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We introduce a mixed density fitting scheme that uses both a Gaussian and a plane-wave fitting basis to accurately evaluate electron repulsion integrals in crystalline systems. We use this scheme to enable efficient all-electron Gaussian…

Chemical Physics · Physics 2017-11-22 Qiming Sun , Timothy C. Berkelbach , James D. McClain , Garnet Kin-Lic Chan

The electron density of a molecule or material has recently received major attention as a target quantity of machine-learning models. A natural choice to construct a model that yields transferable and linear-scaling predictions is to…

Chemical Physics · Physics 2022-06-29 Andrea Grisafi , Alan M. Lewis , Mariana Rossi , Michele Ceriotti

First principles calculations based on density functional theory are having an incerasing impact on our understanding of molecule-surface interactions. For example, calculations of the multi-dimensional potential energy surface have…

Materials Science · Physics 2007-05-23 O. Gulseren , D. M. Bird , S. E. Humphreys

Basis sets are a crucial but often largely overlooked choice when setting up quantum chemistry calculations. The choice of basis set can be critical in determining the accuracy and calculation time of your quantum chemistry calculations.…

A class of variational schemes for the hydrodynamic-electrodynamic model of lossless free-electron gas in a quasineutral background is developed for high-quality simulations of surface plasmon polaritons. The Lagrangian density of lossless…

Computational Physics · Physics 2019-02-27 Qiang Chen , Lifei Geng , Xiang Chen , Xiaojun Hao , Chuanchuan Wang , Xiaoyang Wang

The $GW$ approximation has been recently gaining popularity among the method for simulating molecular core-level X-ray photoemission spectra. Traditionally, $GW$ core-level binding energies have been computed using either the cc-pV$n$Z or…

Chemical Physics · Physics 2022-07-13 Daniel Mejia-Rodriguez , Alexander Kunitsa , Edoardo Aprà , Niranjan Govind

Using multiwavelets, we have obtained total energies and corresponding atomization energies for the GGA-PBE and hybrid-PBE0 density functionals for a test set of 211 molecules with an unprecedented and guaranteed $\mu$Hartree accuracy.…

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

Finite-range numerical atomic orbitals are the basis functions of choice for several first principles methods, due to their flexibility and scalability. Generating and testing such basis sets, however, remains a significant challenge for…

Chemical Physics · Physics 2013-11-12 Fabiano Corsetti , M. -V. Fernández-Serra , José M. Soler , Emilio Artacho

To perform efficient many-body calculations in the framework of the exact diagonalization of the Hamiltonian one needs an appropriately tailored Fock basis built from the single-particle orbitals. The simplest way to compose the basis is to…

Computational Physics · Physics 2019-10-22 Andrzej Chrostowski , Tomasz Sowiński

We explore the impact of optimizations of the single-particle basis on the convergence behavior and robustness of ab initio no-core shell model calculations. Our focus is on novel basis sets defined by the natural orbitals of a correlated…

Nuclear Theory · Physics 2019-03-27 Alexander Tichai , Julius Müller , Klaus Vobig , Robert Roth

Recent developments have seen the application of finite Gaussian basis sets to the $\alpha(Z\alpha)^{n\geq3}$ vacuum polarization. The energy shift for $s$ and $p$ electron states have been tabulated and their convergence investigated. In…

Atomic Physics · Physics 2026-04-28 Haisum Hayat , Harry M. Quiney

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 present a method to compute the photoionization spectra of atoms and molecules in linear response time-dependent density functional theory. The electronic orbital variations corresponding to ionized electrons are expanded on a basis set…

Computational Physics · Physics 2023-05-24 Ivan Duchemin , Antoine Levitt

Relativistic Hartree-Fock and random phase approximation methods for open shells are used to calculate ionization potentials and static scalar polarizabilities of eight superheavy elements with open $6d$-shell, which include Db, Sg, Bh, Hs,…

Atomic Physics · Physics 2016-04-06 V. A. Dzuba

Since in periodic systems, a given element may be present in different spatial arrangements displaying vastly different physical and chemical properties, an elemental basis set that is independent of physical properties of materials may…

Chemical Physics · Physics 2021-05-04 Yanbing Zhou , Emanuel Gull , Dominika Zgid

We derive a formalism, the separation method, for the efficient and accurate calculation of two-body matrix elements for a Gaussian potential in the cylindrical harmonic-oscillator basis. This formalism is of critical importance for…

Nuclear Theory · Physics 2010-11-02 W. Younes

In this work we examine critically the electronic structure of the rare-earth elements by use of the so-called Hubbard I approximation. From the theoretical side all measured features of both occupied and unoccupied states are reproduced,…

We have developed a new self-consistent scheme of generating variational basis based on the exactdiagonalization, which can be applied efficiently to various types of electron-phonon systems. This scheme is quite general and brings down the…

Strongly Correlated Electrons · Physics 2015-10-18 Monodeep Chakraborty , B. I. Min

A one-electron Schroedinger equation based on special one-electron potentials for atoms is shown to exist that produces orbitals for an arbitrary molecule that are sufficiently accurate to be used without modification to construct single-…

Chemical Physics · Physics 2022-05-16 Jerry L. Whitten