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Molecular calculations in quantum Monte Carlo frequently employ a mixed basis consisting of contracted and primitive Gaussian functions. While standard basis sets of varying size and accuracy are available in the literature, we demonstrate…

Chemical Physics · Physics 2015-05-14 F. R. Petruzielo , Julien Toulouse , C. J. Umrigar

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

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

We introduce highly local basis sets for electronic structure which are very efficient for correlation calculations near the complete basis set limit. Our approach is based on gausslets, recently introduced wavelet-like smooth orthogonal…

Chemical Physics · Physics 2019-02-20 Steven R. White , E. Miles Stoudenmire

Gausslets are one of the few basis constructions for electronic structure that combine locality, orthonormality, variable resolution, and an accurate diagonal approximation for the electron-electron interaction, but the original…

Chemical Physics · Physics 2026-05-07 Steven R. White

The rapidly growing interest in simulating condensed-phase materials using quantum chemistry methods calls for a library of high-quality Gaussian basis sets suitable for periodic calculations. Unfortunately, most standard Gaussian basis…

Chemical Physics · Physics 2022-06-07 Hong-Zhou Ye , Timothy C. Berkelbach

In high magnetic field calculations, anisotropic Gaussian type orbital (AGTO) basis functions are capable of reconciling the competing demands of the spherically symmetric Coulombic interaction and cylindrical magnetic ($B$ field)…

Computational Physics · Physics 2018-01-17 Wuming Zhu , S. B. Trickey

We introduce an efficient method to construct optimal and system adaptive basis sets for use in electronic structure and quantum Monte Carlo calculations. The method is based on an embedding scheme in which a reference atom is singled out…

Strongly Correlated Electrons · Physics 2016-02-02 Sandro Sorella , Nicolas Devaux , Mario Dagrada , Guglielmo Mazzola , Michele Casula

We present a general methodology to evaluate matrix elements of the effective core potentials (ECPs) within one-electron basis set of Slater-type orbitals (STOs). The scheme is based on translation of individual STO distributions in the…

Chemical Physics · Physics 2017-05-17 Michal Lesiuk , Aleksandra M. Tucholska , Robert Moszynski

We describe a method for imposing the correct electron-nucleus (e-n) cusp in molecular orbitals expanded as a linear combination of (cuspless) Gaussian basis functions. Enforcing the e-n cusp in trial wave functions is an important asset in…

Chemical Physics · Physics 2020-06-05 Pierre-François Loos , Anthony Scemama , Michel Caffarel

We investigate the use of optimized correlation consistent gaussian basis sets for the study of insulating solids with auxiliary-field quantum Monte Carlo (AFQMC). The exponents of the basis set are optimized through the minimization of the…

Chemical Physics · Physics 2021-02-03 Miguel A. Morales , Fionn D. Malone

We demonstrate that basis sets suitable for electronic structure calculations can be obtained from simple accuracy considerations for the hydrogenic one-electron ions $Y^{(Y-1)+}$ for $Y\in[1,Z]$, necessitating no self-consistent field…

Computational Physics · Physics 2020-04-06 Susi Lehtola

Electronic structure calculations are mostly carried out with Coulomb potential singularity adapted basis sets like STO or contracted GTO. With other basis or for heavy elements the pseudopotentials may appear as a practical alternative.…

Chemical Physics · Physics 2022-11-14 Tommi Höynälänmaa , Tapio Rantala

An efficient method for calculating the electronic structure of systems that need a very fine sampling of the Brillouin zone is presented. The method is based on the variational optimization of a "single" (i.e. common to all points in the…

Materials Science · Physics 2009-10-31 Sandro Scandolo , Jorge Kohanoff

The Slater-type orbital basis with non-integer principal quantum numbers is a physically and mathematically motivated choice for molecular electronic structure calculations in both non-relativistic and relativistic theory. The…

Quantum Physics · Physics 2022-03-15 A Bagci , Philip E Hoggan , M Adak

Strong magnetic fields such as those found on white dwarfs have significant effects on the electronic structure of atoms and molecules. However, the vast majority of molecular studies in the literature in such fields are carried out with…

Chemical Physics · Physics 2025-02-07 Hugo Åström , Susi Lehtola

Electronic structure calculations on small systems such as H$_2$, H$_2$O, LiH, and BeH$_2$ with chemical accuracy are still a challenge for the current generation of the noisy intermediate-scale quantum (NISQ) devices. One of the reasons is…

Chemical Physics · Physics 2022-11-15 Hyuk-Yong Kwon , Gregory M. Curtin , Zachary Morrow , C. T. Kelley , Elena Jakubikova

We introduce a family of all-electron Gaussian basis sets, augmented MOLOPT, optimized for excited-state calculations on large molecules. We generate these basis sets by augmenting existing STO-3G, STO-6G, and MOLOPT basis sets optimized…

Chemical Physics · Physics 2025-12-15 Rémi Pasquier , Maximilian Graml , Jan Wilhelm

We present model-assisted density fitting (MADF) basis set generator, an algorithm for generating primitive atomic Gaussian density fitting (DF) basis sets (DFBSs) from a contracted Gaussian orbital basis set (OBS). The MADF algorithm…

Chemical Physics · Physics 2025-10-14 Kshitijkumar A. Surjuse , Edward F. Valeev

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
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