Self-Interaction Error in Density Functional Theory: An Appraisal,The Journal of Physical Chemistry Letters

当前位置： X-MOL 学术 › J. Phys. Chem. Lett. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Self-Interaction Error in Density Functional Theory: An Appraisal
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2018-04-06 00:00:00 , DOI: 10.1021/acs.jpclett.8b00242
Junwei Lucas Bao ₁ , Laura Gagliardi ₁ , Donald G. Truhlar ₁

Affiliation

Self-interaction error (SIE) is considered to be one of the major sources of error in most approximate exchange-correlation functionals for Kohn–Sham density-functional theory (KS-DFT), and it is large with all local exchange-correlation functionals and with some hybrid functionals. In this work, we consider systems conventionally considered to be dominated by SIE. For these systems, we demonstrate that by using multiconfiguration pair-density functional theory (MC-PDFT), the error of a translated local density-functional approximation is significantly reduced (by a factor of 3) when using an MCSCF density and on-top density, as compared to using KS-DFT with the parent functional; the error in MC-PDFT with local on-top functionals is even lower than the error in some popular KS-DFT hybrid functionals. Density-functional theory, either in MC-PDFT form with local on-top functionals or in KS-DFT form with some functionals having 50% or more nonlocal exchange, has smaller errors for SIE-prone systems than does CASSCF, which has no SIE.

中文翻译：

密度泛函理论中的自相互作用误差：一个评估

对于Kohn-Sham密度泛函理论（KS-DFT），自交互误差（SIE）被认为是大多数近似交换相关函数中的主要误差源之一，并且对于所有局部交换相关函数而言，自交互误差都很大。以及一些混合功能。在这项工作中，我们认为系统通常被视为由SIE主导。对于这些系统，我们证明了通过使用多配置对密度泛函理论（MC-PDFT），当使用MCSCF密度并置放于顶部时，翻译后的局部密度泛函近似值的误差显着降低了（减少了3倍）。与使用带有父功能的KS-DFT相比，密度更高；具有局部置顶功能的MC-PDFT中的错误甚至比某些流行的KS-DFT混合功能中的错误还要低。密度泛函理论，

更新日期：2018-04-06

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南