How does it become possible to treat delocalized and/or open-shell systems in fragmentation-based linear-scaling electronic structure calculations? The case of the divide-and-conquer method.
How does it become possible to treat delocalized and/or open-shell systems in fragmentation-based linear-scaling electronic structure calculations? The case of the divide-and-conquer method.
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DOI：
10.1039/c2cp40153c
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发表时间：
2012-05
期刊：
影响因子：
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通讯作者：
Masato Kobayashi;H. Nakai
中科院分区：
文献类型：
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作者：
Masato Kobayashi;H. Nakai
作者开发了一种基于碎裂的线性标度电子结构计算策略，称为分治（DC）方法，该方法已被实现到Gamess程序包中。虽然有很多种基于碎裂的线性标度方案，但大多数方案都要求每个碎片的电荷和自旋多重性是先验的。因此，它们在离域和/或开壳层系统中的应用受到限制。然而，DC方法是一个值得注意的例外，因为电子在整个系统中的分布是由通用费米能级自动确定的。从这个角度出发，作者总结了基于DC方法的线性标度自洽场（SCF）和后SCF计算离域和/或开壳层系统的性能。最后对该方法的发展前景进行了展望。
The authors have developed a fragmentation-based linear-scaling electronic structure calculation strategy named the divide-and-conquer (DC) method, which has been implemented into the Gamess program package. Although there are many sorts of fragmentation-based linear-scaling schemes, most of them require the charge and spin multiplicity of each fragment a priori. Therefore, their applications to delocalized and/or open-shell systems have been limited. However, the DC method is a notable exception because the distribution of electrons in the entire system is automatically determined by the universal Fermi level. In this perspective, the authors have summarized the performance of the linear-scaling self-consistent field (SCF) and post-SCF calculations of delocalized and/or open-shell systems based on the DC method. Furthermore, some future prospects of the method have been discussed.