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HF-DFT, the practice of evaluating approximate density functionals on Hartree-Fock densities, has long been used in testing density functional approximations. Density-corrected DFT (DC-DFT) is a general theoretical framework for identifying…

Chemical Physics · Physics 2021-10-18 Suhwan Song , Stefan Vuckovic , Eunji Sim , Kieron Burke

The crucial step in density-corrected Hartree-Fock density functional theory (DC(HF)-DFT) is to decide whether the density produced by the density functional for a specific calculation is erroneous and hence should be replaced by, in this…

Chemical Physics · Physics 2023-09-20 Daniel Graf , Alex J. W. Thom

Standard density functional approximations often give questionable results for odd-electron radical complexes, with the error typically attributed to self-interaction. In density corrected density functional theory (DC-DFT), certain classes…

Chemical Physics · Physics 2015-06-19 Min-Cheol Kim , Eunji Sim , Kieron Burke

DFT calculations have become widespread in both chemistry and materials, because they usually provide useful accuracy at much lower computational cost than wavefunction-based methods. All practical DFT calculations require an approximation…

Chemical Physics · Physics 2022-03-15 Eunji Sim , Suhwan Song , Stefan Vuckovic , Kieron Burke

Delocalization errors, such as charge-transfer and some self-interaction errors, plague computationally-efficient and otherwise-accurate density functional approximations (DFAs). Evaluating a semi-local DFA non-self-consistently on the…

Chemical Physics · Physics 2023-01-02 Aaron D. Kaplan , Chandra Shahi , Pradeep Bhetwal , Raj K. Sah , John P. Perdew

Empirical fitting of parameters in approximate density functionals is common. Such fits conflate errors in the self-consistent density with errors in the energy functional, but density-corrected DFT (DC-DFT) separates these two. We…

Chemical Physics · Physics 2020-12-02 Suhwan Song , Stefan Vuckovic , Eunji Sim , Kieron Burke

Density functional theory (DFT) is widely used to predict chemical properties, but its accuracy is limited by functional approximations and their approximate self-consistent densities. Density-corrected DFT (DC-DFT) is the study of the…

Chemical Physics · Physics 2023-07-21 Hayoung Yu , Suhwan Song , Seungsoo Nam , Kieron Burke , Eunji Sim

Density-corrected density functional theory (DC-DFT) is enjoying substantial success in improving semilocal DFT calculations in a wide variety of chemical problems. This paper provides the formal theoretical framework and assumptions for…

Chemical Physics · Physics 2019-08-19 Stefan Vuckovic , Suhwan Song , John Kozlowski , Eunji Sim , Kieron Burke

For the large and chemically diverse GMTKN55 benchmark suite, we have studied the performance of density-corrected density functional theory (HF-DFT), compared to self-consistent DFT, for several pure and hybrid GGA and meta-GGA…

Chemical Physics · Physics 2021-03-29 Golokesh Santra , Jan M. L. Martin

Density Functional Theory (DFT) sees prominent use in computational chemistry and physics, however, problems due to the self-interaction error (SIE) pose additional challenges to obtaining qualitatively correct results. An unphysical energy…

Chemical Physics · Physics 2023-02-08 Dale R. Lonsdale , Lars Goerigk

Standard flavors of density-functional theory (DFT) calculations are known to fail in describing anions, due to large self-interaction errors. The problem may be circumvented by using localized basis sets of reduced size, leaving no…

Chemical Physics · Physics 2019-12-23 Francesco Nattino , Céline Dupont , Nicola Marzari , Oliviero Andreussi

We present a self-interaction-corrected (SIC) density-functional-theory (DFT) approach for the description of systems with an unpaired electron or hole such as spin 1/2 defect-centers in solids or radicals. Our functional is…

Materials Science · Physics 2009-11-10 Mayeul d'Avezac , Matteo Calandra , Francesco Mauri

Density functional theory (DFT), one of the most widely utilized methods available to computational chemistry, fails to describe systems with statically correlated electrons. To address this shortcoming, in previous work we transformed DFT…

Chemical Physics · Physics 2023-01-02 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

We argue that any general mathematical measure of density error, no matter how reasonable, is too arbitrary to be of universal use. However the energy functional itself provides a universal relevant measure of density errors. For the…

Computational Physics · Physics 2018-11-13 Eunji Sim , Suhwan Song , Kieron Burke

We recently introduced an efficient methodology to perform density-corrected Hartree-Fock density functional theory (DC(HF)-DFT) calculations and an extension to it we called "corrected" HF DFT (C(HF)-DFT). In this work, we take a further…

Chemical Physics · Physics 2023-11-10 Daniel Graf , Alex J. W. Thom

Density functional theory (DFT) can run into serious difficulties with localized states in elements such as transition metals with occupied-d states and oxygen. In contrast, Hartree-Fock (HF) method can be a better approach for such…

Materials Science · Physics 2018-08-01 Hengxin Tan , Yuanchang Li , S. B. Zhang , Wenhui Duan

Unrestricted DFT methods are typically expected to describe the homolytic dissociation of nonpolar single bonds in neutral species with qualitative accuracy, due to the lack of significant delocalization error. We however find that many…

Chemical Physics · Physics 2019-03-15 Diptarka Hait , Adam Rettig , Martin Head-Gordon

The practical utility of M{\o}ller-Plesset (MP) perturbation theory is severely constrained by the use of Hartree-Fock (HF) orbitals. It has recently been shown that use of regularized orbital-optimized MP2 orbitals and scaling of MP3…

Chemical Physics · Physics 2021-01-06 Adam Rettig , Diptarka Hait , Luke W. Bertels , Martin Head-Gordon

Static correlation error(SCE) inevitably emerges when a dissociation of a covalent bond is described with a conventional denstiy-functional theory (DFT) for electrons. SCE gives rise to a serious overshoot in the potential energy at the…

Computational Physics · Physics 2020-08-10 Hideaki Takahashi

We review the role of self-consistency in density functional theory. 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…

Chemical Physics · Physics 2016-11-22 Adam Wasserman , Jonathan Nafziger , Kaili Jiang , Min-Cheol Kim , Eunji Sim , Kieron Burke
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