Related papers: Systematically improvable optimized atomic basis s…
We present a detailed study of the use of localized spherical-wave basis sets, first introduced in the context of linear-scaling, in first-principles density-functional calculations. Several parameters that control the completeness of this…
The well-known spatial integration schemes in molecular electronic structure theory, immune to cusps and point singularities of some kind at atomic positions, use a set of weighting functions to split the integrand into a sum of…
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…
We present a first-principles computer code package (ABACUS) that is based on density functional theory and numerical atomic basis sets. Theoretical foundations and numerical techniques used in the code are described, with focus on the…
First-principles density functional theory (DFT) codes which employ a localized basis offer advantages over those which use plane-wave bases, such as better scaling with system size and better suitability to low-dimensional systems. The…
We reexamine the recently introduced basis-set correction theory based on density-functional theory consisting in correcting the basis-set incompleteness error of wave-function methods using a density functional. We use a one-dimensional…
We propose a general method for constructing system-dependent basis functions for correlated quantum chemical calculations. Our construction combines features from several traditional approaches: plane waves, localized basis functions, and…
In this contribution, we employ a density matrix based optimization procedure to obtain customized basis functions to describe chains of rotating water molecules in interaction regimes associated with different intermolecular distances.…
In this paper, we propose a parallel optimization method for electronic structure calculations based on a single orbital-updating approximation. It is shown by our numerical experiments that the method is efficient and reliable for atomic…
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…
A mixed basis approach based on density functional theory is employed for low dimensional systems. The basis functions are taken to be plane waves for the periodic direction multiplied by B-spline polynomials in the non-periodic direction.…
An efficient method for calculating the electronic structure of systems that need a very fine sampling of the Brillouin zone is presented. The method is based on the variational optimization of a "single" (i.e. common to all points in the…
The paper proposes a method to obtain the optimal basis set for solving the self consistent field (SCF) equations for large atomic systems in order to calculate the energy barriers in tunneling structures, with higher accuracy and speed.…
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…
We present a method to discretize the Kohn-Sham Hamiltonian matrix in the pseudopotential framework by a small set of basis functions automatically contracted from a uniform basis set such as planewaves. Each basis function is localized…
In this paper, we propose a computational framework for the optimal design of broadband absorbing materials composed of plasmonic nanoparticle arrays. This design problem poses several key challenges: (1) the complex multi-particle…
Recent developments in fully numerical methods promise interesting opportunities for new, compact atomic orbital (AO) basis sets that maximize the overlap to fully numerical reference wave functions, following the pioneering work of…
The reduced basis method is used to construct a "universal" basis of Dirac orbitals that may be applicable throughout the nuclear chart to calibrate covariant energy density functionals. Relative to our earlier work using the…
The description of weakly bound electronic states is especially difficult with atomic orbital basis sets. The diffuse atomic basis functions that are necessary to describe the extended electronic state generate significant linear…
In density functional theory, charge density is the core attribute of atomic systems from which all chemical properties can be derived. Machine learning methods are promising in significantly accelerating charge density prediction, yet…