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The performance of basis sets made of numerical atomic orbitals is explored in density-functional calculations of solids and molecules. With the aim of optimizing basis quality while maintaining strict localization of the orbitals, as…

Materials Science · Physics 2009-11-07 Javier Junquera , Oscar Paz , Daniel Sanchez-Portal , Emilio Artacho

Basis sets of atomic orbitals are very efficient for density functional calculations but lack a systematic variational convergence. We present a variational method to optimize numerical atomic orbitals using a single parameter to control…

Condensed Matter · Physics 2009-11-07 E. Anglada , J. Soler , J. Junquera , E. Artacho

We propose a unique scheme to construct fully optimized atomic basis sets for density-functional calculations. The shapes of the radial functions are optimized by minimizing the {\it spillage} of the wave functions between the atomic…

Materials Science · Physics 2015-05-19 Mohan Chen , G-C Guo , Lixin He

We determine and compare structural, dynamical, and electronic properties of liquid water at near ambient conditions through density-functional molecular dynamics simulations, when using either plane-wave or atomic-orbital basis sets. In…

Chemical Physics · Physics 2016-09-26 Giacomo Miceli , Jürg Hutter , Alfredo Pasquarello

Calculating dipole moments with high-order basis sets is generally only possible for the light molecules, such as water. A simple, yet highly effective strategy of obtaining high-order dipoles with small, computationally less expensive…

Chemical Physics · Physics 2020-01-14 Eamon K. Conway , Iouli E. Gordon , Oleg L. Polyansky , Jonathan Tennyson

Water structure, measured by the height of the first peak in oxygen-oxygen radial distributions, is converged with respect to plane-wave basis energy cutoffs for ab initio molecular dynamics simulations, confirming the reliability of…

Statistical Mechanics · Physics 2019-03-27 Susan B. Rempe , Thomas R. Mattsson , Kevin Leung

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

Electronic structure methods for accurate calculation of molecular properties have a high cost that grows steeply with the problem size, therefore, it is helpful to have the underlying atomic basis functions that are less in number but of…

Chemical Physics · Physics 2019-03-15 Dimitri N. Laikov

In this contribution, we employ a density matrix based optimization procedure to obtain customized basis functions to describe chains of rotating water molecules in interaction regimes associated with different intermolecular distances.…

Chemical Physics · Physics 2023-06-14 Tobias Serwatka , Pierre-Nicholas Roy

The input of almost every machine learning algorithm targeting the properties of matter at the atomic scale involves a transformation of the list of Cartesian atomic coordinates into a more symmetric representation. Many of the most popular…

Machine Learning · Statistics 2022-01-11 Alexander Goscinski , Félix Musil , Sergey Pozdnyakov , Michele Ceriotti

Molecule-optimized basis sets, based on approximate natural orbitals, are developed for accelerating the convergence of quantum calculations with strongly correlated (multi-referenced) electrons. We use a low-cost approximate solution of…

Chemical Physics · Physics 2014-02-12 Gergely Gidofalvi , David A. Mazziotti

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

We present an approach for generating local numerical basis sets of improving accuracy for first-principles nanoplasmonics simulations within time-dependent density functional theory. The method is demonstrated for copper, silver, and gold…

Materials Science · Physics 2015-09-04 Tuomas P. Rossi , Susi Lehtola , Arto Sakko , Martti J. Puska , Risto M. Nieminen

We study orbit-finite systems of linear equations, in the setting of sets with atoms. Our principal contribution is a decision procedure for solvability of such systems. The procedure works for every field (and even commutative ring) under…

Computation and Language · Computer Science 2024-02-28 Arka Ghosh , Piotr Hofman , Sławomir Lasota

We present a systematic study of the performance of numerical pseudo-atomic orbital basis sets in the calculation of dielectric matrices of extended systems using the self-consistent Sternheimer approach of [F. Giustino et al., Phys. Rev. B…

Materials Science · Physics 2015-06-04 Hannes Hübener , Miguel A. Pérez-Osorio , Pablo Ordejón , Feliciano Giustino

Atomic basis sets are widely employed within quantum mechanics based simulations of matter. We introduce a machine learning model that adapts the basis set to the local chemical environment of each atom, prior to the start of self…

Chemical Physics · Physics 2024-04-29 Danish Khan , Maximilian L. Ach , O. Anatole von Lilienfeld

Relativistic quintuple-zeta basis sets for the p elements are presented. The basis sets for the occupied spinors were optimized at the Dirac-Coulomb self-consistent field (SCF) level on the ground configurations. Valence and core…

A complete discrete set of spherical single-particle wave functions for studies of weakly-bound many-body systems is proposed. The new basis is obtained by means of a local-scale point transformation of the spherical harmonic oscillator…

Nuclear Theory · Physics 2008-11-26 M. V. Stoitsov , W. Nazarewicz , S. Pittel

We propose a system-oriented basis-set design based on even-tempered basis functions to variationally encode electronic ground-state information into molecular orbitals. First, we introduce a reduced formalism of concentric even-tempered…

Chemical Physics · Physics 2026-02-23 Weishi Wang , Casey Dowdle , James D. Whitfield

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
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