Related papers: Accurate Anisotropic Gaussian Type Orbital Basis S…
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…
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…
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…
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…
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…
We propose a unique scheme to construct fully optimized atomic basis sets for density-functional calculations. The shapes of the radial functions are optimized by minimizing the {\it spillage} of the wave functions between the atomic…
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…
We present an approach for augmenting Gaussian atomic orbitals with correct nuclear cusps. Like the atomic orbital basis set itself, and unlike previous cusp corrections, this approach is independent of the many-body method used to prepare…
Most modern calculations of many-electron atoms use basis sets of atomic orbitals. An accurate account for the electronic correlations in heavy atoms is very difficult computational problem and optimization of the basis sets can reduce…
Atomic orbitals underpin our understanding of electronic structure, providing intuitive descriptions of bonding, charge transfer, magnetism, and correlation effects. Despite their utility, an atomic basis that is adaptable, strictly…
Basis sets of atomic orbitals are very efficient for density functional calculations but lack a systematic variational convergence. We present a variational method to optimize numerical atomic orbitals using a single parameter to control…
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…
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…
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…
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…
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…
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…
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…
Choosing a basis set is the first step of a quantum chemistry calculation and it sets its maximum accuracy. This choice of orbitals is limited by strong technical constraints as one must be able to compute a large number of six dimensional…
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…