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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

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

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

We present a new kind of basis function for discretizing the Schr\"odinger equation in electronic structure calculations, called a gausslet, which has wavelet-like features but is composed of a sum of Gaussians. Gausslets are placed on a…

Chemical Physics · Physics 2018-01-17 Steven R. White

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

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 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

A general procedure for the optimization of atomic density-fitting basis functions is designed with the balance between accuracy and numerical stability in mind. Given one-electron wavefunctions and energies, weights are assigned to the…

Chemical Physics · Physics 2020-10-13 Dimitri N. Laikov

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

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 present a new adaptive method for electronic structure calculations based on novel fast algorithms for reduction of multivariate mixtures. In our calculations, spatial orbitals are maintained as Gaussian mixtures whose terms are selected…

Numerical Analysis · Mathematics 2019-06-19 Gregory Beylkin , Lucas Monzon , Xinshuo Yang

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

Coulomb integrals, i.e., matrix elements of bare or screened Coulomb interaction between one-electron orbitals, are fundamental objects in many approaches developed to tackle the challenging problem of calculating the electronic structure…

Strongly Correlated Electrons · Physics 2023-06-21 Coraline Letouzé , Guillaume Radtke , Benjamin Lenz , Christian Brouder

A precise understanding of mechanisms governing the dynamics of electrons in atoms and molecules subjected to intense laser fields has a key importance for the description of attosecond processes such as the high-harmonic generation and…

The first discussion of basis sets consisting of exponentially decaying Coulomb Sturmian functions for modelling electronic structures is presented. The proposed basis set construction selects Coulomb Sturmian functions using separate upper…

Chemical Physics · Physics 2019-01-23 Michael F. Herbst , James Emil Avery , Andreas Dreuw

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

There are many ways to numerically represent of chemical systems in order to compute their electronic structure. Basis functions may be localized in real-space (atomic orbitals), in momentum-space (plane waves), or in both components of…

Chemical Physics · Physics 2019-09-09 James Brown , James D. Whitfield

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 a new basis function (the spherical gaussian) for electronic structure calculations on spheres of any dimension $D$. We find \alert{general} expressions for the one- and two-electron integrals and propose an efficient…

Chemical Physics · Physics 2015-06-09 Peter M. W. Gill , Pierre-François Loos , Davids Agboola

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
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