An Additive Long-range Potential to Correct for the Charge-transfer Failure of Time-dependent Density Functional Theory

被引：11

作者：

Dreuw, Andreas ^{[1
]}

Ploetner, Juergen ^{[1
]}

Wormit, Michael ^{[1
]}

Head-Gordon, Martin ^{[2
,3
]}

Dutoi, Anthony Dean ^{[4
]}

机构：

[1] Goethe Univ Frankfurt, Inst Phys & Theoret Chem, D-60438 Frankfurt, Germany

[2] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA

[3] Univ Calif Berkeley, Lawrence Berkeley Lab, Chem Sci & Phys Biosci Div, Berkeley, CA 94720 USA

[4] Heidelberg Univ, Inst Phys & Theoret Chem, D-69120 Heidelberg, Germany

来源：

ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-INTERNATIONAL JOURNAL OF RESEARCH IN PHYSICAL CHEMISTRY & CHEMICAL PHYSICS | 2010年 / 224卷 / 3-4期

关键词：

Excited States; Time Dependent Density Functional Theory; Charge Transfer; Long-range Corrected Potential; Hartree-Fock Exchange; TRANSFER EXCITED-STATES; CORRELATION ENERGIES; EXCITATION-ENERGIES; APPROXIMATION;

D O I：

10.1524/zpch.2010.6107

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Time-dependent density functional theory is one of the most widely used methods for the calculation of excited states of large molecules. However, it exhibits substantial problems with charge-transfer excited states when conventional exchange-correlation functionals are employed. Here, we introduce an additive long-range potential that can, in principle, be directly employed with any existing local, GGA or hybrid-functional, without re-fitting of the original functionals. The additive potential shifts the excitation energies to higher values and corrects for the wrong asymptotic behavior of their potential energy surfaces with respect to charge-separating coordinates. First examples of its successful application are shown.

引用

页码：311 / 324

页数：14

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