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This article is concerned with the mathematical analysis of the Kohn-Sham and extended Kohn-Sham models, in the local density approximation (LDA) and generalized gradient approximation (GGA) frameworks. After recalling the mathematical…

Quantum Physics · Physics 2008-10-01 Arnaud Anantharaman , Eric Cancès

Localized molecular orbitals are often used for the analysis of chemical bonds, but they can also serve to efficiently and comprehensibly compute linear response properties. While conventional canonical molecular orbitals provide an…

Chemical Physics · Physics 2023-02-08 Souloke Sen , Bruno Senjean , Lucas Visscher

We present a physically motivated correlation functional belonging to the meta-generalized gradient approximation (meta-GGA) rung, which can be supplemented with long-range dispersion corrections without introducing double-counting of…

We perform systematic density functional theory (DFT) calculations to assess the performance of various exchange-correlation potentials $V_{xc}$ in describing the chalcogenide GaM$_4$Q$_8$ lacunar spinels (M=Mo, V, Nb, Ta; Q=S, Se). We…

Materials Science · Physics 2019-09-25 Yiqun Wang , Danilo Puggioni , James M. Rondinelli

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

We study static correlation and delocalisation errors and show that even methods with good energies can yield significant delocalization errors that affect the density, leading to large errors in predicting {\em e.g.} dipole moments. We…

Chemical Physics · Physics 2020-06-01 Maria Hellgren , Tim Gould

Density functional theory (DFT) embedding provides a formally exact framework for interfacing correlated wave-function theory (WFT) methods with lower-level descriptions of electronic structure. Here, we report techniques to improve the…

Chemical Physics · Physics 2015-06-12 Jason D. Goodpaster , Taylor A. Barnes , Frederick R. Manby , Thomas F. Miller

We introduce in detail our newly developed \textit{ab initio} LDA+Gutzwiller method, in which the Gutzwiller variational approach is naturally incorporated with the density functional theory (DFT) through the "Gutzwiller density functional…

Strongly Correlated Electrons · Physics 2013-05-29 XiaoYu Deng , Lei Wang , Xi Dai , Zhong Fang

Kohn-Sham Density Functional Theory (KS-DFT) provides the exact ground state energy and electron density of a molecule, contingent on the as-yet-unknown universal exchange-correlation (XC) functional. Recent research has demonstrated that…

We study the accuracy of Kohn-Sham density functional theory (DFT) for warm- and hot-dense matter (WDM and HDM). Specifically, considering a wide range of systems, we perform accurate ab initio molecular dynamics simulations with…

Computational Physics · Physics 2024-11-21 Phanish Suryanarayana , Arpit Bhardwaj , Xin Jing , Shashikant Kumar , John E. Pask

The random phase approximation (RPA) for the correlation energy functional of density functional theory has recently attracted renewed interest. Formulated in terms of the Kohn-Sham (KS) orbitals and eigenvalues, it promises to resolve some…

Other Condensed Matter · Physics 2009-11-13 Hong Jiang , Eberhard Engel

We propose a generalized gradient approximation (GGA) for the angle- and system-averaged exchange-correlation hole of a many-electron system. This hole, which satisfies known exact constraints, recovers the PBEsol (Perdew-Burke-Ernzerhof…

Materials Science · Physics 2009-11-13 Lucian A. Constantin , John P. Perdew , J. M. Pitarke

In this paper, we propose a new Green's function embedding method called PEXSI-$\Sigma$ for describing complex systems within the Kohn-Sham density functional theory (KSDFT) framework, after revisiting the physics literature of Green's…

Computational Physics · Physics 2016-10-20 Xiantao Li , Lin Lin , Jianfeng Lu

Quasiparticle energies and fundamental band gaps in particular are critical properties of molecules and materials. It was rigorously established that the generalized Kohn-Sham HOMO and LUMO orbital energies are the chemical potentials of…

Chemical Physics · Physics 2019-03-06 Yuncai Mei , Chen Li , Neil Qiang Su , Weitao Yang

Efficient hybrid DFT simulations of solid state materials would be extremely beneficial for computational chemistry and materials science, but is presently bottlenecked by difficulties in computing Hartree-Fock (HF) exchange with plane wave…

Chemical Physics · Physics 2024-10-30 Yuanheng Wang , Diptarka Hait , Pablo A. Unzueta , Juncheng Harry Zhang , Todd J. Martínez

The development of kinetic energy functional (KEF) is known as one of the most difficult subjects in the electronic density functional theory (DFT). In particular, the sound description of chemical bonds using a KEF is a matter of great…

Chemical Physics · Physics 2025-03-03 Hideaki Takahashi

Density Functional Theory (DFT) is a pivotal method within quantum chemistry and materials science, with its core involving the construction and solution of the Kohn-Sham Hamiltonian. Despite its importance, the application of DFT is…

Recently, Tao and Mo proposed an accurate meta-generalized gradient approximation for the exchange-correlation energy. The exchange part is derived from the density matrix expansion, while the correlation part is obtained by improving the…

Chemical Physics · Physics 2017-10-11 Yuxiang Mo , Guocai Tian , Jianmin Tao

A systematic way of improving exchange-correlation energy functionals of density functional theory has been to make them satisfy more and more exact relations. Starting from the initial GGA functionals, this has culminated into the recently…

Chemical Physics · Physics 2017-10-11 Rabeet Singh , Manoj K. Harbola

The local density approximation (LDA) constructed through quantum Monte Carlo calculations of the homogeneous electron gas (HEG) is the most common approximation to the exchange-correlation functional in density functional theory. We…

Other Condensed Matter · Physics 2021-01-15 Mike Entwistle , Matthew Hodgson , Jack Wetherell , Bradley Longstaff , James Ramsden , Rex Godby
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