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Kohn-Sham inversion, that is, the finding of the exact Kohn-Sham potential for a given density, is difficult in localized basis sets. We study the precision and reliability of several inversion schemes, finding estimates of density-driven…

Chemical Physics · Physics 2020-04-27 Seungsoo Nam , Suhwan Song , Eunji Sim , Kieron Burke

Adsorbed transition metal atoms can have partially filled $d$- or $f$-shells due to strong on-site Coulomb interaction. Capturing all effects originating from electron correlation in such strongly correlated systems is a challenge for…

Strongly Correlated Electrons · Physics 2018-01-17 Marc Philipp Bahlke , Michael Karolak , Carmen Herrmann

Density functional theory stems from the Hohenberg-Kohn-Sham-Mermin (HKSM) theorem in the grand canonical ensemble (GCE). However, as recent work shows, although its extension to the canonical ensemble (CE) is not straightforward, work in…

Statistical Mechanics · Physics 2009-11-07 J. A. Hernando

We present a first-principles approach to describe magnetic and superconducting systems and the phenomena of competition between these electronic effects. We develop a density functional theory: SpinSCDFT, by extending the Hohenberg-Kohn…

Superconductivity · Physics 2016-05-10 A. Linscheid , A. Sanna , F. Essenberger , E. K. U. Gross

For electronic systems with multi-reference (MR) character, Kohn-Sham density functional theory (KS-DFT) with the conventional exchange-correlation (xc) energy functionals can lead to incorrect spin densities and related properties. For…

Chemical Physics · Physics 2024-06-14 Yu-Yang Wang , Jeng-Da Chai

Kohn-Sham density functional theory is one of the most widely used electronic structure theories. In the pseudopotential framework, uniform discretization of the Kohn-Sham Hamiltonian generally results in a large number of basis functions…

Numerical Analysis · Mathematics 2015-05-27 Lin Lin , Jianfeng Lu , Lexing Ying , E. Weinan

Kohn-Sham density functional theory (KS-DFT) has found widespread application in accurate electronic structure calculations. However, it can be computationally demanding especially for large-scale simulations, motivating recent efforts…

Computational Physics · Physics 2024-06-25 Feitong Song , Ji Feng

The design of better exchange-correlation functionals for Density Functional Theory (DFT) is a central challenge of modern electronic structure theory. However, current developments are limited by the mathematical form of the functional,…

Chemical Physics · Physics 2024-08-19 Kyle Bystrom , Boris Kozinsky

We showcase the advantages of orbital-free density-potential functional theory (DPFT), a more flexible variant of Hohenberg-Kohn density functional theory. DPFT resolves the usual trouble with the gradient-expanded kinetic energy functional…

Quantum Gases · Physics 2021-06-16 Martin-Isbjörn Trappe , Jun Hao Hue , Berthold-Georg Englert

The reconstruction of the exchange-correlation potential from accurate ab initio electron densities can provide insights into the limitations of the currently available approximate functionals and provide guidance for devising improved…

Strongly Correlated Electrons · Physics 2013-02-05 Katharina Boguslawski , Christoph R. Jacob , Markus Reiher

Electrons in zero external magnetic field can be studied with density functional theory (DFT) or with spin-DFT (SDFT). The latter is normally used for open shell systems because its approximations appear to model better the exchange and…

Chemical Physics · Physics 2022-04-06 Timothy Callow , Benjamin Pearce , Nikitas Gidopoulos

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

Density functional theory is a successful branch of numerical simulations of quantum systems. While the foundations are rigorously defined, the universal functional must be approximated resulting in a `semi'-ab initio approach. The search…

Quantum Physics · Physics 2017-11-22 James Daniel Whitfield , Norbert Schuch , Frank Verstraete

According to the Hohenberg-Kohn theorem of density-functional theory (DFT), all observable quantities of systems of interacting electrons can be expressed as functionals of the ground-state density. This includes, in principle, the spin…

Strongly Correlated Electrons · Physics 2019-09-04 Carsten A. Ullrich

We outline a Kohn-Sham-Dirac density-functional-theory (DFT) scheme for graphene sheets that treats slowly-varying inhomogeneous external potentials and electron-electron interactions on an equal footing. The theory is able to account for…

Strongly Correlated Electrons · Physics 2008-09-23 Marco Polini , Andrea Tomadin , Reza Asgari , A. H. MacDonald

A previously proposed non-canonical coupled-perturbed Kohn-Sham density functional theory (KS-DFT)/Hartree-Fock (HF) treatment for spin-orbit coupling is here generalized to infinite periodic systems. The scalar-relativistic periodic…

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

Different steps leading to the new functional for pairing based on natural orbitals and occupancies proposed in ref. [D. Lacroix and G. Hupin, arXiv:1003.2860] are carefully analyzed. Properties of quasi-particle states projected onto good…

Nuclear Theory · Physics 2011-03-22 Guillaume Hupin , Denis Lacroix

We present a computationally efficient approach to perform large-scale all-electron density functional theory calculations by enriching the classical finite element basis with compactly supported atom-centered numerical basis functions that…

Computational Physics · Physics 2017-01-11 Bikash Kanungo , Vikram Gavini

Hybrid density functional theory (DFT) remains intractable for large periodic systems due to the demanding computational cost of exact exchange. We apply the tensor hypercontraction (THC) (or interpolative separable density fitting)…

Computational Physics · Physics 2023-10-13 Adam Rettig , Joonho Lee , Martin Head-Gordon