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Exact density functionals for the exchange and correlation energies are approximated in practical calculations for the ground-state electronic structure of a many-electron system. An important exact constraint for the construction of…

In the density functional (DF) theory of Kohn and Sham, the kinetic energy of the ground state of a system of noninteracting electrons in a general external field is calculated using a set of orbitals. Orbital free methods attempt to…

Strongly Correlated Electrons · Physics 2009-11-13 Jeng-Da Chai , John D Weeks

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

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 train a neural network as the universal exchange-correlation functional of density-functional theory that simultaneously reproduces both the exact exchange-correlation energy and potential. This functional is extremely non-local, but…

Computational Physics · Physics 2019-10-10 Jonathan Schmidt , Carlos L. Benavides-Riveros , Miguel A. L. Marques

The conventional approaches to the inverse density functional theory problem typically assume non-degeneracy of the Kohn-Sham (KS) eigenvalues, greatly hindering their use in open-shell systems. We present a generalization of the inverse…

Chemical Physics · Physics 2024-01-09 Bikash Kanungo , Jeffrey Hatch , Paul M. Zimmerman , Vikram Gavini

We develop a method that can constrain any local exchange-correlation potential to preserve ba-sic exact conditions. Using the method of Lagrange multipliers, we calculate for each set of given Kohn-Sham orbitals, a constraint-preserving…

Strongly Correlated Electrons · Physics 2009-05-11 Yair Kurzweil Martin Head-Gordon

It is known that the asymptotic decay of the electron density $n(\br)$ outside a molecule is informative about its first ionization potential $I_0$, $n(|\br|\to\infty) \sim \text{exp}(-2\sqrt{2I_0}\,r)$. This dictates the orbital energy of…

Chemical Physics · Physics 2015-12-31 P. Gori-Giorgi , T. Gál , E. J. Baerends

Ensemble density functional theory extends the usual Kohn-Sham machinery to quantum state ensembles involving ground- and excited states. Recent work by the authors [Phys. Rev. Lett. 119, 243001 (2017); 123, 016401 (2019)] has shown that…

Strongly Correlated Electrons · Physics 2020-01-28 Tim Gould , Stefano Pittalis

We propose a new generalised Kohn-Sham or constrained hybrid method, where the exchange potential is the (equally weighted) average of the nonlocal Fock exchange term and the self-interaction-corrected exchange potential, as obtained from…

Chemical Physics · Physics 2022-01-05 Thomas C. Pitts , Nektarios N. Lathiotakis , Nikitas I. Gidopoulos

One of the most powerful strategies to address properties of real many-body systems is to incorporate data obtained for models, for example, to use data of the homogeneous electron gas in order to build the Local Density Approximation for…

Materials Science · Physics 2026-05-05 Muhammed Hüseyin Güneş , Ayoub Aouina , Vitaly Gorelov , Matteo Gatti , Lucia Reining

In this work, we have used the exchange-only optimized effective potential in the self-consistent calculations of the density functional Kohn-Sham equations for simple metal clusters in stabilized jellium model with self-compression. The…

Atomic and Molecular Clusters · Physics 2009-11-11 M. Payami

A Kohn-Sham (KS) inversion determines a KS potential and orbitals corresponding to a given electron density, a procedure that has applications in developing and evaluating functionals used in density functional theory. Despite the utility…

Computational Physics · Physics 2021-04-07 Seungsoo Nam , Ryan J. McCarty , Hansol Park , Eunji Sim

Physically valid and numerically efficient approximations for the exchange and correlation energy are critical for reduced density-matrix functional theory to become a widely used method in electronic structure calculations. Here we examine…

Strongly Correlated Electrons · Physics 2016-03-23 A. Putaja , F. G. Eich , T. Baldsiefen , E. Rasanen

In this work we describe a model for the exchange interaction of electrons, as it follows from the Pauli exclusion principle. Starting from Hartree-Fock theory and making use of the free electron-gas model we propose a simple scheme to…

Materials Science · Physics 2025-06-11 G. Schiwietz , P. L. Grande

Using an end-to-end differentiable implementation of the Kohn-Sham self-consistent field equations, we obtain an accurate neural network-based exchange and correlation (XC) functional of the electronic density. The functional is optimized…

Chemical Physics · Physics 2021-06-09 Sebastian Dick , Marivi Fernandez-Serra

We identify peak and valley structures in the exact exchange-correlation potential of time-dependent density functional theory that are crucial for time-resolved electron scattering in a model one-dimensional system. These structures are…

Chemical Physics · Physics 2018-01-03 Yasumitsu Suzuki , Lionel Lacombe , Kazuyuki Watanabe , Neepa T. Maitra

The behavior of the surface barrier that forms at the metal-vacuum interface is important for several fields of surface science. Within the Density Functional Theory framework, this surface barrier has two non-trivial components: exchange…

Other Condensed Matter · Physics 2009-11-11 C. M. Horowitz , C. R. Proetto , S. Rigamonti

Kohn-Sham density functional theory (DFT) has long struggled with the accurate description of strongly correlated and open shell systems and improvements have been minor even in the newest hybrid functionals. In this Letter we treat the…

Chemical Physics · Physics 2021-04-01 Danny Gibney , Jan-Niklas Boyn , David A. Mazziotti

Exchange-correlation potentials vxc and energy densities exc are derived for integer and fractional electron counts using an orbital-averaged Kohn-Sham inversion procedure. The reference densities for inversion come from full configuration…

Chemical Physics · Physics 2025-04-30 Vaibhav Khanna , Bikash Kanungo , Jeffrey Hatch , Joshua Kammeraad , Paul M. Zimmerman
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