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The systematic underestimation of band gaps is one of the most fundamental challenges in semilocal density functional theory (DFT). In addition to hindering the application of DFT to predicting electronic properties, the band gap problem is…

Chemical Physics · Physics 2024-08-27 Kyle Bystrom , Stefano Falletta , Boris Kozinsky

In electronic structure methods based on the correction of approximate density-functional theory (DFT) for systematic inaccuracies, Hubbard $U$ parameters may be used to quantify and amend the self-interaction errors ascribed to selected…

Strongly Correlated Electrons · Physics 2017-04-27 Glenn Moynihan , Gilberto Teobaldi , David D. O'Regan

Semi-local DFT methods exhibit significant errors for the phase diagrams of transition-metal oxides that are caused by an incorrect description of molecular oxygen and the large self-interaction error in materials with strongly localized…

Materials Science · Physics 2022-03-29 Nongnuch Artrith , José Antonio Garrido Torres , Alexander Urban , Mark S. Hybertsen

We derive an exact representation of the exchange-correlation energy within density functional theory (DFT) which spawns a class of approximations leading to correct long-range asymptotic behavior. In what amounts to be the simplest…

Materials Science · Physics 2009-11-10 Roi Baer , Daniel Neuhauser

The band-gap problem and other systematic failures of approximate functionals are explained from an analysis of total energy for fractional charges. The deviation from the correct intrinsic linear behavior in finite systems leads to…

Materials Science · Physics 2009-11-13 Paula Mori-Sánchez , Aron J. Cohen , Weitao Yang

A critical challenge for density functional theory (DFT) in practice is its limited ability to treat static electron correlation, leading to errors in its prediction of charges, multiradicals, and reaction barriers. Recently, we combined…

Chemical Physics · Physics 2024-11-05 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

We propose a method that incorporates explicit derivative discontinuity of the total energy with respect to the number of electrons and treats both delocalization and static correlation effects in density functional calculations. Our…

Strongly Correlated Electrons · Physics 2018-03-08 Fei Zhou , Vidvuds Ozolins

A systematic comparative study has been performed to better understand DFT$+U$ (density functional theory + $U$) method. We examine the effect of choosing different double counting and exchange-correlation functionals. The calculated energy…

Strongly Correlated Electrons · Physics 2018-06-26 Siheon Ryee , Myung Joon Han

Hubbard-corrected density functional theory, denoted by DFT+U method, was developed to enable correct prediction of insulating properties for strongly-correlated electron systems. UO$_2$ is an example having O-$2p$, U-$6d$, and U-$5f$…

Strongly Correlated Electrons · Physics 2023-02-28 Mahmoud Payami

Density functional theory (DFT) is the most promising method for calculating quantum properties of molecules and materials at moderate and large scales. However, commonly used density functional approximations (DFAs) have systematic…

Chemical Physics · Physics 2026-03-24 Yichen Fan , Jacob Z. Williams , Weitao Yang

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

Density functional theory (DFT) is used in thousands of papers each year, yet lack of universality reduces DFT's predictive capacity, and functionals may produce energy-density imbalances. The absolute electronegativity (\chi) and hardness…

Chemical Physics · Physics 2020-07-15 Klaus A. Moltved , Kasper P. Kepp

Density-functional theory (DFT) has revolutionized computer simulations in chemistry and material science. A faithful implementation of the theory requires self-consistent calculations. However, this effort involves repeatedly diagonalizing…

Quantum Physics · Physics 2023-07-17 Taehee Ko , Xiantao Li , Chunhao Wang

Practical density functional theory (DFT) owes its success to the groundbreaking work of Kohn and Sham that introduced the exact calculation of the non-interacting kinetic energy of the electrons using an auxiliary mean-field system.…

Chemical Physics · Physics 2023-11-17 P. del Mazo-Sevillano , J. Hermann

Density functional theory (DFT) has been widely applied to a variety of realistic materials but often struggles to explain the properties of correlated systems. The DFT + U method, which introduces a Hubbard U correction to the DFT, has…

Strongly Correlated Electrons · Physics 2025-08-20 Ju Hyeon Lee , Bongjae Kim

We develop a generalization of the Kohn-Sham density functional theory (KS-DFT) + Hubbard $U$ (DFT+$U$) method to the excited-state regime. This has the form of Hubbard $U$ corrected linear-response time-dependent DFT, or `TDDFT+$U$'.…

Strongly Correlated Electrons · Physics 2019-04-24 Okan K. Orhan , David D. O'Regan

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

Many-body theories such as dynamical mean field theory (DMFT) have enabled the description of the electron exchange-correlation interactions that are missing in current density functional theory (DFT) calculations. However, there has been…

Strongly Correlated Electrons · Physics 2021-01-19 A. D. N. James , E. I. Harris-Lee , A. Hampel , M. Aichhorn , S. B. Dugdale

In their famous paper Kohn and Sham formulated a formally exact density-functional theory (DFT) for the ground-state energy and density of a system of $N$ interacting electrons, albeit limited at the time by certain troubling…

Mesoscale and Nanoscale Physics · Physics 2015-06-16 Miquel Huix-Rotllant , Mark E. Casida

The delocalization error of popular density functional approximations (DFAs) leads to diversified problems in present-day density functional theory calculations. For achieving a universal elimination of delocalization error, we develop a…

Chemical Physics · Physics 2017-09-07 Chen Li , Xiao Zheng , Neil Qiang Su , Weitao Yang