Related papers: Mathematical Analysis and Numerical Approximations…
We develop an energy density matrix that parallels the one-body reduced density matrix (1RDM) for many-body quantum systems. Just as the density matrix gives access to the number density and occupation numbers, the energy density matrix…
We introduce a new approach to density functional theory based on kinetic theory, showing that the Kohn-Sham equations can be derived as a macroscopic limit of a suitable Boltzmann kinetic equation in the limit of small mean free path…
A recently proposed linear-scaling scheme for density-functional pseudopotential calculations is described in detail. The method is based on a formulation of density functional theory in which the ground state energy is determined by…
Here we present a density matrix based KS inversion method formulated entirely within a Gaussian basis representation to optimize a KS potential matrix that reproduces a target electron density. Inverse Kohn-Sham (KS) density functional…
We present an accurate and efficient formulation for the calculation of phonons in real-space Kohn-Sham density functional theory. Specifically, employing a local exchange-correlation functional, norm-conserving pseudopotential in the…
We present a method for total energy minimizations and molecular dynamics simulations based either on tight-binding or on Kohn-Sham hamiltonians. The method leads to an algorithm whose computational cost scales linearly with the system…
Starting from the observation that one of the most successful methods for solving the Kohn-Sham equations for periodic systems -- the plane-wave method -- is a spectral method based on eigenfunction expansion, we formulate a spectral method…
Molecular dynamics simulations are indispensable for exploring the behavior of atoms and molecules. Grounded in quantum mechanical principles, quantum molecular dynamics provides high predictive power but its computational cost is dominated…
Recently, a new connection between density functional theory and kinetic theory has been proposed. In particular, it was shown that the Kohn-Sham (KS) equations can be reformulated as a macroscopic limit of the steady-state solution of a…
We derive and analyze a hierarchy of approximations to the strongly correlated limit of the Hohenberg-Kohn functional. These "density representability approximations" are obtained by first noting that in the strongly correlated limit,…
Density matrix embedding theory (DMET) provides a theoretical framework to treat finite fragments in the presence of a surrounding molecular or bulk environment, even when there is significant correlation or entanglement between the two. In…
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…
Machine learning is employed to build an energy density functional for self-bound nuclear systems for the first time. By learning the kinetic energy as a functional of the nucleon density alone, a robust and accurate orbital-free density…
We introduce a general, variational scheme applied to Kohn-Sham density functional theory that allows for partitioning of the ground-state density matrix into distinct spectral domains, each of which spanned by an independent diagonal…
Density functional calculations on atoms are often used for determining accurate initial guesses as well as generating various types of pseudopotential approximations and efficient atomic-orbital basis sets for polyatomic calculations. To…
We introduce a new form of density functional theory for the {\em ab initio} description of electronic systems in contact with a molecular liquid environment. This theory rigorously joins an electron density-functional for the electrons of…
Electrochemical energy storage always involves the capacitive process. The prevailing electrode model used in the molecular simulation of polarizable electrode-electrolyte systems is the Siepmann-Sprik model developed for perfect metal…
In the density functional (DF) theory of Kohn and Sham, the kinetic energy of the ground state of a system of noninteracting electrons in a general external field is calculated using a set of orbitals. Orbital free methods attempt to…
Motivated by the qualitative picture of Canonical Typicality, we propose a refined formulation of the Eigenstate Thermalization Hypothesis (ETH) for chaotic quantum systems. The new formulation, which we refer to as subsystem ETH, is in…
We derive the expressions for configurational forces in Kohn-Sham density functional theory, which correspond to the generalized variational force computed as the derivative of the Kohn-Sham energy functional with respect to the position of…