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A method for calculating the Kohn--Sham exchange-correlation potential, $v_\text{XC}(\mathbf{r})$, from a given electronic wavefunction is devised and implemented. It requires on input one- and two-electron density matrices and involves…

Chemical Physics · Physics 2015-08-19 Ilya G. Ryabinkin , Sviataslau V. Kohut , Viktor N. Staroverov

We examine the density-functional theory of macroscopic insulators, obtained in the large-cluster limit or under periodic boundary conditions. For polar crystals, we find that the two procedures are not equivalent. In a large-cluster case,…

Materials Science · Physics 2009-10-28 X. Gonze , Ph. Ghosez , R. W. Godby

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

By extrapolating the energies of non-relativistic atoms and their ions with up to 3000 electrons within Kohn-Sham density functional theory, we find that the ionization potential remains finite and increases across a row, even as…

Materials Science · Physics 2015-05-19 Lucian A. Constantin , John C. Snyder , John P. Perdew , Kieron Burke

We argue that the success of DFT can be understood in terms of a semiclassical expansion around a very specific limit. This limit was identified long ago by Lieb and Simon for the total electronic energy of a system. This is a universal…

Chemical Physics · Physics 2021-05-18 Pavel Okun , Kieron Burke

The density functional theory originally developed by Hohenberg, Kohn and Sham provides a rigorous conceptual framework for dealing with inhomogeneous interacting Fermi systems. We extend this approach to deal with inhomogeneous interacting…

Condensed Matter · Physics 2015-06-25 A. Griffin

We analyze the various approaches to construct exchange-correlation functionals which are able to describe states of definite spin multiplicity in the DFT realm and outline the characteristics of possible functionals consistent with the…

Chemical Physics · Physics 2019-01-04 A. L. Tchougréeff , J. G. Ángyán

Density functional theory is generalized to incorporate electron-phonon coupling. A Kohn-Sham equation yielding the electronic density $n_U(\mathbf{r})$, a conditional probability density depending parametrically on the phonon normal mode…

Materials Science · Physics 2019-04-25 Ryan Requist , C. R. Proetto , E. K. U. Gross

The accurate prediction of electronic response properties of extended molecular systems has been a challenge for conventional, explicit density functionals. We demonstrate that a self-interaction correction implemented rigorously within…

Materials Science · Physics 2009-11-13 T. Körzdörfer , M. Mundt , S. Kümmel

With the development of low order scaling methods for performing Kohn-Sham Density Functional Theory, it is now possible to perform fully quantum mechanical calculations of systems containing tens of thousands of atoms. However, with an…

Chemical Physics · Physics 2020-04-03 William Dawson , Stephan Mohr , Laura E. Ratcliff , Takahito Nakajima , Luigi Genovese

Density functional theory can be extended to excited states by means of a unified variational approach for passive state ensembles. This extension overcomes the restriction of the typical density functional approach to ground states, and…

Chemical Physics · Physics 2019-07-10 Tim Gould , Stefano Pittalis

The correlation energy in density functional theory can be expressed exactly in terms of the change in the probability of finding two electrons at a given distance $r_{12}$ (intracule density) when the electron-electron interaction is…

Other Condensed Matter · Physics 2017-08-23 Paola Gori-Giorgi , Michael Seidl , Andreas Savin

First-principles calculations based on density functional theory have been widely used in studies of the structural, thermoelastic, rheological, and electronic properties of earth-forming materials. The exchange-correlation term, however,…

Computational Physics · Physics 2009-11-13 S. H. Lee , Jones T. K. Wan

We generalize the exact strong-interaction limit of the exchange-correlation energy of Kohn-Sham density functional theory to open systems with fluctuating particle numbers. When used in the self-consistent Kohn-Sham procedure on…

Strongly Correlated Electrons · Physics 2015-06-16 André Mirtschink , Michael Seidl , Paola Gori-Giorgi

Starting from the observation that one of the most successful methods for solving the Kohn-Sham equations for periodic systems -- the plane-wave method -- is a spectral method based on eigenfunction expansion, we formulate a spectral method…

Computational Physics · Physics 2016-03-08 Amartya S. Banerjee , Ryan S. Elliott , Richard D. James

The reconstruction of the exchange-correlation potential from accurate ab initio electron densities can provide insights into the limitations of the currently available approximate functionals and provide guidance for devising improved…

Strongly Correlated Electrons · Physics 2013-02-05 Katharina Boguslawski , Christoph R. Jacob , Markus Reiher

A sufficiently damped iteration of the Kohn-Sham equations with the exact functional is proven to always converge to the true ground-state density, regardless of the initial density or the strength of electron correlation, for finite…

Materials Science · Physics 2013-08-30 Lucas O. Wagner , E. M. Stoudenmire , Kieron Burke , Steven R. White

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

We introduce an orbital free electron density functional approximation based on alchemical perturbation theory. Given convergent perturbations of a suitable reference system, the accuracy of popular self-consistent Kohn-Sham density…

Chemical Physics · Physics 2020-05-27 Guido Falk von Rudorff , O. Anatole von Lilienfeld

We use spin-density functional theory to obtain novel expressions for the charge and spin local-field factors of an electron gas in terms of its electron-pair structure factors. These expressions (i) satisfy the compressibility and spin…

Strongly Correlated Electrons · Physics 2009-11-07 B. Davoudi , M. Polini , M. P. Tosi