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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

Despite the great success Kohn-Sham density functional theory (KS-DFT) has achieved, the delocalization error remains a major challenge for commonly used density functional approximations (DFAs), resulting in systematic errors in ionization…

Chemical Physics · Physics 2026-02-12 Yichen Fan , Jincheng Yu , Jiayi Du , Weitao Yang

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

Density functional theory offers accurate structure prediction at acceptable computational cost, but commonly used approximations suffer from delocalization error; this results in inaccurate predictions of quantities such as energy band…

Materials Science · Physics 2022-08-17 Aaron Mahler , Jacob Z. Williams , Neil Qiang Su , Weitao Yang

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

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

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

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

The stochastic density functional theory (DFT) [Phys. Rev. Lett. 111, 106402 (2013)] is a valuable linear scaling approach to Kohn-Sham DFT that does not rely on the sparsity of the density matrix. Linear (and often sub-linear) scaling is…

Chemical Physics · Physics 2019-02-20 Ming Chen , Roi Baer , Daniel Neuhauser , Eran Rabani

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

Approximate semi-local density functional theory (DFT) is known to underestimate surface formation energies yet paradoxically overbind adsorbates on catalytic transition-metal oxide surfaces due to delocalization error. The low-cost DFT+U…

Materials Science · Physics 2021-11-24 Akash Bajaj , Heather J. Kulik

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

The recently developed localized orbital scaling correction (LOSC) method shows the ability to systematically and size-consistently reduce the delocalization error existing in conventional density functional approximations (DFAs). Applying…

Chemical Physics · Physics 2020-10-19 Yuncai Mei , Zehua Chen , Weitao Yang

A detailed account of the implementation of equations of the Relativistic Density Functional Theory (RDFT) using basis sets of APW/LAPW type with flexible extensions provided by local orbitals is given. Earlier discoveries of the importance…

Materials Science · Physics 2021-04-07 Andrey L. Kutepov

Density functional theory within the local or semilocal density approximations (DFT-LDA/GGA) has become a workhorse in electronic structure theory of solids, being extremely fast and reliable for energetics and structural properties, yet…

Density Functional Theory (DFT) is a pivotal method within quantum chemistry and materials science, with its core involving the construction and solution of the Kohn-Sham Hamiltonian. Despite its importance, the application of DFT is…

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

Machine-learned interatomic potentials (MLIPs) based on message passing neural networks hold promise to enable large-scale atomistic simulations of complex materials with ab initio accuracy. A number of MLIPs trained on energies and forces…

Materials Science · Physics 2025-04-09 Mikkel Ohm Sauer , Peder Meisner Lyngby , Kristian Sommer Thygesen

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

One of the most important open challenges in modern Kohn-Sham (KS) density-functional theory (DFT) is the correct treatment of fractional electron charges and spins. Approximate exchange-correlation (XC) functionals struggle to do this in a…

Chemical Physics · Physics 2015-12-24 Jonathan Nafziger , Adam Wasserman
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