Related papers: Optimized local basis set for Kohn-Sham density fu…
A bivariate perspective on Kohn-Sham density functional theory is proposed, treating potential and density as simultaneous independent variables, and used to make fruitful connection between Lieb's rigorous foundational framework and…
The use of energy functionals based on density as the basic variable is advocated for ab initio molecular dynamics. It is demonstrated that the constraint of positivity of density can be incorporated easily by using square root density for…
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…
Density functional theory is currently the most widely applied method in electronic structure theory. The Kohn-Sham method, based on a fictitious system of non-interacting particles, is the work horse of the theory. The particular form of…
The Kohn-Sham equation is a powerful, widely used approach for computation of ground state electronic energies and densities in chemistry, materials science, biology, and nanosciences. In this paper, we study the adaptive finite element…
Deriving accurate energy density functional is one of the central problems in condensed matter physics, nuclear physics, and quantum chemistry. We propose a novel method to deduce the energy density functional by combining the idea of the…
In this note, we show that the Local Molecular Field theory of Weeks et. al. can be re-derived as an extremum problem for an approximate Helmholtz free energy. Using the resulting free energy as a classical, fluid density functional yields…
We present a computational approach which is tailored for reducing the complexity of the description of extended systems at the density functional theory level. We define a recipe for generating a set of localized basis functions which are…
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…
Linear scaling methods for density-functional theory (DFT) simulations are formulated in terms of localised orbitals in real-space, rather than the delocalised eigenstates of conventional approaches. In local-orbital methods, relative to…
A way to improve the accuracy of the spectral properties in density functional theory (DFT) is to impose constraints on the effective, Kohn-Sham (KS), local potential [J. Chem. Phys. {\bf 136}, 224109 (2012)]. As illustrated, a convenient…
Limited resources motivate decomposing large-scale problems into smaller,``local" subsystems and stitching together the so-found solutions. We explore the physics underlying this approach and discuss the concept of ``local hardness", i.e.,…
An accurate expression of the kinetic energy density of an electronic distribution in terms of the single particle reduced density matrix for atomic and molecular systems is a long-standing problem in electron structure theory. Existing…
As a proof of principle, self-consistent Kohn--Sham calculations are performed with the exact exchange-correlation functional. Finding the exact functional for even one trial density requires solving the interacting Schr\"odinger equation…
The rectangular collocation approach makes it possible to solve the Schr\"odinger equation with basis functions that do not have amplitude in all regions in which wavefunctions have significant amplitude. Collocation points can be…
We propose a general machine learning-based framework for building an accurate and widely-applicable energy functional within the framework of generalized Kohn-Sham density functional theory. To this end, we develop a way of training…
The general procedure underlying Hartree-Fock and Kohn-Sham density functional theory calculations consists in optimizing orbitals for a self-consistent solution of the Roothaan-Hall equations in an iterative process. It is often ignored…
We present a computationally efficient approach to solve the time-dependent Kohn-Sham equations in real-time using higher-order finite-element spatial discretization, applicable to both pseudopotential and all-electron calculations. To this…
One of the most powerful strategies to address properties of real many-body systems is to incorporate data obtained for models, for example, to use data of the homogeneous electron gas in order to build the Local Density Approximation for…
In recent years, many types of machine learning potentials (MLPs) have been introduced, which are able to represent high-dimensional potential-energy surfaces (PES) with close to first-principles accuracy. Most current MLPs rely on atomic…