Wasserman Adam, Nafziger Jonathan, Jiang Kaili, Kim Min-Cheol, Sim Eunji, Burke Kieron
Department of Chemistry, Purdue University, West Lafayette, Indiana 47907; email:
Department of Physics and Astronomy, Purdue University, West Lafayette, Indiana 47907.
Annu Rev Phys Chem. 2017 May 5;68:555-581. doi: 10.1146/annurev-physchem-052516-044957. Epub 2017 Feb 6.
We review the role of self-consistency in density functional theory (DFT). We apply a recent analysis to both Kohn-Sham and orbital-free DFT, as well as to partition DFT, which generalizes all aspects of standard DFT. In each case, the analysis distinguishes between errors in approximate functionals versus errors in the self-consistent density. This yields insights into the origins of many errors in DFT calculations, especially those often attributed to self-interaction or delocalization error. In many classes of problems, errors can be substantially reduced by using better densities. We review the history of these approaches, discuss many of their applications, and give simple pedagogical examples.
我们回顾了自洽性在密度泛函理论（DFT）中的作用。我们将最近的一种分析方法应用于Kohn-Sham密度泛函理论、无轨道密度泛函理论以及分区密度泛函理论，后者概括了标准密度泛函理论的所有方面。在每种情况下，该分析都区分了近似泛函中的误差与自洽密度中的误差。这有助于深入了解密度泛函理论计算中许多误差的来源，尤其是那些通常归因于自相互作用或离域误差的误差。在许多类问题中，通过使用更好的密度可以大幅减少误差。我们回顾了这些方法的历史，讨论了它们的许多应用，并给出了简单的教学示例。
