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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

Despite of its huge successes in vast amount of applications, the Kohn-Sham scheme of density functional theory (DFT-Kohn-Sham) has not been able to get reliable ionization potentials (IP) for semiconductors, due to self-interaction error…

Materials Science · Physics 2016-04-07 Lin-Hui Ye

We calculate the exact Kohn-Sham potential that describes, within time-dependent density-functional theory, the propagation of an electron quasiparticle wavepacket of non-zero crystal momentum added to a ground-state model semiconductor.…

Mesoscale and Nanoscale Physics · Physics 2015-06-05 J. D. Ramsden , R. W. Godby

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

Informed by an abstraction of Kohn-Sham computation called a KS machine, a functional analytic perspective is developed on mathematical aspects of density functional theory. A natural semantics for the machine is bivariate, consisting of a…

Other Condensed Matter · Physics 2023-09-25 Paul E. Lammert

The finite basis optimized effective potential (OEP) method within density functional theory is examined as an ill-posed problem. It is shown that the generation of nonphysical potentials is a controllable manifestation of the use of…

Materials Science · Physics 2009-11-11 Tim Heaton-Burgess , Felipe A. Bulat , Weitao Yang

Kohn-Sham regularizer (KSR) is a differentiable machine learning approach to finding the exchange-correlation functional in Kohn-Sham density functional theory (DFT) that works for strongly correlated systems. Here we test KSR for weak…

Chemical Physics · Physics 2022-03-22 Bhupalee Kalita , Ryan Pederson , Jielun Chen , Li Li , Kieron Burke

We present here novel insight into exchange-correlation functionals in density functional theory, based on the viewpoint of optimal transport. We show that in the case of two electrons and in the semiclassical limit, the exact…

Analysis of PDEs · Mathematics 2015-03-19 Codina Cotar , Gero Friesecke , Claudia Klüppelberg

From a simplified version of the mathematical structure of the strong coupling limit of the exact exchange-correlation functional, we construct an approximation for the electronic repulsion energy at physical coupling strength, which is…

Chemical Physics · Physics 2017-05-11 Stefan Vuckovic , Paola Gori-Giorgi

The optimized effective potential method is formulated as a convex minimization problem. This formulation does not require assumptions about $v$-representability nor functional differentiability. The formulation provides a natural framework…

Chemical Physics · Physics 2022-02-01 Erik I. Tellgren , Andre Laestadius , Markus Penz

Kohn-Sham density functional theory is the base of modern computational approaches to electronic structures. Their accuracy vitally relies on the exchange-correlation energy functional, which encapsulates electron-electron interaction…

Computational Physics · Physics 2019-11-04 Ryo Nagai , Ryosuke Akashi , Osamu Sugino

Most of the density-to-potential inversion methods developed over the years follow a general algorithm $ v_{xc}^{i+1}(\textbf{r}) = v_{xc}^{i}(\textbf{r}) + \Delta v_{xc}(\textbf{r})$, where $\Delta v_{xc}(\textbf{r}) = \frac{\delta…

Atomic Physics · Physics 2021-07-28 Ashish Kumar , Manoj K. Harbola

This is a comprehensive review of the strong-interaction limit of density functional theory. It covers the derivation of the limiting strictly correlated electrons (SCE) functional from exact Hohenberg-Kohn DFT, basic aspects of SCE physics…

Chemical Physics · Physics 2022-02-22 Gero Friesecke , Augusto Gerolin , Paola Gori-Giorgi

By exploiting freedoms in the definitions of 'correlation', 'exchange' and 'Hartree' physics in ensemble systems we better generalise the notion of 'exact exchange' (EXX) to systems with fractional occupations functions of the frontier…

Atomic Physics · Physics 2014-07-28 Tim Gould , John F. Dobson

The effective potential of electron--electron interaction and the two-particle \textquotedblleft density--density\textquotedblright\ correlation function have been calculated for a simple semiinfinite metal making allowance for the…

Mesoscale and Nanoscale Physics · Physics 2015-03-29 B. M. Markovych , I. M. Zadvorniak

We present SPARC-atomSFE, a spectral finite-element package for accurate and efficient atomic structure calculations within the framework of Kohn-Sham density functional theory. The package supports both all-electron and norm conserving…

Computational Physics · Physics 2026-05-19 Qihao Cheng , Shubhang Krishnakant Trivedi , Phanish Suryanarayana

Inverse Kohn-Sham (iKS) problems are needed to fully understand the one-to-one mapping between densities and potentials on which Density Functional Theory is based. They are also important to advance computational schemes that rely on…

Chemical Physics · Physics 2021-07-06 Yuming Shi , Adam Wasserman

Accurate local Kohn-Sham potentials have been constructed for the ground $1s^2 ^1S$ state and, in particular, for the lowest triplet $1s2s ^{3}S$ state of the helium atom, using electron densities from many-body calculations and the…

Atomic Physics · Physics 2016-08-16 I. Lindgren , S. Salomonson , F. Möller

The polarization-dependence of the exchange-correlation (XC) energy functional of periodic insulators within Kohn-Sham (KS) density-functional theory requires a ${\cal O} (1/q^2)$ divergence in the XC kernel for small vectors q. This…

Materials Science · Physics 2009-10-30 Ph. Ghosez , X. Gonze , R. W. Godby

We model a Kohn-Sham potential with a discontinuity at integer particle numbers derived from the GLLB approximation of Gritsenko et al. We evaluate the Kohn-Sham gap and the discontinuity to obtain the quasiparticle gap. This allows us to…

Materials Science · Physics 2013-05-29 M. Kuisma , J. Ojanen , J. Enkovaara , T. T. Rantala