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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

The predominance of Kohn-Sham density functional theory (KS-DFT) for the theoretical treatment of large experimentally relevant systems in molecular chemistry and materials science relies primarily on the existence of efficient software…

Computational Physics · Physics 2020-07-08 David B. Williams-Young , Wibe A. de Jong , Hubertus J. J. van Dam , Chao Yang

Ryabinkin, Kohut, and Staroverov (RKS) [Phys. Rev. Lett. 115, 083001 (2015)] devised an iterative method for reducing many-electron wave functions to Kohn-Sham exchange-correlation potentials, $v_\text{XC}(\mathbf{r})$. For a given type of…

Chemical Physics · Physics 2017-02-27 Egor Ospadov , Ilya G. Ryabinkin , Viktor N. Staroverov

We present a new density-functional method of the self-consistent electronic-structure calculation which does not exploit any local density approximations (LDA). We use the exchange-correlation energy which consists of the exact exchange…

Statistical Mechanics · Physics 2009-10-30 Takao Kotani

Explicitly orbital-dependent approximations to the exchange-correlation energy functional of density functional theory typically not only depend on the single-particle Kohn-Sham orbitals but also on their occupation numbers in the ground…

Materials Science · Physics 2009-05-14 S. Kurth , C. R. Proetto , K. Capelle

The frequency-dependent exchange-correlation potential, which appears in the usual Kohn-Sham formulation of a time-dependent linear response problem, is a strongly nonlocal functional of the density, so that a consistent local density…

Condensed Matter · Physics 2009-10-28 G. Vignale , Walter Kohn

Popular density functionals for the exchange-correlation energy typically fail to reproduce the degeneracy of different ground states of open-shell atoms. As a remedy, functionals which explicitly depend on the current density have been…

Materials Science · Physics 2007-07-31 S. Pittalis , S. Kurth , S. Sharma , E. K. U. Gross

In ab initio pseudopotential calculations within density-functional theory the nonlinear exchange-correlation interaction between valence and core electrons is often treated linearly through the pseudopotential. We discuss the accuracy and…

Materials Science · Physics 2009-10-30 Martin Fuchs , Michel Bockstedte , Eckhard Pehlke , Matthias Scheffler

The prominence of density functional theory (DFT) in the field of electronic structure computation stems from its ability to usefully balance accuracy and computational effort. At the base of this ability is a functional of the electron…

A simple, novel, non-empirical, constraint-based orbital-free generalized gradient approximation (GGA) non-interacting kinetic energy density functional is presented along with illustrative applications. The innovation is adaptation of…

Chemical Physics · Physics 2018-08-01 K. Luo , V. V. Karasiev , S. B. Trickey

For exchange-correlation functionals that depend explicitly on the Kohn-Sham orbitals, the potential $V_{\mathrm{xc}\sigma}(\re)$ must be obtained as the solution of the optimized effective potential (OEP) integral equation. This is very…

Materials Science · Physics 2009-11-07 Stephan Kümmel , John P. Perdew

We formulate an adiabatic connection for the exchange-correlation energy in terms of pairing matrix fluctuation. This connection opens new channels for density functional approximations based on pairing interactions. Even the simplest…

Chemical Physics · Physics 2015-06-16 Helen van Aggelen , Yang Yang , Weitao Yang

Most density functionals have been developed by imposing the known exact constraints on the exchange-correlation energy, or by a fit to a set of properties of selected systems, or by both. However, accurate modeling of the conventional…

Materials Science · Physics 2016-08-24 Jianmin Tao , Yuxiang Mo

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

We present an efficient real space formalism for hybrid exchange-correlation functionals in generalized Kohn-Sham density functional theory (DFT). In particular, we develop an efficient representation for any function of the real space…

Computational Physics · Physics 2024-06-26 Xin Jing , Phanish Suryanarayana

Spin-orbit coupling induces a current density in the ground state, which consequently requires a generalization for meta-generalized gradient approximations. That is, the exchange-correlation energy has to be constructed as an explicit…

Chemical Physics · Physics 2024-05-09 Yannick J. Franzke , Christof Holzer

For orbital-free {\it ab initio} molecular dynamics, especially on systems in extreme thermodynamic conditions, we provide the first pseudo-potential-adapted generalized gradient approximation (GGA) functional for the non-interacting free…

Chemical Physics · Physics 2020-02-19 Kai Luo , Valentin V. Karasiev , S. B. Trickey

Using the Kohn-Sham (KS) inversion method of Hollins et al. [J. Phys.: Condens. Matter 29, 04LT01 (2017)], we invert densities from variational and diffusion quantum Monte Carlo (QMC) calculations to obtain benchmark QMC-KS potentials for a…

This paper presents a novel Riemannian conjugate gradient method for the Kohn-Sham energy minimization problem in density functional theory (DFT), with a focus on non-metallic crystal systems. We introduce an energy-adaptive metric that…

Numerical Analysis · Mathematics 2025-03-21 Daniel Peterseim , Jonas Püschel , Tatjana Stykel

We propose a new generalised Kohn-Sham or constrained hybrid method, where the exchange potential is the (equally weighted) average of the nonlocal Fock exchange term and the self-interaction-corrected exchange potential, as obtained from…

Chemical Physics · Physics 2022-01-05 Thomas C. Pitts , Nektarios N. Lathiotakis , Nikitas I. Gidopoulos
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