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Certain excitations, especially ones of long-range charge transfer character, are poorly described by time-dependent density functional theory (TDDFT) when typical (semi-)local functionals are used. A proper description of these excitations…

Chemical Physics · Physics 2018-08-01 J. Garhammer , F. Hofmann , R. Armiento , S. Kümmel

The exchange-correlation potentials stemming from the local-density approximation and several generalized-gradient approximations are known to have incorrect asymptotic decay. This failure is independent of the dimensionality, but so far…

Strongly Correlated Electrons · Physics 2010-09-01 S. Pittalis , E. Rasanen

The augmented potential introduced by Levy and Zahariev [Phys. Rev. Lett. 113, 113002 (2014)] is shifted with respect to the standard exchange-correlation potential of Kohn-Sham density functional theory by a density-dependent constant that…

Chemical Physics · Physics 2018-01-17 Stefan Vuckovic , Mel Levy , Paola Gori-Giorgi

An accurate analytical parametrization for the exchange-correlation free energy of the homogeneous electron gas, including interpolation for partial spin-polarization, is derived via thermodynamic analysis of recent restricted path integral…

Chemical Physics · Physics 2015-06-17 Valentin V. Karasiev , Travis Sjostrom , James Dufty , S. B. Trickey

We present a global hybrid meta-generalized gradient approximation (meta-GGA) with three empirical parameters, as well as its underlying semilocal meta-GGA and a meta-GGA with only one empirical parameter. All of them are based on the new…

Orbital-free density functional theory as an extension of traditional Thomas-Fermi theory has attracted a lot of interest in the past decade because of developments in both more accurate kinetic energy functionals and highly efficient…

Materials Science · Physics 2009-11-10 Hong Jiang , Weitao Yang

We investigate basic hydrogen quantities like the molecular bond length, the molecular dissociation energy and the van-der-Waals interaction in idealized situations in an effort to discern a suitable exchange-correlation functional for the…

We use the exact strong-interaction limit of the Hohenberg-Kohn energy density functional to approximate the exchange-correlation energy of the restricted Kohn-Sham scheme. Our approximation corresponds to a highly non-local density…

Strongly Correlated Electrons · Physics 2012-12-12 Francesc Malet , Paola Gori-Giorgi

A Neural-Networks-based approach is proposed to construct a new type of exchange-correlation functional for density functional theory. It is applied to improve B3LYP functional by taking into account of high-order contributions to the…

Chemical Physics · Physics 2009-11-10 Xiao Zheng , LiHong Hu , XiuJun Wang , GuanHua Chen

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

We show that the Kohn-Sham positive-definite kinetic energy (KE) density significantly differs from the von Weizs\"acker (VW) one at the nuclear cusp as well as in the asymptotic region. At the nuclear cusp, the VW functional is shown to be…

Chemical Physics · Physics 2015-02-03 F. Della Sala , E. Fabiano , L. A. Constantin

It is shown here that Kohn-Sham equations cannot be derived from Hohenberg-Kohn theory without an additional postulate. Assuming that a functional derivative with respect to total electron density exists leads in general to a theory…

Condensed Matter · Physics 2007-05-23 R. K. Nesbet

A decade ago Rhie \et (Phys. Rev. Lett. {\bf 90}, 247201 (2003)) reported that when ferromagnetic nickel is subject to an intense ultrashort laser pulse, its exchange splitting is reduced quickly. But to simulate such reduction remains a…

Materials Science · Physics 2016-11-15 G. P. Zhang , Y. H. Bai , Thomas F. George

Despite the great success Kohn-Sham density functional theory (KS-DFT) has achieved, the delocalization error remains a major challenge for commonly used density functional approximations (DFAs), resulting in systematic errors in ionization…

Chemical Physics · Physics 2026-02-12 Yichen Fan , Jincheng Yu , Jiayi Du , Weitao Yang

We propose a novel approach to the problem of polarizabilities and dissociation in electric fields from the static limit of the Vignale-Kohn (VK) functional. We consider the response to the purely scalar part of the VK response…

Materials Science · Physics 2009-11-11 Neepa T. Maitra , Meta van Faassen

As a proof of principle, self-consistent Kohn--Sham calculations are performed with the exact exchange-correlation functional. Finding the exact functional for even one trial density requires solving the interacting Schr\"odinger equation…

Chemical Physics · Physics 2014-07-14 Lucas O. Wagner , Thomas E. Baker , E. M. Stoudenmire , Kieron Burke , Steven R. White

We introduced a new electron density n({\epsilon}) by projecting the spatial electron density n(r) onto the energy coordinate {\epsilon} defined with the external potential \upsion (r) of interest. Then, a density functional theory (DFT)…

Chemical Physics · Physics 2018-02-20 Hideaki Takahashi

We present a substantial extension of our constraint-based approach for development of orbital-free (OF) kinetic-energy (KE) density functionals intended for the calculation of quantum-mechanical forces in multi-scale molecular dynamics…

Materials Science · Physics 2015-05-13 V. V. Karasiev , R. S. Jones , S. B. Trickey , Frank E. Harris

We model the exchange-correlation (XC) energy density of the Si crystal and atom as calculated by variational Monte Carlo (VMC) methods with a gradient analysis beyond the local density approximation (LDA). We find the Laplacian of the…

Materials Science · Physics 2009-11-11 Antonio C. Cancio , M. Y. Chou

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
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