Related papers: Systematically improvable optimized atomic basis s…
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…
In the framework of a recently reported linear-scaling method for density-functional-pseudopotential calculations, we investigate the use of localized basis functions for such work. We propose a basis set in which each local orbital is…
We introduce a method for solving a self consistent electronic calculation within localized atomic orbitals, that allows us to converge to the complete basis set (CBS) limit in a stable, controlled, and systematic way. We compare our…
Leveraging ab initio data at scale has enabled the development of machine learning models capable of extremely accurate and fast molecular property prediction. A central paradigm of many previous works focuses on generating predictions for…
We propose a method for obtaining effective lifetimes of scattering electronic states for avoiding the artificially confinement of the wave function due to the use of incomplete basis sets in time-dependent electronic-structure calculations…
We present a systematic study of the performance of numerical pseudo-atomic orbital basis sets in the calculation of dielectric matrices of extended systems using the self-consistent Sternheimer approach of [F. Giustino et al., Phys. Rev. B…
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…
Computational studies of chemical reactions in complex environments such as proteins, nanostructures, or on surfaces require accurate and efficient atomistic models applicable to the nanometer scale. In general, an accurate parametrization…
We present an implementation of localized atomic orbital basis sets in the projector augmented wave (PAW) formalism within the density functional theory (DFT). The implementation in the real-space GPAW code provides a complementary basis…
We present a classically solvable model that leads to optimized low-depth quantum circuits leveraging separable pair approximations. The obtained circuits are well suited as a baseline circuit for emerging quantum hardware and can, in the…
A mixed basis approach based on density functional theory is extended to one-dimensional(1D) systems. The basis functions here are taken to be the localized B-splines for the two finite non-periodic dimensions and the plane waves for the…
Variational wave function ansatze are an invaluable tool to study the properties of strongly correlated systems. We propose such a wave function, based on the theory of auxiliary fields and combining aspects of auxiliary-field quantum Monte…
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…
A widely used strategy to reduce the computational cost in quantum-chemical calculations is to partition the system into an active subsystem, which is the focus of the computational efforts and an environment that is treated at a lower…
The implementation of the orbital minimization method (OMM) for solving the self-consistent Kohn-Sham (KS) problem for electronic structure calculations in a basis of non-orthogonal numerical atomic orbitals of finite-range is reported. We…
In recent years, "composite" density-functional-theory-based methods comprising specially optimized combinations of functionals, basis sets, and empirical corrections have become widely used owing to their robustness and computational…
A new scheme for constructing approximate effective electron potentials within density-functional theory is proposed. The scheme consists of calculating the effective potential for a series of reference systems, and then using these…
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…
This study presents a novel optimisation technique for atomic structure calculations using the Flexible Atomic Code, focussing on complex multielectron systems relevant to $r$-process nucleosynthesis and kilonova modelling. We introduce a…
Ab initio calculations face the challenge of describing a complex multiscale quantum many-body system. The nuclear wave function has both strong short-range correlations and long-range contributions. Natural orbitals provide a means of…