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Despite the fact that most quantum chemistry basis sets are designed for accurately modelling valence chemistry, these general-purpose basis sets continue to be widely used to model core-dependent properties. Core-specialised basis sets are…

Chemical Physics · Physics 2024-09-09 Robbie T. Ireland , Laura K. McKemmish

A simple yet general method for constructing basis sets for molecular electronic structure calculations is presented. These basis sets consist of atomic natural orbitals from a multi-configurational self-consistent field calculation…

Materials Science · Physics 2015-05-19 F. R. Petruzielo , Julien Toulouse , C. J. Umrigar

We introduce nested gausslet (NG) bases, an improvement on previous gausslet bases which can treat systems containing atoms with much larger atomic number. We also introduce pure Gaussian distorted gausslet bases, which allow the…

Chemical Physics · Physics 2023-09-20 Steven R. White , Michael J. Lindsey

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

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 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

This work presents new Gaussian single- and double-zeta basis sets optimized for stochastic density functional theory (sDFT) using real-space auxiliary grids. Previous studies showed standard basis sets like STO-3G and 6-31G are sub-optimal…

Chemical Physics · Physics 2025-04-25 Marcel David Fabian , Eran Rabani , Roi Baer

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

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

We introduce hybrid gausslet/Gaussian basis sets, where a standard Gaussian basis is added to a gausslet basis in order to increase accuracy near the nuclei while keeping the spacing of the grid of gausslets relatively large. The Gaussians…

Chemical Physics · Physics 2024-06-19 Yiheng Qiu , Steven R. White

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

Simulating solids with quantum chemistry methods and Gaussian-type orbitals (GTOs) has been gaining popularity. Nonetheless, there are few systematic studies that assess the basis set incompleteness error (BSIE) in these GTO-based…

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

A novel Gaussian-Sinc mixed basis set for the calculation of the one-electron electronic structure within a uniform magnetic field in three dimensions is presented. The one-electron system is used to demonstrate the utility of this new…

Computational Physics · Physics 2014-11-12 Jonathan L. Jerke , Young Lee , C. J. Tymczak

For accurate ab initio description of Rydberg excited states the study suggests generating the appropriate diffuse basis functions by a cheap variational optimization of virtual orbitals of the corresponding ion core. By following this…

Chemical Physics · Physics 2023-08-16 Jan Šmydke

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

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

A basis set of generalized nonspherical Gaussian functions (GGTOs) is presented and discussed. As a first example we report on Born-Oppenheimer energies of the hydrogen molecule. Although accurate results have been obtained, we conclude…

Chemical Physics · Physics 2009-10-31 T. Detmer , P. Schmelcher , L. S. Cederbaum

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

Gausslets are one of the few examples of basis sets for electronic structure which allow for two-index/diagonal electron-electron interaction terms. A weakness of gausslets is that, because of their 1D origin, they have been tied to…

Chemical Physics · Physics 2026-04-09 Steven R. White
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