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We present an efficient and accurate implementation of hybrid exchange-correlation (XC) functionals in the SIESTA code, enabling large-scale simulations based on Hartree-Fock-type exact exchange combined with strictly localized numerical…

We develop an efficient approach to evaluate range-separated exact exchange for grid or plane-wave based representations within the Generalized Kohn-Sham DFT (GKS-DFT) framework. The Coulomb kernel is fragmented in reciprocal space, and we…

Chemical Physics · Physics 2023-09-11 Nadine C. Bradbury , Tucker Allen , Minh Nguyen , Daniel Neuhauser

A new, very fast, implementation of the exact (Fock) exchange operator for electronic structure calculations within the plane-wave pseudopotential method is described in detail for both molecular and periodic systems, and carefully…

Materials Science · Physics 2018-12-12 Ivan Carnimeo , Stefano Baroni , Paolo Giannozzi

Calculating highly accurate thermochemical properties of condensed matter via wave function-based approaches (such as e.g. Hartree-Fock or hybrid functionals) has recently attracted much interest. We here present two strategies providing…

A recently developed finite element approach for fully numerical atomic structure calculations [S. Lehtola, Int. J. Quantum Chem. 119, e25945 (2019)] is extended to the description of atoms with spherically symmetric densities via…

Computational Physics · Physics 2020-01-30 Susi Lehtola

We estimate the prediction sensitivity with respect to Hartree-Fock exchange in approximate density functionals for representative Fe(II) and Fe(III) octahedral complexes. Based on the observation that the range of parameters spanned by the…

Materials Science · Physics 2015-07-16 Efthymios I. Ioannidis , Heather J. Kulik

We compare two different approaches to investigations of many-electron systems. The first is the Hartree-Fock (HF) method and the second is the Density Functional Theory (DFT). Overview of the main features and peculiar properties of the HF…

Materials Science · Physics 2009-11-07 M. Ya. Amusia , A. Z. Msezane , V. R. Shaginyan

Within the finite-field Kohn-Sham framework, static electric response properties of diatomic molecules are presented. The electronic energy, dipole moment ({\boldmath$\mu$}), static dipole polarizability ({\boldmath$\alpha$}) and…

Chemical Physics · Physics 2019-04-26 Abhisek Ghosal , Tanmay Mandal , Amlan K. ~Roy

A detailed convex analysis-based formulation of density-functional theory for periodic systems in arbitrary dimensions is presented. The electron-electron interaction is taken to be of Yukawa type, harmonising with underlying function…

Chemical Physics · Physics 2026-02-23 Oliver M. Bohle , Maryam Lotfigolian , Andre Laestadius , Erik I. Tellgren

The crystalline structure of ground-state orthorhombic SrRuO$_3$ is reproduced by applying hybrid density functional theory scheme to the functionals based on the revised generalized-gradient approximations for solid-state calculations. The…

Materials Science · Physics 2016-10-11 Š. Masys , V. Jonauskas

The high cost associated with the evaluation of Hartree-Fock exchange (HFX) makes hybrid functionals computationally challenging for large systems. In this work, we present an efficient way to accelerate HFX calculations with numerical…

Computational Physics · Physics 2020-09-09 Xinming Qin , Jie Liu , Wei Hu , Jinlong Yang

We model the Hartree-exchange-correlation potential of Kohn-Sham density-functional theory adopting a novel strategy inspired by the strictly-correlated-electrons limit and relying on the exact decomposition of the potential based on the…

Chemical Physics · Physics 2024-09-09 Sara Giarrusso , Federica Agostini

A translationally invariant formulation of the Hartree-Fock (HF) $\Gamma$-point approximation is presented. This formulation is achieved through introduction of the Minimum Image Convention (MIC) at the level of primitive two-electron…

Materials Science · Physics 2016-08-16 C. J. Tymczak , Valéry T. Weber , Eric Schwegler , Matt Challacombe

We present a fully numerical framework for the optimization of molecule-specific quantum chemical basis functions within the quantics tensor train format using a finite-difference scheme. The optimization is driven by solving the…

Chemical Physics · Physics 2025-06-12 Paul Haubenwallner , Matthias Heller

The isostructural {\alpha}-{\gamma} phase transition in cerium is analyzed using density-functional theory with different exchange-correlation functionals, in particular the PBE0 hybrid functional and the exact- exchange plus correlation in…

Strongly Correlated Electrons · Physics 2015-06-11 Marco Casadei , Xinguo Ren , Patrick Rinke , Angel Rubio , Matthias Scheffler

We evaluate the accuracy of electron densities and quasiparticle energy gaps given by hybrid functionals by directly comparing these to the exact quantities obtained from solving the many-electron Schrodinger equation. We determine the…

Materials Science · Physics 2021-01-15 A. R. Elmaslmane , Jack Wetherell , M. J. P. Hodgson , K. P. McKenna , R. W. Godby

In this article we present an algorithm to efficiently evaluate the exchange matrix in periodic systems when Gaussian basis set with pseudopotentials are used. The usual algorithm for evaluating exchange matrix scales cubically with the…

Strongly Correlated Electrons · Physics 2022-11-11 Sandeep Sharma , Alec F. White , Gregory Beylkin

We develop a new method of implementing the Hartree-Fock calculations. A class of Gaussian bases is assumed, which includes the Kamimura-Gauss basis-set as well as the set equivalent to the harmonic-oscillator basis-set. By using the…

Nuclear Theory · Physics 2011-07-19 H. Nakada , M. Sato

Self-interaction is a fundamental flaw of practical Kohn-Sham Density Functional Theory (KS DFT) approximations responsible for numerous qualitative and even catastrophic shortcomings. Whereas self-interaction is easy to characterize in…

Chemical Physics · Physics 2024-07-16 Samuel A. Slattery , Edward F. Valeev

In this article, we derive fully guaranteed error bounds for the energy of convex nonlinear mean-field models. These results apply in particular to Kohn-Sham equations with convex density functionals, which includes the reduced Hartree-Fock…