Ab initio crystal structure prediction -: I.: Rigid molecules
Ab initio crystal structure prediction -: I.: Rigid molecules
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DOI：
10.1002/jcc.20165
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发表时间：
2005-02-01
影响因子：
3
通讯作者：
Pantelides, CC
中科院分区：
文献类型：
--
作者：
Karamertzanis, PG;Pantelides, CC
提出了一种仅利用分子的原子连接性来预测分子晶体结构的新方法。该方法是基于晶体的晶格焓的全局最小化。静电相互作用的建模是通过一组分布式电荷来完成的，这些电荷是基于量子力学计算的结果来优化和自动选择和定位的。一个四步全局优化算法用于识别的晶格焓表面的局部极小值。该算法的并行实现允许更广泛的搜索的解决方案空间比迄今为止是可能的，允许识别的晶体结构，在不太频繁出现的空间群和一个以上的分子在不对称单元。该算法已成功地应用于3-氮杂双环（3.3.1）壬烷-2，4-二酮（P2（1）/a，Z' = 1）、别嘌呤醇（P2（1）/c，Z'= 1）、1，3，4，6，7，9-六氮杂环（3.3.3）吖嗪（Pbca，Z' = 2）和三亚乙基二胺（P6（3）/m，Z' = 1）的晶体结构预测。在所有情况下，实验已知的结构是最稳定的预测结构，但不一定是全局最小值。(C)2004 Wiley Periodicals，Inc.
A new methodology for the prediction of molecular crystal structures using only the atomic connectivity of the molecule under consideration is presented. The approach is based on the global minimization of the lattice enthalpy of the crystal. The modeling of the electrostatic interactions is accomplished through a set of distributed charges that are optimally and automatically selected and positioned based on results of quantum mechanical calculations. A four-step global optimization algorithm is used for the identification of the local minima of the lattice enthalpy surface. A parallelized implementation of the algorithm permits a much more extensive search of the solution space than has hitherto been possible, allowing the identification of crystal structures in less frequently occurring space groups and with more than one molecule in the asymmetric unit. The algorithm has been applied successfully to the prediction of the crystal structures of 3-aza-bicyclo(3.3.1)nonane-2,4-dione (P2(1)/a, Z' = 1), allopurinol (P2(1)/c Z' = 1), 1,3,4,6,7,9-hexa-azacycl(3.3.3)azine (Pbca, Z' = 2), and triethylenediamine (P6(3)/m, Z' = 1). In all cases, the experimentally known structure is among the most stable predicted structures, but not necessarily the global minimum. (C) 2004 Wiley Periodicals, Inc.