Related papers: Predicting the Charge Density Response in Metal El…
We examine the density-functional theory of macroscopic insulators, obtained in the large-cluster limit or under periodic boundary conditions. For polar crystals, we find that the two procedures are not equivalent. In a large-cluster case,…
Non-adiabaticity in adsorption on metal surfaces gives rise to a number of measurable effects, such as chemicurrents and exo-electron emission. Here we present a quantitative theory of chemicurrents on the basis of ground-state…
The Gordian knot of density-functional theories for classical molecular liquids remains finding an accurate free-energy functional in terms of the densities of the atomic sites of the molecules. Following Kohn and Sham, we show how to solve…
Within exact electron density-functional theory, we investigate Kohn-Sham (KS) potentials, orbital energies, and non-interacting kinetic energies of the fractional ions of Li, C and F. We use quantum Monte Carlo densities as input, which…
Machine learning (ML) techniques have rapidly found applications in many domains of materials chemistry and physics where large data sets are available. Aiming to accelerate the discovery of materials for battery applications, in this work,…
This work explores the use of joint density-functional theory, a new form of density-functional theory for the ab initio description of electronic systems in thermodynamic equilibrium with a liquid environment, to describe electrochemical…
We describe a rapidly converging algorithm for solving the Kohn--Sham equations and equations of similar structure that appear frequently in calculations of the structure of inhomogeneous electronic many--body systems. The algorithm has its…
Machine-learning interatomic potentials (MLIPs) have enabled molecular dynamics at near ab initio accuracy, yet remain limited to energies and forces by construction, leaving electronic observables such as dipole moments and…
Electron dynamics in metallic clusters are examined using a time-dependent density functional theory that in-cludes a "memory term", i.e. attempts to describe temporal non-local correlations. Using the Iwamoto, Gross and Kohn…
The Kohn-Sham equations underlie many important applications such as the discovery of new catalysts. Recent machine learning work on catalyst modeling has focused on prediction of the energy, but has so far not yet demonstrated significant…
In this thesis we present a new formalism to study linear and non-linear response in extended systems. Our approach is based on real-time solution of an effective Schr\"odinger equation. The coupling between electrons and external field is…
Understanding the electrodes' surface morphology influence on the ions' distribution is essential for designing the supercapacitors with enhanced energy density characteristics. We develop a model for the structure of electrolytes near the…
Using the Kohn-Sham (KS) inversion method of Hollins et al. [J. Phys.: Condens. Matter 29, 04LT01 (2017)], we invert densities from variational and diffusion quantum Monte Carlo (QMC) calculations to obtain benchmark QMC-KS potentials for a…
Methods for calculating an electron density of a periodic crystal constructed using non-orthogonal localised orbitals are discussed. We demonstrate that an existing method based on the matrix expansion of the inverse of the overlap matrix…
We obtain the conductance of a system of electrons connected to leads, within time-dependent density-functional theory, using a direct relation between the conductance and the density response function. Corrections to the non-interacting…
A Kohn-Sham (KS) inversion determines a KS potential and orbitals corresponding to a given electron density, a procedure that has applications in developing and evaluating functionals used in density functional theory. Despite the utility…
We calculate the exact Kohn-Sham potential that describes, within time-dependent density-functional theory, the propagation of an electron quasiparticle wavepacket of non-zero crystal momentum added to a ground-state model semiconductor.…
A model is developed, based on the density functional perturbation theory and the inverse Kohn-Sham method, that can be used to improve relativistic nuclear energy density functionals towards an exact but unknown Kohn-Sham…
Cluster-assembled metallic films show interesting electrical properties, both in the near-to-percolation regime, when deposited clusters do not form a complete layer yet, and when the film thickness is well above the electrical percolation…
In this chapter, we provide a review of ground-state Kohn-Sham density-functional theory of electronic systems and some of its extensions, we present exact expressions and constraints for the exchange and correlation density functionals,…