rouvray, France.
J Chem Phys. 2011 Oct 7;135(13):134508. doi: 10.1063/1.3644935.
Nucleation in a two-component incompressible system was studied by examining the topology of the free-energy landscape. The properties of a single nucleus during nucleation were derived from the minimum free-energy pathway (MFEP) within the Cahn-Hilliard continuum theory of nucleation. MFEPs were computed using the string method. In particular, we have provided a detailed description of the nucleation process for a regular solution (T/T(c) = 0.8656) for increasing supersaturation up to the spinodal line. Two original results were found in terms of the physics of nucleation. A universal two-step behaviour was found whatever the supersaturation: nuclei sharply enrich up to equilibrium and then grow. Embryos show diffuse interfaces along the MFEP. The width of interfaces quickly saturates to its value at the critical nuclei and stays constant afterwards.
通过研究自由能景观的拓扑结构,研究了双组份不可压缩体系中的成核现象。通过成核的 Cahn-Hilliard 连续体理论,从最小自由能途径 (MFEP) 推导出成核过程中单核的性质。使用弦方法计算 MFEP。特别是,我们详细描述了过饱和度增加到旋节线时的正溶液(T/T(c) = 0.8656)的成核过程。在成核物理方面发现了两个原始结果。无论过饱和度如何,都发现了普遍的两步行为:核急剧富集到平衡,然后生长。胚胎沿着 MFEP 显示出弥散的界面。界面的宽度迅速饱和到临界核的宽度,然后保持不变。