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Density functional theory (DFT) embedding provides a formally exact framework for interfacing correlated wave-function theory (WFT) methods with lower-level descriptions of electronic structure. Here, we report techniques to improve the…

Chemical Physics · Physics 2015-06-12 Jason D. Goodpaster , Taylor A. Barnes , Frederick R. Manby , Thomas F. Miller

We present a general multi-component density functional theory in which electrons and nuclei are treated completely quantum mechanically, without the use of a Born-Oppenheimer approximation. The two fundamental quantities in terms of which…

Materials Science · Physics 2007-05-23 Thomas Kreibich , Robert van Leeuwen , E. K. U. Gross

The basis-set correction method based on density-functional theory consists in correcting the energy calculated by a wave-function method with a given basis set by a density functional. This basis-set correction density functional…

Chemical Physics · Physics 2023-07-05 Diata Traore , Emmanuel Giner , Julien Toulouse

Most modern calculations of many-electron atoms use basis sets of atomic orbitals. An accurate account for the electronic correlations in heavy atoms is very difficult computational problem and optimization of the basis sets can reduce…

Atomic Physics · Physics 2024-01-17 M. G. Kozlov , Yu. A. Demidov , M. Y. Kaygorodov , E. V. Triapitsyna

It is shown for two electron atoms that ground-state wavefunctions of the form \begin{equation} \Psi(\vec{r_{1}}, \vec{r_{2}})=\phi(\vec{r_{1}})\phi(\vec{r_{2}})(\cosh ar_{1}+\cosh ar_{2})(1+0.5 r_{12}e^{-b r_{12}}) \end{equation} where…

Atomic Physics · Physics 2015-06-04 Rabeet Singh Chauhan , Manoj K. Harbola

Density functional calculations on atoms are often used for determining accurate initial guesses as well as generating various types of pseudopotential approximations and efficient atomic-orbital basis sets for polyatomic calculations. To…

Computational Physics · Physics 2023-10-30 Susi Lehtola

The description of weakly bound electronic states is especially difficult with atomic orbital basis sets. The diffuse atomic basis functions that are necessary to describe the extended electronic state generate significant linear…

Chemical Physics · Physics 2019-12-30 Susi Lehtola

Density functional theory (DFT) is an exact alternative formulation of quantum mechanics, in which it is possible to calculate the total energy, the spin and the charge density of many-electron systems in the ground state. In practice, it…

Atomic Physics · Physics 2014-03-25 Uri Argaman , Guy Makov , Eli Kraisler

Employing a local formula for the electron-electron interaction energy, we derive a self-consistent approximation for the total energy of a general $N$-electron system. Our scheme works as a local variant of the Thomas-Fermi approximation…

Chemical Physics · Physics 2013-10-31 E. Rasanen , A. Odriazola , I. Makkonen , A. Harju

All-electron calculations play an important role in density functional theory, in which improving computational efficiency is one of the most needed and challenging tasks. In the model formulations, both nonlinear eigenvalue problem and…

Computational Physics · Physics 2020-07-29 Bin Gao , Guanghui Hu , Yang Kuang , Xin Liu

First-principles density functional theory (DFT) codes which employ a localized basis offer advantages over those which use plane-wave bases, such as better scaling with system size and better suitability to low-dimensional systems. The…

Materials Science · Physics 2024-11-25 Daniel Bennett , Michele Pizzochero , Javier Junquera , Efthimios Kaxiras

The variational procedure to construct compact and accurate wave functions for three-electron atoms and ions is developed. The procedure is based on the use of six-dimensional gaussoids written in the relative four-body coordinates $r_{12},…

Atomic Physics · Physics 2011-01-11 Alexei M. Frolov , David M. Wardlaw

Coulomb interactions that occur in electronic structure calculations are correlated by allowing basis function components of the interacting densities to polarize, thereby reducing the magnitude of the interaction. Exchange integrals of…

Chemical Physics · Physics 2022-05-16 Jerry L. Whitten

The projection of the eigenfunctions obtained in standard plane-wave first-principle electronic-structure calculations into atomic-orbital basis sets is proposed as a formal and practical link between the methods based on plane waves and…

Condensed Matter · Physics 2009-10-28 Daniel Sanchez-Portal , Emilio Artacho , Jose M. Soler

The interaction between electronic and nuclear spins in the presence of external magnetic fields can be described by a spin Hamiltonian, with parameters obtained from first principles, electronic structure calculations. We describe an…

Materials Science · Physics 2019-04-10 Krishnendu Ghosh , He Ma , Vikram Gavini , Giulia Galli

We present and discuss some ideas concerning an ``average-pair-density functional theory'', in which the ground-state energy of a many-electron system is rewritten as a functional of the spherically and system-averaged pair density. These…

Materials Science · Physics 2009-11-11 Paola Gori-Giorgi , Andreas Savin

Since in periodic systems, a given element may be present in different spatial arrangements displaying vastly different physical and chemical properties, an elemental basis set that is independent of physical properties of materials may…

Chemical Physics · Physics 2021-05-04 Yanbing Zhou , Emanuel Gull , Dominika Zgid

Parameterized tight-binding models fit to first principles calculations can provide an efficient and accurate quantum mechanical method for predicting properties of molecules and solids. However, well-tested parameter sets are generally…

Materials Science · Physics 2023-04-28 Kevin F. Garrity , Kamal Choudhary

We present the first wavelet-based all-electron density-functional calculations to include gradient corrections and the first in a solid. Direct comparison shows this approach to be unique in providing systematic ``transparent''…

Materials Science · Physics 2009-11-07 I. P. Daykov , T. D. Engeness , T. A. Arias

We propose a new molecular simulation framework that combines the transferability, robustness and chemical flexibility of an ab initio method with the accuracy and efficiency of a machine learned force field. The key to achieve this mix is…

Computational Physics · Physics 2020-01-08 Sebastian Dick , Marivi Fernandez-Serra
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