Role of the Prestructured Surface Cloud in Crystal Nucleation
Role of the Prestructured Surface Cloud in Crystal Nucleation
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DOI：
10.1103/physrevlett.106.085701
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发表时间：
2011-02-22
影响因子：
8.6
通讯作者：
Bolhuis, Peter G.
中科院分区：
文献类型：
--
作者：
Lechner, Wolfgang;Dellago, Christoph;Bolhuis, Peter G.
对于软核胶体模型中的均质结晶成核过程，我们采用过渡路径采样技术结合committor函数的似然最大化，从一组基于核内局部结构的新阶参数中确定最佳反应坐标。我们发现成核是由固体团簇控制的，这些团簇由嵌入在表面粒子云中的hcp核组成，这些粒子云与它们最近的邻居高度相关，但不是在高对称的晶体结构中有序。结果对经典成核理论中表面项和体积项的解释有了新的启示。
For the homogeneous crystal nucleation process in a soft-core colloid model, we identify optimal reaction coordinates from a set of novel order parameters based on the local structure within the nucleus, by employing transition path sampling techniques combined with a likelihood maximization of the committor function. We find that nucleation is governed by solid clusters that consist of an hcp core embedded within a cloud of surface particles that are highly correlated with their nearest neighbors but not ordered in a high-symmetry crystal structure. The results shed new light on the interpretation of the surface and volume terms in classical nucleation theory.