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Quantum computing has shown great potential in various quantum chemical applications such as drug discovery, material design, and catalyst optimization. Although significant progress has been made in quantum simulation of simple molecules,…
The route to reliable quantum nanoelectronic devices hinges on precise control of the electrostatic environment. For this reason, accurate methods for electrostatic simulations are essential in the design process. The most widespread…
The accurate computational determination of chemical, materials, biological, and atmospheric properties has critical impact on a wide range of health and environmental problems, but is deeply limited by the computational scaling of…
The inclusion of nucleonic exchange energy has been a long-standing challenge for the relativistic density functional theory (RDFT) in nuclear physics. We propose an orbital-dependent relativistic Kohn-Sham density functional theory to…
A detailed study of energy differences between the highest occupied and lowest unoccupied molecular orbitals (HOMO-LUMO gaps) in protein systems and water clusters is presented. Recent work questioning the applicability of Kohn-Sham…
The standard way to calculate the Kohn-Sham orbitals utilizes an approximation of the potential. The approximation consists in a projection of the potential into a finite subspace of basis functions. The orbitals, calculated with the…
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…
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…
We propose a lattice density-functional theory for {\it ab initio} quantum chemistry or physics as a route to an efficient approach that approximates the full configuration interaction energy and orbital occupations for molecules with…
For properties of interacting electron systems, Kohn-Sham (KS) theory is often favored over many-body perturbation theory (MBPT) owing to its low computational cost. However, the exact KS potential can be challenging to approximate, for…
The correlation energy in density functional theory can be expressed exactly in terms of the change in the probability of finding two electrons at a given distance $r_{12}$ (intracule density) when the electron-electron interaction is…
We propose a novel scheme to bring reduced density matrix functional theory (RDMFT) into the realm of density functional theory (DFT) that preserves the accurate density functional description at equilibrium, while incorporating accurately…
Long ranged electrostatic interactions are time consuming to calculate in molecular dynamics and Monte-Carlo simulations. We introduce an algorithmic framework for simulating charged particles which modifies the dynamics so as to allow…
In contrast to the original Kohn-Sham (KS) formalism, we propose a density functional theory (DFT) with fractional orbital occupations for the study of ground states of many-electron systems, wherein strong static correlation is shown to be…
A direct orbital optimization method is presented for density functional calculations of excited electronic states using either a real space grid or a plane wave basis set. The method is variational, provides atomic forces in the excited…
The grand canonical density functional theory for inhomogeneous systems of interacting bosons is developed in the effective action approach. The Legendre transform of the generating functional for Green's functions is used to define the…
We propose a local, O(N) molecular dynamics algorithm for the simulation of charged systems. The long ranged Coulomb potential is generated by a propagating electric field that obeys modified Maxwell equations. On coupling the…
A single-term density functional model for nondynamic and strong correlation is presented, based on single-determinant Kohn-Sham density functional theory. It is derived from modeling the adiabatic connection and contains only two nonlinear…
The recent progress of linear-scaling or O(N) methods in the density functional theory (DFT) is remarkable. We expect that first-principles molecular dynamics (FPMD) simulations based on DFT can now treat more realistic and complex systems…
With the continuous growth of processing power for scientific computing, first principles Born-Oppenheimer molecular dynamics (MD) simulations are becoming increasingly popular for the study of a wide range of problems in materials science,…