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We present, within Kohn-Sham Density Functional Theory calculations, a quantitative method to identify and assess the partitioning of a large quantum mechanical system into fragments. We then show how within this framework simple…

Chemical Physics · Physics 2017-09-28 Stephan Mohr , Michel Masella , Laura E. Ratcliff , Luigi Genovese

The derivative discontinuity of the exchange-correlation functional of density-functional theory is cast as the difference of two types of electron affinities. We show that standard Kohn-Sham calculations can be used to calculate both…

Chemical Physics · Physics 2007-12-13 F. P. Rosselli , A. B. F. da Silva , K. Capelle

The most widely-used density functionals for the exchange-correlation energy are inexact for one-electron systems. Their self-interaction errors can be severe in some applications. The problem is not only to correct the self-interaction…

Chemical Physics · Physics 2009-11-10 Stephan Kümmel , John P. Perdew

We present a density difference based analysis for a range of orbital--dependent Kohn--Sham functionals. Results for atoms, some members of the neon isoelectronic series and small molecules are reported and compared with ab initio…

Chemical Physics · Physics 2015-01-22 I. Grabowski , A. M. Teale , E. Fabiano , S. Smiga , A. Buksztel , F. Della Sala

In this paper, we investigate the energy minimization model of the ensemble Kohn-Sham density functional theory for metallic systems, in which a pseudo-eigenvalue matrix and a general smearing approach are involved. We study the invariance…

Numerical Analysis · Mathematics 2022-01-19 Xiaoying Dai , Stefano de Gironcoli , Bin Yang , Aihui Zhou

The constrained electron density method of embedding a Kohn-Sham system in a substrate system (first described by P. Cortona, Phys. Rev. B {\bf 44}, 8454 (1991) and T.A. Wesolowski and A. Warshel, J. Phys. Chem {\bf 97}, 8050 (1993)) is…

Materials Science · Physics 2015-05-14 J. R. Trail , D. M. Bird

Density Functional Theory (DFT) is one of the most widely used methods for "ab initio" calculations of the structure of atoms, molecules, crystals, surfaces, and their interactions. Unfortunately, the customary introduction to DFT is often…

Physics Education · Physics 2010-12-07 Nathan Argaman , Guy Makov

The recently developed Deep Potential [Phys. Rev. Lett. 120, 143001, 2018] is a powerful method to represent general inter-atomic potentials using deep neural networks. The success of Deep Potential rests on the proper treatment of locality…

Computational Physics · Physics 2019-12-05 Leonardo Zepeda-Núñez , Yixiao Chen , Jiefu Zhang , Weile Jia , Linfeng Zhang , Lin Lin

We investigate from a practitioner's point of view the computation of the ionization potential (IP) within density functional theory (DFT). DFT with (semi-)local energy-density functionals is plagued by a self-interaction error which…

Atomic and Molecular Clusters · Physics 2015-06-16 Peter Klüpfel , Mai Phuong Dinh , Paul-Gerhard Reinhard , Eric Suraud

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

Degenerate perturbation theory from quantum mechanics is inadequate in density functional theory (DFT) because of nonlinearity in the Kohn-Sham potential. Herein, we develop the fully general perturbation theory for open-shell, degenerate…

Materials Science · Physics 2017-07-19 Mark C. Palenik , Brett I. Dunlap

The reliability of density-functional calculations hinges on accurately approximating the unknown exchange-correlation (xc) potential. Common (semi-)local xc approximations lack the jump experienced by the exact xc potential as the number…

Atomic Physics · Physics 2021-01-15 M. J. P. Hodgson , E. Kraisler , E. K. U. Gross

We develop a method in which the electronic densities of small fragments determined by Kohn-Sham density functional theory (DFT) are embedded using stochastic DFT to form the exact density of the full system. The new method preserves the…

Chemical Physics · Physics 2015-06-19 Daniel Neuhauser , Roi Baer , Eran Rabani

Understanding many processes, e.g. fusion experiments, planetary interiors and dwarf stars, depends strongly on microscopic physics modeling of warm dense matter (WDM) and hot dense plasma. This complex state of matter consists of a…

Computational Physics · Physics 2020-08-05 Alexander J. White , Lee A. Collins

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

A density functional theory (DFT) framework is presented that links functional derivatives of free-energy functionals to non-linear static density response functions in quantum many-body systems. Within this framework, explicit expressions…

We propose a hybrid approach which employs the dynamical mean-field theory (DMFT) self-energy for the correlated, typically rather localized orbitals and a conventional density functional theory (DFT) exchange-correlation potential for the…

Strongly Correlated Electrons · Physics 2021-06-16 Sumanta Bhandary , Karsten Held

Here we present a density matrix based KS inversion method formulated entirely within a Gaussian basis representation to optimize a KS potential matrix that reproduces a target electron density. Inverse Kohn-Sham (KS) density functional…

Chemical Physics · Physics 2026-03-24 Ziwei Chai , Sandra Luber

We present an implementation of the optimised effective potential (OEP) scheme for the exact-exchange (EXX) and random phase approximation (RPA) energy functionals and apply these methods to a range of bulk materials. We calculate the…

Materials Science · Physics 2014-05-16 Jiří Klimeš , Georg Kresse

Capturing the discontinuous shift by $\Delta$ in the exact exchange-correlation (xc) potential is the standard proposal for calculating the fundamental gap, $E_\mathrm{g}$, from the Kohn-Sham (KS) gap, $\varepsilon_\mathrm{g}$, within KS…

Materials Science · Physics 2021-01-14 M. J. P. Hodgson , J. Wetherell , Emmanuel Fromager
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