Related papers: A new parametrizable model of molecular electronic…

A framework for developing new approximate electronic structure methods is presented, in which the correlation energy of a many-electron system in the ground state is computed as in the single-reference second-order many-body perturbation…

The symmetry-projected Hartree--Fock ansatz for the electronic structure problem can efficiently account for static correlation in molecules, yet it is often unable to describe dynamic correlation in a balanced manner. Here, we consider a…

For the Hirshfeld-I atom-in-molecule model, associated single-atom energies and interaction energies at the Hartree-Fock level are determined efficiently in one-electron Hilbert space. In contrast to most other approaches, the energy terms…

Atomic effective one-electron potentials in a compact analytic form in terms of a few Gaussian charge distributions are developed, for Hydrogen through Nobelium, for starting molecular electronic structure calculations by a simple…

We introduce an energy functional for ground-state electronic structure calculations. Its variables are the natural spin-orbitals of singlet many-body wave functions and their joint occupation probabilities deriving from controlled…

This chapter discusses contemporary quantum chemical methods and provides general insights into modern electronic structure theory with a focus on heavy-element-containing compounds. We first give a short overview of relativistic…

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…

We have investigated structure and properties of small metal clusters using all-electron ab initio theoretical methods based on the Hartree-Fock approximation and density functional theory, perturbation theory and compared results of our…

Ab initio electronic structure methods give accurate results for small systems, but do not scale well to large systems. Chemical insight tells us that molecular functional groups will behave approximately the same way in all molecules,…

This article is an introduction to a new approach to first principles electronic structure calculation. The starting point is the Hartree-Fock-Roothaan equation, in which molecular integrals are approximated by polynomials by way of Taylor…

We derive and implement symmetry-projected Hartree-Fock-Bogoliubov (HFB) equations and apply them to the molecular electronic structure problem. All symmetries (particle number, spin, spatial, and complex conjugation) are deliberately…

To leverage the redundancy between the electronic structure computed at each step of first-principles molecular dynamics, we present a data-driven modeling framework for Kohn-Sham Density Functional Theory that bypasses the explicit…

Machine learning is rapidly accelerating materials and chemical discovery, but most current models target energies, forces, or selected molecular properties rather than the underlying many-body electronic structure. Learning…

In this article, we set up a functional setting for mean-field electronic structure models of Hartree-Fock or Kohn-Sham types for disordered crystals. The electrons are quantum particles and the nuclei are classical point-like articles…

Donor-based quantum devices in silicon are attractive platforms for universal quantum computing and analog quantum simulations. The nearly-atomic precision in dopant placement promises great control over the quantum properties of these…

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…

Two of the most widely used electronic structure theory methods, namely Hartree-Fock and Kohn-Sham density functional theory, both requires the iterative solution of a set of Schr\"odinger-like equations. The speed of convergence of such…

Electronic structure methods for accurate calculation of molecular properties have a high cost that grows steeply with the problem size, therefore, it is helpful to have the underlying atomic basis functions that are less in number but of…

We introduce a novel energy functional for ground-state electronic-structure calculations. Its fundamental variables are the natural spin-orbitals of the implied singlet many-body wave function and their joint occupation probabilities. The…

A fully analytical approximation for the observable characteristics of many-electron atoms is developed via a complete and orthonormal hydrogen-like basis with a single-effective charge parameter for all electrons of a given atom. The basis…