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We have recently discussed an algorithm to automatically generate auxiliary basis sets (ABSs) of the standard form for density fitting (DF) or resolution-of-the-identity (RI) calculations in a given atomic orbital basis set (OBS) of any…

Computational Physics · Physics 2023-10-30 Susi Lehtola

Density fitting (DF), also known as the resolution of the identity (RI), is a widely used technique in quantum chemical calculations with various types of atomic basis sets - Gaussian-type orbitals, Slater-type orbitals, as well as…

Chemical Physics · Physics 2021-12-22 Susi Lehtola

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 this study, we present a general workflow that enables the automatic generation of auxiliary density basis sets for all elements of the periodic table (from H to Og) to facilitate the general applicability of relativistic Dirac-Kohn-Sham…

Chemical Physics · Physics 2025-06-19 Nicolo' Antonini , Enrico Ronca , Loriano Storchi , Leonardo Belpassi

We present a systematic, quasi-automated methodology for generating electronic models in the framework of second-principles density functional theory (SPDFT). This approach enables the construction of accurate and computationally efficient…

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 reports an efficient density-fitting implementation of the density-based basis-set correction (DBBSC) method in the MOLPRO software. This method consists in correcting the energy calculated by a wave-function method with a given…

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

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

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

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

Pair atomic density fitting (PADF) is a promising strategy to reduce the scaling with system size of quantum chemical methods for the calculation of the correlation energy like the direct random phase approximation (RPA) or second-order…

Chemical Physics · Physics 2023-03-14 Edoardo Spadetto , Pier Herman Theodoor Philipsen , Arno Förster , Lucas Visscher

We present low-scaling algorithms for $GW$ and constrained random phase approximation based on a symmetry-adapted interpolative separable density fitting (ISDF) procedure that incorporates the space-group symmetries of crystalline systems.…

Materials Science · Physics 2024-01-24 Chia-Nan Yeh , Miguel A. Morales

Although many programs have been published for fully numerical Hartree--Fock (HF) or density functional (DF) calculations on atoms, we are not aware of any that support hybrid DFs, which are popular within the quantum chemistry community…

Chemical Physics · Physics 2019-08-19 Susi Lehtola

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

A challenge in modeling time-dependent strong-field processes such as high-harmonic generation for many-body systems, is how to effectively represent the electronic continuum. We apply Rothe's method to the time-dependent Hartree-Fock…

Chemical Physics · Physics 2025-08-22 Simon Elias Schrader , Håkon Emil Kristiansen , Thomas Bondo Pedersen , Simen Kvaal

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

Density Functional Tight-Binding (DFTB), an approximative approach derived from Density Functional Theory (DFT), has the potential to pave the way for simulations of large periodic or non-periodic systems. We have specifically tailored DFTB…

We present an efficient implementation of periodic Gaussian density fitting (GDF) using the Coulomb metric. The three-center integrals are divided into two parts by range-separating the Coulomb kernel, with the short-range part evaluated in…

Chemical Physics · Physics 2021-04-08 Hong-Zhou Ye , Timothy C. Berkelbach

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
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