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A very specific ensemble of ground and excited states is shown to yield an exact formula for any excitation energy as a simple correction to the energy difference between orbitals of the Kohn-Sham ground state. This alternative scheme…

Chemical Physics · Physics 2017-07-26 Zeng-hui Yang , Aurora Pribram-Jones , Kieron Burke , Carsten A. Ullrich

Over the past decade, fundamentals of time independent density functional theory for excited state have been established. However, construction of the corresponding energy functionals for excited states remains a challenging problem. We…

Other Condensed Matter · Physics 2012-03-06 M. Hemanadhan , Manoj K. Harbola

A widely used approximation to the exchange-correlation functional in density functional theory is the local density approximation (LDA), typically derived from the properties of the homogeneous electron gas (HEG). We previously introduced…

Other Condensed Matter · Physics 2018-06-27 Mike Entwistle , Michele Casula , Rex Godby

We present an approach for accurate calculation of exchange energy and total energy for excited states using time independent density functional formalism. This is done by inclusion of gradient correction into the excited state exchange…

Chemical Physics · Physics 2012-01-31 Md. Shamim , Manoj K. Harbola

We propose exchanging the energy functionals in ground-state DFT with physically equivalent exact force expressions as a new promising route towards approximations to the exchange-correlation potential and energy. In analogy to the usual…

The ground state of an homogeneous electron gas is a paradigmatic state that has been used to model and predict the electronic structure of matter at equilibrium for nearly a century. For half a century, it has been successfully used to…

Chemical Physics · Physics 2024-06-11 Tim Gould , Stefano Pittalis

Density functional theory has become the workhorse of quantum physics, chemistry, and materials science. Within these fields, a broad range of applications needs to be covered. These applications range from solids to molecular systems, from…

Chemical Physics · Physics 2025-01-20 Christof Holzer , Yannick J. Franzke

We extend ground-state density-functional theory to excited states and provide the theoretical formulation for the widely used $\Delta SCF$ method for calculating excited-state energies and densities. As the electron density alone is…

Chemical Physics · Physics 2024-03-08 Weitao Yang , Paul W. Ayers

A review of the approximations in any time-dependent density functional calculation of excitation energies is given. The single-pole approximation for the susceptibility is used to understand errors in popular approximations for the…

Materials Science · Physics 2007-05-23 Kieron Burke , Martin Petersilka , E. K. U. Gross

Based on exact limits and quantum Monte Carlo simulations, we obtain, at any density and spin polarization, an accurate estimate for the energy of a modified homogeneous electron gas where electrons repel each other only with a long-range…

Materials Science · Physics 2009-11-11 Simone Paziani , Saverio Moroni , Paola Gori-Giorgi , Giovanni B. Bachelet

We introduce a new functional for simulating ground-state and time-dependent electronic systems within density-functional theory. The functional combines an expression for the exact Kohn-Sham (KS) potential in the limit of complete electron…

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

Time-dependent density functional theory (TDDFT) is presently enjoying enormous popularity in quantum chemistry, as a useful tool for extracting electronic excited state energies. This article explains what TDDFT is, and how it differs from…

Materials Science · Physics 2007-05-23 Peter Elliott , Kieron Burke , Filipp Furche

The force-balance equation of time-dependent density-functional theory presents a promising route towards obtaining approximate functionals, however, so far, no practical correlation functionals have been derived this way. In this work,…

Chemical Physics · Physics 2025-04-08 Nicolas Tancogne-Dejean , Markus Penz , Michael Ruggenthaler , Angel Rubio

The generator-coordinate method is a flexible and powerful reformulation of the variational principle. Here we show that by introducing a generator coordinate in the Kohn-Sham equation of density-functional theory, excitation energies can…

Chemical Physics · Physics 2009-11-09 E. Orestes , A. B. F. da Silva , K. Capelle

We present an alternative to the Kohn-Sham formulation of density functional theory for the ground-state properties of strongly interacting electronic systems. The idea is to start from the limit of zero kinetic energy and systematically…

Strongly Correlated Electrons · Physics 2015-05-13 Paola Gori-Giorgi , Michael Seidl , G. Vignale

We derive a local approximation for the correlation energy in two-dimensional electronic systems. In the derivation we follow the scheme originally developed by Colle and Salvetti for three dimensions, and consider a Gaussian approximation…

Strongly Correlated Electrons · Physics 2008-11-21 S. Pittalis , E. Rasanen , M. Marques

We present an accurate local density-functional for electronic-structure calculations within the density functional theory (DFT). The functional is derived by analyzing the structure of the standard perturbative expansion of the correlation…

Materials Science · Physics 2024-11-28 Mario Benites , Angel Rosado , Efstratios Manousakis

We discuss energy densities in the strong-interaction limit of density functional theory, deriving an exact expression within the definition (gauge) of the electrostatic potential of the exchange-correlation hole. Exact results for small…

Chemical Physics · Physics 2012-11-14 André Mirtschink , Michael Seidl , Paola Gori-Giorgi

We construct a generalized-gradient approximation for the exchange-energy density of finite two-dimensional systems. Guided by non-empirical principles, we include the proper small-gradient limit and the proper tail for the exchange-hole…

Strongly Correlated Electrons · Physics 2014-03-26 J. G. Vilhena , E. Rasanen , M. A. L. Marques , S. Pittalis

We report a local, weight-dependent correlation density-functional approximation that incorporates information about both ground and excited states in the context of density-functional theory for ensembles (eDFT). This density-functional…

Chemical Physics · Physics 2020-06-05 Pierre-François Loos , Emmanuel Fromager