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In practical implementations of density-functional theory, the only term where an orbital description is needed is the kinetic one. Even this term in principle depends on the density only, but its explicit form is unknown. We provide a…

In this study, we explore the potential of machine learning for modeling molecular electronic spectral intensities as a continuous function in a given wavelength range. Since presently available chemical space datasets provide excitation…

We suggest to include the density of electron charge explicitly in the electron potential of density functional theory, rather than implicitly via exchange-correlation functionals. The advantages of the approach are conceptual and…

The H\"uckel Hamiltonian is an incredibly simple tight-binding model famed for its ability to capture qualitative physics phenomena arising from electron interactions in molecules and materials. Part of its simplicity arises from using only…

While in principle exact, Kohn-Sham density functional theory -- the workhorse of computational chemistry -- must rely on approximations for the exchange-correlation functional. Despite staggering successes, present-day approximations still…

The Hohenberg-Kohn theorem plays a fundamental role in density functional theory, which has become a basic tool for the study of electronic structure of matter. In this article, we study the Hohenberg-Kohn theorem for a class of external…

Kohn-Sham density functional theory (KS-DFT) is a powerful method to obtain key materials' properties, but the iterative solution of the KS equations is a numerically intensive task, which limits its application to complex systems. To…

When a molecule dissociates, the exact Kohn-Sham (KS) and Pauli potentials may form step structures. Reproducing these steps correctly is central for the description of dissociation and charge-transfer processes in density functional theory…

Development of the electronic kinetic-energy density functional is a subject of major interest in theoretical physics and chemistry. In this work, the nonlocal kinetic-energy functional is developed in terms of the response function for the…

Density functional theory has become the world's favorite electronic structure method, and is routinely applied to both materials and molecules. Here, we review recent attempts to use modern machine-learning to improve density functional…

According to the Hohenberg-Kohn theorem of density-functional theory (DFT), all observable quantities of systems of interacting electrons can be expressed as functionals of the ground-state density. This includes, in principle, the spin…

In this paper, we investigate the energy minimization model of the ensemble Kohn-Sham density functional theory for metallic systems, in which a pseudo-eigenvalue matrix and a general smearing approach are involved. We study the invariance…

We introduce machine learning models of quantum mechanical observables of atoms in molecules. Instant out-of-sample predictions for proton and carbon nuclear chemical shifts, atomic core level excitations, and forces on atoms reach…

Predicting electronic energies, densities, and related chemical properties can facilitate the discovery of novel catalysts, medicines, and battery materials. By developing a physics-inspired equivariant neural network, we introduce a method…

The theoretical solid-state physicist Walter Kohn was awarded one-half of the 1998 Nobel Prize in Chemistry for his mid-1960's creation of an approach to the many-particle problem in quantum mechanics called density functional theory (DFT).…

We present a computationally efficient approach to perform systematically convergent real-space all-electron Kohn-Sham DFT calculations for solids using an enriched finite element (FE) basis. The enriched FE basis is constructed by…

Machine Learning (ML)-based force fields are attracting ever-increasing interest due to their capacity to span spatiotemporal scales of classical interatomic potentials at quantum-level accuracy. They can be trained based on high-fidelity…

The relationship between the exact kinetic energy density in a quantum system in the frame of Density Functional Theory and the semiclassical functional expression for the same quantity is investigated. The analysis is performed with Monte…

It is shown here that Kohn-Sham equations cannot be derived from Hohenberg-Kohn theory without an additional postulate. Assuming that a functional derivative with respect to total electron density exists leads in general to a theory…

Density-functional theory with extended Hubbard functionals (DFT+$U$+$V$) provides a robust framework to accurately describe complex materials containing transition-metal or rare-earth elements. It does so by mitigating self-interaction…