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While density functional theory (DFT) is widely applied for its combination of cost and accuracy, corrections (e.g., DFT+U) that improve it are often needed to tackle correlated transition-metal chemistry. In principle, the functional form…

Chemical Physics · Physics 2021-03-12 Akash Bajaj , Heather J. Kulik

Approximate density functional theory (DFT) suffers from many-electron self- interaction error, otherwise known as delocalization error, that may be diagnosed and then corrected through elimination of the deviation from exact piecewise…

Materials Science · Physics 2016-11-08 Terry Z. H. Gani , Heather J. Kulik

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

Low-cost, non-empirical corrections to semi-local density functional theory are essential for accurately modeling transition metal chemistry. Here, we demonstrate the judiciously-modified density functional theory (jmDFT) approach with…

Materials Science · Physics 2022-05-25 Akash Bajaj , Chenru Duan , Aditya Nandy , Michael G. Taylor , Heather J. Kulik

We apply Density Functional Theory (DFT) and the DFT+U technique to study the adsorption of transition metal porphine molecules on atomistically flat Au(111) surfaces. DFT calculations using the Perdew-Burke-Ernzerhof (PBE) exchange…

Despite its widespread use, the predictive accuracy of density functional theory (DFT) is hampered by delocalization errors, especially for correlated systems such as transition-metal complexes. Two complementary tuning strategies have been…

Materials Science · Physics 2022-04-11 Yael Cytter , Aditya Nandy , Akash Bajaj , Heather J. Kulik

Accurate computational predictions of band gaps are of practical importance to the modeling and development of semiconductor technologies, such as (opto)electronic devices and photoelectrochemical cells. Among available electronic-structure…

Materials Science · Physics 2021-03-16 Nicole E. Kirchner-Hall , Wayne Zhao , Yihuang Xiong , Iurii Timrov , Ismaila Dabo

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

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

A density functional theory (DFT) approach to computing transition metal oxide heat of formation without adjustable parameters is presented. Different degrees of $d$-electron localization in oxides are treated within the DFT+$U$ approach…

Materials Science · Physics 2022-04-01 Johannes Voss

It is believed that the density functional theory (DFT) describes most elements with s, p and d orbitals very well, except some materials that having strongly localized and correlated valence electrons. In this work, we find that the widely…

Materials Science · Physics 2020-03-17 Y. X. Wang , Hua Y. Geng , Q. Wu , Xiang R. Chen

Density functional theory (DFT) underpins modern atomistic simulations of transition-metal surfaces. It can predict key properties linked to catalytic performance, such as adsorption energies and barrier heights, enabling new paradigms in…

Materials Science · Physics 2026-03-23 Benjamin X. Shi , Timothy C. Berkelbach

DFT+X methods, such as DFT+U and DFT+DMFT, are important supplements to standard density functional theory when strong on-site Coulomb interactions are present. However, the involvement of external parameters in the underlying model…

Strongly Correlated Electrons · Physics 2026-03-03 X. L. Pan , H. X. Song , Y. Sun , F. C. Wu , H. Wang , Y. F. Wang , Y. Chen , X. R. Chen , Hua Y. Geng

Accurate predictions of the properties of transition metal oxides using density functional theory (DFT) calculations are essential for the computational design of energy materials. In this work, we investigate the anomalous reversal of the…

We present an orbital-resolved extension of the Hubbard $U$ correction to density-functional theory (DFT). Compared to the conventional shell-averaged approach, the prediction of energetic, electronic and structural properties is strongly…

Materials Science · Physics 2024-09-18 Eric Macke , Iurii Timrov , Nicola Marzari , Lucio Colombi Ciacchi

Accurately modeling compounds with partially filled $d$ and $f$ shells remains a hard challenge for density-functional theory, due to large self-interaction errors stemming from local or semi-local exchange-correlation functionals. Hubbard…

Materials Science · Physics 2026-01-19 Kinga Warda , Eric Macke , Iurii Timrov , Lucio Colombi Ciacchi , Piotr M. Kowalski

Approximate functionals used in practical density functional theory (DFT) deviate from the piecewise linear behavior of the exact functional for fractional charges. This deviation causes excess charge delocalization, which leads to…

Chemical Physics · Physics 2018-10-23 Diptarka Hait , Martin Head-Gordon

Density functional theory augmented with a Hubbard correction (DFT+U) is widely used to treat localized electronic states, but its predictions are often sensitive to the choice of the local projection space defining the correlated subspace.…

Strongly Correlated Electrons · Physics 2026-04-13 Manjula Raman , Kenneth Park

Delocalization error prevents density functional theory (DFT) from reaching its full potential, causing problems like systematically underestimated band gaps and misaligned energy levels at interfaces. We introduce lrLOSC to correct…

Materials Science · Physics 2026-04-29 Jacob Z. Williams , Weitao Yang

Stochastic and mixed stochastic-deterministic density functional theory (DFT) are promising new approaches for the calculation of the equation-of-state and transport properties in materials under extreme conditions. In the intermediate warm…

Computational Physics · Physics 2023-09-27 Vidushi Sharma , Lee A. Collins , Alexander J. White
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