Structural optimization of molecular clusters with density functional theory combined with basin hopping
Structural optimization of molecular clusters with density functional theory combined with basin hopping
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DOI：
10.1063/1.4755994
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发表时间：
2012-10-07
影响因子：
4.4
通讯作者：
Besley, Nicholas A.
中科院分区：
文献类型：
--
作者：
Do, Hainam;Besley, Nicholas A.
识别分子簇的能量最小值是一个具有挑战性的问题。传统上，模拟退火、遗传算法或盆地跳跃等搜索算法通常与经验力场结合使用。我们实施了与密度泛函理论相结合的盆地跳跃搜索算法，无需经验力场即可优化分子簇。这种方法可以应用于经验势不可用或可能不够准确的系统。我们通过在 B3LYP+D/6-31+G* 理论水平上对水、甲醇、水+甲醇簇以及质子化水和甲醇簇的研究来说明该方法的有效性。预测 H+(H2O)(7) 的新最低能量结构位于 B3LYP+D/6-31+G* 能级。在所有质子化的水和甲醇混合簇中，我们发现在最低能量结构中，H+更喜欢与甲醇而不是水结合。 (C) 2012 年美国物理研究所。 [http://dx.doi.org/10.1063/1.4755994]
Identifying the energy minima of molecular clusters is a challenging problem. Traditionally, search algorithms such as simulated annealing, genetic algorithms, or basin hopping are usually used in conjunction with empirical force fields. We have implemented a basin hopping search algorithm combined with density functional theory to enable the optimization of molecular clusters without the need for empirical force fields. This approach can be applied to systems where empirical potentials are not available or may not be sufficiently accurate. We illustrate the effectiveness of the method with studies on water, methanol, and water + methanol clusters as well as protonated water and methanol clusters at the B3LYP+D/6-31+G* level of theory. A new lowest energy structure for H+(H2O)(7) is predicted at the B3LYP+D/6-31+G* level. In all of the protonated mixed water and methanol clusters, we find that H+ prefers to combine with methanol rather than water in the lowest-energy structures. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4755994]