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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

Fromager and Lasorne [Electron. Struct. 6 025002 (2024)] have recently derived an in-principle exact Kohn-Sham density functional theory (KS-DFT) of electrons and nuclei, where the nuclear density and the (so-called conditional) electronic…

Chemical Physics · Physics 2026-03-10 Lucien Dupuy , Benjamin Lasorne , Emmanuel Fromager

When a molecule dissociates, the exact Kohn-Sham (KS) and Pauli potentials may form step structures. Reproducing these steps correctly is central for the description of dissociation and charge-transfer processes in density functional theory…

Chemical Physics · Physics 2021-03-23 Jakub Kocák , Eli Kraisler , Axel Schild

We re-adapt a spectral renormalization method, introduced in nonlinear optics, to solve the Kohn-Sham (KS) equations of density functional theory (DFT), with a focus on functionals based on the strictly-correlated electrons (SCE) regime,…

Strongly Correlated Electrons · Physics 2020-04-23 Juri Grossi , Ziad H. Musslimani , Michael Seidl , Paola Gori-Giorgi

When running time-dependent density functional theory (TDDFT) calculations for real-time simulations of non-equilibrium dynamics, the user has a choice of initial Kohn-Sham state, and typically a Slater determinant is used. We explore the…

Chemical Physics · Physics 2016-08-24 Johanna I. Fuks , Soeren E. B. Nielsen , Michael Ruggenthaler , Neepa T. Maitra

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

We obtain the exact Kohn-Sham potentials $V_{\mathrm{KS}}$ of time-dependent density-functional theory for 1D Hubbard chains, driven by a d.c.\ external field, using the time-dependent electron density and current density obtained from…

Mesoscale and Nanoscale Physics · Physics 2021-01-15 L. Mancini , J. D. Ramsden , M. J. P. Hodgson , R. W. Godby

Modeling many-body quantum systems with strong interactions is one of the core challenges of modern physics. A range of methods has been developed to approach this task, each with its own idiosyncrasies, approximations, and realm of…

Statistical Mechanics · Physics 2018-11-21 Brett Larder , Dirk Gericke , Scott Richardson , Paul Mabey , Thomas White , Gianluca Gregori

Kohn-Sham density functional theory is the base of modern computational approaches to electronic structures. Their accuracy vitally relies on the exchange-correlation energy functional, which encapsulates electron-electron interaction…

Computational Physics · Physics 2019-11-04 Ryo Nagai , Ryosuke Akashi , Osamu Sugino

The random phase approximation (RPA) for the electron correlation energy, combined with the exact-exchange energy, represents the state-of-the-art exchange-correlation functional within density-functional theory (DFT). However, the standard…

Other Condensed Matter · Physics 2015-05-20 Xinguo Ren , Patrick Rinke , Alexandre Tkatchenko , Matthias Scheffler

Embedded density functional theory (e-DFT) is used to describe the electronic structure of strongly interacting molecular subsystems. We present a general implementation of the Exact Embedding (EE) method [J. Chem. Phys. 133, 084103 (2010)]…

Other Condensed Matter · Physics 2011-07-27 Jason D. Goodpaster , Taylor A. Barnes , Thomas F. Miller

Kohn-Sham density functional theory (DFT) is nowadays widely used for electronic structure theory simulations, and the accuracy and efficiency of DFT rely on approximations of the exchange-correlation functional. By inclusion of the kinetic…

Materials Science · Physics 2023-06-01 Renxi Liu , Daye Zheng , Xinyuan Liang , Xinguo Ren , Mohan Chen , Wenfei Li

Density functional approximations to the exchange-correlation energy of Kohn-Sham theory, such as the local density approximation and generalized gradient approximations, lack the well-known integer discontinuity, a feature that is critical…

Chemical Physics · Physics 2015-06-18 Martin A. Mosquera , Adam Wasserman

In this work we have studied a new functional for the correlation energy obtained from the exact-exchange (EXX) approximation within time-dependent density functional theory (TDDFT). Correlation energies have been calculated for a number of…

Mesoscale and Nanoscale Physics · Physics 2015-05-14 Maria Hellgren , Ulf von Barth

It has long been postulated that within density-functional theory (DFT) the total energy of a finite electronic system is convex with respect to electron count, so that 2 E_v[N_0] <= E_v[N_0 - 1] + E_v[N_0 + 1]. Using the…

Chemical Physics · Physics 2023-12-25 Andrew C. Burgess , Edward Linscott , David D. O'Regan

We present calculations of the correlation energies of crystalline solids and isolated systems within the adiabatic-connection fluctuation-dissipation formulation of density-functional theory. We perform a quantitative comparison of a set…

Materials Science · Physics 2016-07-29 Christopher E. Patrick , Kristian S. Thygesen

Quantum-electrodynamical density-functional theory (QEDFT) provides a promising avenue for exploring complex light-matter interactions in optical cavities for real materials. Similar to conventional density-functional theory, the Kohn-Sham…

Computational Physics · Physics 2024-02-16 I-Te Lu , Michael Ruggenthaler , Nicolas Tancogne-Dejean , Simone Latini , Markus Penz , Angel Rubio

We study non-linear adiabatic connection paths in density-functional theory using modified electron-electron interactions that perform a long-range/short-range separation of the Coulomb interaction. These adiabatic connections allows to…

Chemical Physics · Physics 2009-11-11 Julien Toulouse , Francois Colonna , Andreas Savin

In contrast to the original Kohn-Sham (KS) formalism, we propose a density functional theory (DFT) with fractional orbital occupations for the study of ground states of many-electron systems, wherein strong static correlation is shown to be…

Chemical Physics · Physics 2015-06-03 Jeng-Da Chai

Recent experimental advances in strongly coupled light-matter systems has sparked the development of general ab-initio methods capable of describing interacting light-matter systems from first principles. One of these methods,…

Chemical Physics · Physics 2022-10-12 Johannes Flick