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Two electrons at the threshold of ionization represent a severe test case for electronic structure theory. A pseudospectral method yields a very accurate density of the two-electron ion with nuclear charge close to the critical value.…

Chemical Physics · Physics 2014-08-12 Paul E. Grabowski , Kieron Burke

The exact formulation of multi-configuration density-functional theory (DFT) is discussed in this work. As an alternative to range-separated methods, where electron correlation effects are split in the coordinate space, the combination of…

Chemical Physics · Physics 2015-02-26 Emmanuel Fromager

Density-potential functional theory (DPFT) is an alternative formulation of orbital-free density functional theory that may be suitable for modeling the electronic structure of large systems. To date, DPFT has been applied mainly to quantum…

Materials Science · Physics 2023-04-21 Martin-Isbjörn Trappe , William C. Witt , Sergei Manzhos

The recently developed hypercomplex Kohn-Sham (HCKS) theory shows great potential to overcome the static/strong correlation issue in density functional theory (DFT), which highlights the necessity of further exploration of the HCKS theory…

Chemical Physics · Physics 2022-03-16 Neil Qiang Su

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

The advent of the Hohenberg-Kohn theorem in 1964, its extension to finite-T, Kohn-Sham theory, and relativistic extensions provide the well-established formalism of density-functional theory (DFT). This theory enables the calculation of all…

Quantum Physics · Physics 2013-07-18 M. W. C. Dharma-wardana

A recently developed approach, conditional probability density functional theory (CP-DFT), yields direct access to the exchange-correlation hole of a system, an important correlation function that is not available from any standard DFT…

Materials Science · Physics 2026-05-14 Peiwei You , Ryan Pederson , Kieron Burke , E. K. U. Gross

We introduce a practical hybrid approach that combines orbital-free density functional theory (DFT) with Kohn-Sham DFT for speeding up first-principles molecular dynamics simulations. Equilibrated ionic configurations are generated using…

We establish a rigorous density functional theory (DFT) framework for core-level X-ray absorption spectroscopy (XAS) by formulating a constrained search for core-excited states based on the Gunnarsson-Lundqvist theorem. Within this…

Materials Science · Physics 2025-11-25 Seokkyu An , Taisuke Ozaki

The widespread use of (generalized) Kohn-Sham density functional theory (KS-DFT) lies in the fact that hierarchical sets of approximations of the exchange-correlation (XC) energy functional can be designed, offering versatile choices to…

Materials Science · Physics 2023-01-31 Igor Ying Zhang , Xinguo Ren

We present a perturbative approach within the scope of Kohn-Sham density functional theory (DFT). The method is based on the exact exchange-only optimized effective potential method, and correlation is included via perturbation expansion…

Chemical Physics · Physics 2007-05-23 P. Sule

It was recently shown [Phys. Rev. Lett. 105, 123002 (2010)] that the complete wavefunction for a system of electrons and nuclei evolving in a time-dependent external potential can be exactly factorized into an electronic wavefunction and a…

Chemical Physics · Physics 2015-06-11 Ali Abedi , Neepa T. Maitra , E. K. U. Gross

Transition-metal compounds (TMCs) with open-shell d-electrons are characterized by a complex interplay of lattice, charge, orbital, and spin degrees of freedom, giving rise to a diverse range of fascinating applications. Often exhibiting…

Materials Science · Physics 2025-03-19 Yubo Zhang , Akilan Ramasamy , Kanun Pokharel , James W. Furness , Jinliang Ning , Ruiqi Zhang , Jianwei Sun

Density functional theory (DFT) provides a theoretical framework for efficient and fairly accurate calculations of the electronic structure of molecules and crystals. The main features of density functional theory are described and DFT…

Chemical Physics · Physics 2012-06-12 Hauke Paulsen , Alfred Xaver Trautwein

The ground state electron density -- obtainable using Kohn-Sham Density Functional Theory (KS-DFT) simulations -- contains a wealth of material information, making its prediction via machine learning (ML) models attractive. However, the…

We formulate a time-dependent density functional theory for the coupled dynamics of electrons and nuclei that goes beyond the Born-Oppenheimer (BO) approximation. We prove that the time-dependent marginal nuclear probability density…

Chemical Physics · Physics 2025-11-14 Chen Li , Ryan Requist , E. K. U. Gross

Absolute binding energies of core electrons in molecules and bulk materials can be efficiently calculated by spin paired density-function theory employing a $\Delta$ Kohn-Sham ($\Delta$KS) scheme corrected by offsets that are highly…

Materials Science · Physics 2016-08-03 Michael Walter , Michael Moseler , Lars Pastewka

Last year, at least 30,000 scientific papers used the Kohn-Sham scheme of density functional theory to solve electronic structure problems in a wide variety of scientific fields, ranging from materials science to biochemistry to…

Computational Physics · Physics 2018-02-07 Felix Brockherde , Leslie Vogt , Li Li , Mark E. Tuckerman , Kieron Burke , Klaus-Robert Müller

Ground-state Kohn-Sham density functional theory provides, in principle, the exact ground-state energy and electronic spin-densities of real interacting electrons in a static external potential. In practice, the exact density functional for…

Chemical Physics · Physics 2022-07-11 Aaron D. Kaplan , Mel Levy , John P. Perdew

Approximate molecular calculations via standard Kohn-Sham Density Functional Theory are exactly reproduced by performing self-consistent calculations on isolated fragments via Partition Density Functional Theory [Phys. Rev. A 82, 024501…

Other Condensed Matter · Physics 2016-11-25 Jonathan Nafziger , Qin Wu , Adam Wasserman
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