Beyond the isotropic atom model in crystal structure prediction of rigid molecules: Atomic multipoles versus point charges
Beyond the isotropic atom model in crystal structure prediction of rigid molecules: Atomic multipoles versus point charges
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DOI：
10.1021/cg049651n
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发表时间：
2005-05-01
影响因子：
3.8
通讯作者：
Jones, W
中科院分区：
文献类型：
--
作者：
Day, GM;Motherwell, WDS;Jones, W
用以原子为中心的多极模型势计算了50个具有约束(刚性)几何构型的有机小分子的预测和已知晶体结构的晶格能。与以往使用原子点电荷静电学预测相比，晶格能量最小化预测晶体结构的可靠性有了重要的改进。实验观察到的晶体结构中有一半要么是全球最小能量结构，要么是计算的晶格能在全球最小能量的0.5kJ/mol(0.1kcal/mol)范围内。此外，在69%的情况下，有五个或更少的未观测结构的晶格能被计算为低于观测结构的晶格能。这一结果为晶体结构的从头计算提供了一种全局晶格能量最小化的方法，并证实了用原子为中心的多极子来表示静电对能量的贡献是有用的。
The lattice energies of predicted and known crystal structures for 50 small organic molecules with constrained (rigid) geometries have been calculated with a model potential whose electrostatic component is described by atom-centered multipoles. In comparison to previous predictions using atomic point charge electrostatics, there are important improvements in the reliability of lattice energy minimization for the prediction of crystal structures. Half of the experimentally observed crystal structures are found either to be the global minimum energy structure or to have calculated lattice energies within 0.5 kJ/mol (0.1 kcal/mol) of the global minimum. Furthermore, in 69% of cases, there are five or fewer unobserved structures with lattice energies calculated to be lower than that of the observed structure. The results are promising for the advancement of global lattice energy minimization for the ab initio prediction of crystal structures and confirm the utility of representing electrostatic contributions to the energy with atom-centered multipoles.