Related papers: Multiresolution analysis for efficient, high preci…
In the exact Kohn-Sham density-functional theory (DFT), the total energy versus the number of electrons is a series of linear segments between integer points. However, commonly used approximate density functionals produce total energies…
Accurate calculations of the spectral density in a strongly correlated quantum many-body system are of fundamental importance to study its dynamics in the linear response regime. Typical examples are the calculation of inclusive and…
We train a neural network as the universal exchange-correlation functional of density-functional theory that simultaneously reproduces both the exact exchange-correlation energy and potential. This functional is extremely non-local, but…
Accurate charge densities are essential for reliable electronic structure calculations because they significantly impact predictions of various chemical properties and in particular, according to the Hellmann-Feynman theorem, atomic forces.…
We present a computationally efficient approach to perform large-scale all-electron density functional theory calculations by enriching the classical finite element basis with compactly supported atom-centered numerical basis functions that…
Density-functional theory simplifies many-electron calculations by approximating the exchange and correlation interactions with a one-electron operator that is a functional of the density. Hybrid functionals incorporate some amount of exact…
One of the major computational bottlenecks in one-body reduced density matrix (1RDM) functional theory is the evaluation of approximate 1RDM functionals and their derivatives. The reason is that more advanced approximate functionals are…
We show how to describe the coupling of electrons to non-uniform magnetic fields in the framework of the widely used norm-conserving pseudopotential appro ximation for electronic structure calculations. Our derivation applies to magnetic…
Iterative multiscale methods for electronic structure calculations offer several advantages for large-scale problems. Here we examine a nonlinear full approximation scheme (FAS) multigrid method for solving fixed potential and…
We refine the OrbNet model to accurately predict energy, forces, and other response properties for molecules using a graph neural-network architecture based on features from low-cost approximated quantum operators in the symmetry-adapted…
We have applied the Finite Element Method to the self-consistent electronic structure calculations of molecules and solids for the first time. In this approach all the calculations are performed in "real space" and the use of non-uniform…
We introduce a practical and efficient approach for calculating the all-electron full potential bandstructure in real space, employing a finite element basis. As an alternative to the k-space method, the method involves the self-consistent…
We analyze a model problem representing a multi-electronic molecule sitting on a metal surface. Working with a reduced configuration interaction Hamiltonian, we show that one can extract very accurate ground state wavefunctions as compared…
Plane-wave electronic-structure predictions based upon orbital-dependent density-functional theory (OD-DFT) approximations, such as hybrid density-functional methods and self-interaction density-functional corrections, are severely affected…
Super-resolution theory aims to estimate the discrete components lying in a continuous space that constitute a sparse signal with optimal precision. This work investigates the potential of recent super-resolution techniques for spectral…
Two electrons at the threshold of ionization represent a severe test case for electronic structure theory. A pseudospectral method yields a very accurate density of the two-electron ion with nuclear charge close to the critical value.…
We introduce a spectral density functional theory which can be used to compute energetics and spectra of real strongly--correlated materials using methods, algorithms and computer programs of the electronic structure theory of solids. The…
While there have been many developments in computational probes of both strongly-correlated molecular systems and machine-learning accelerated molecular dynamics, there remains a significant gap in capabilities in simulating accurate…
We perform a theoretical study of vacuum polarization corrections to the hyperfine structure in many-electron atoms. Calculations are performed for systems of interest for precision atomic tests of fundamental physics belonging to the…
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…