Grand and Semigrand Canonical Basin-Hopping.
Grand and Semigrand Canonical Basin-Hopping.
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DOI：
10.1021/acs.jctc.5b00962
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发表时间：
2016-02-09
影响因子：
5.5
通讯作者：
Wales DJ
中科院分区：
文献类型：
--
作者：
Calvo F;Schebarchov D;Wales DJ
我们引入了基于每个势能最小值对（半）大势的局部贡献的流域跳跃的广义和半广义正则全局优化方法。用原子团簇状态的局部谐波振动密度作为温度和化学势的函数对该方法进行了测试。预测的全球最小值从解离态切换到具有较大化学势值和较低温度的团簇，这与拟合选定团簇热容数据的模型的预测一致。半正则优化允许我们识别多组分纳米合金中特别稳定的成分，作为温度升高的函数，而大正则势可以作为全局优化搜索的副产品，对有利结构进行有用的调查。
We introduce grand and semigrand canonical global optimization approaches using basin-hopping with an acceptance criterion based on the local contribution of each potential energy minimum to the (semi)grand potential. The method is tested using local harmonic vibrational densities of states for atomic clusters as a function of temperature and chemical potential. The predicted global minima switch from dissociated states to clusters for larger values of the chemical potential and lower temperatures, in agreement with the predictions of a model fitted to heat capacity data for selected clusters. Semigrand canonical optimization allows us to identify particularly stable compositions in multicomponent nanoalloys as a function of increasing temperature, whereas the grand canonical potential can produce a useful survey of favorable structures as a byproduct of the global optimization search.