A divide and conquer real-space approach for all-electron molecular electrostatic potentials and interaction energies
A divide and conquer real-space approach for all-electron molecular electrostatic potentials and interaction energies
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DOI：
10.1063/1.4721386
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发表时间：
2012-06-07
影响因子：
4.4
通讯作者：
Sundholm, D.
中科院分区：
文献类型：
--
作者：
Losilla, S. A.;Sundholm, D.
本文提出并实现了一种精确计算分子体系静电势和相互作用能的计算方法。分子的电子和能量密度被分成重叠的原子中心的原子贡献和三维分子余数。陡峭的核尖点被包括在原子中心函数中，使得三维剩余部分足够光滑，可以用易处理的网格点数量准确地表示。一维径向函数的原子中心的贡献，以及三维剩余的扩展使用有限元函数。静电势的计算是通过积分库仑势为每个单独的密度贡献，使用我们的张量有限元法的三维剩余部分。我们还提供了算法来计算精确的电子-电子和电子-核相互作用的数值使用建议的分区。该方法已被测试的18个合理的大分子的全电子密度包含元素Zn。当采用步长为0.05a（0）的等距网格时，库仑相互作用能的计算精度在10（-3）~ 10（-6）E-h之间。(C)2012年美国物理学会。[http：//dx.doi.org/10.1063/1.4721386]
A computational scheme to perform accurate numerical calculations of electrostatic potentials and interaction energies for molecular systems has been developed and implemented. Molecular electron and energy densities are divided into overlapping atom-centered atomic contributions and a three-dimensional molecular remainder. The steep nuclear cusps are included in the atom-centered functions making the three-dimensional remainder smooth enough to be accurately represented with a tractable amount of grid points. The one-dimensional radial functions of the atom-centered contributions as well as the three-dimensional remainder are expanded using finite element functions. The electrostatic potential is calculated by integrating the Coulomb potential for each separate density contribution, using our tensorial finite element method for the three-dimensional remainder. We also provide algorithms to compute accurate electron-electron and electron-nuclear interactions numerically using the proposed partitioning. The methods have been tested on all-electron densities of 18 reasonable large molecules containing elements up to Zn. The accuracy of the calculated Coulomb interaction energies is in the range of 10(-3) to 10(-6) E-h when using an equidistant grid with a step length of 0.05 a(0). (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4721386]