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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…

Chemical Physics · Physics 2014-11-14 Tim Gould , Julien Toulouse

Recently, we introduced (e-print arXiv:1407.7128) {\em local reduced density matrix functional theory} (local RDMFT), a theoretical scheme capable of incorporating static correlation effects in Kohn-Sham equations. Here, we apply local…

Chemical Physics · Physics 2014-11-07 Nektarios N. Lathiotakis , Nicole Helbig , Angel Rubio , Nikitas I. Gidopoulos

By introducing the self-energy density functionals for the dissipative interactions between the reduced system and its environment, we develop a time-dependent density-functional theory formalism based on an equation of motion for the…

Quantum Physics · Physics 2009-11-13 Xiao Zheng , Fan Wang , Chi Yung Yam , Yan Mo , GuanHua Chen

In the distributed nucleus approximation we represent the singular nucleus as smeared over a smallportion of a Cartesian grid. Delocalizing the nucleus allows us to solve the Poisson equation for theoverall electrostatic potential using a…

chem-ph · Physics 2009-10-28 Karthik A. Iyer , Michael P. Merrick , Thomas L. Beck

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…

Soft Condensed Matter · Physics 2009-11-11 Sahak Petrosyan , Jean-Francois Briere , David Roundy , T. A. Arias

The constrained electron density method of embedding a Kohn-Sham system in a substrate system (first described by P. Cortona, Phys. Rev. B {\bf 44}, 8454 (1991) and T.A. Wesolowski and A. Warshel, J. Phys. Chem {\bf 97}, 8050 (1993)) is…

Materials Science · Physics 2015-05-14 J. R. Trail , D. M. Bird

We present recent developments of the NTChem program for performing large scale hybrid Density Functional Theory calculations on the supercomputer Fugaku. We combine these developments with our recently proposed Complexity Reduction…

We introduce an energy functional for ground-state electronic structure calculations. Its variables are the natural spin-orbitals of singlet many-body wave functions and their joint occupation probabilities deriving from controlled…

Chemical Physics · Physics 2016-12-04 Ralph Gebauer , Morrel H. Cohen , Roberto Car

We present a simple and general method for construction of localized orbitals to describe electronic structure of extended periodic metals and insulators as well as confined systems. Spatial decay of these orbitals is found to exhibit…

Materials Science · Physics 2007-05-23 Joydeep Bhattacharjee , Umesh V Waghmare

We introduce a novel energy functional for ground-state electronic-structure calculations. Its fundamental variables are the natural spin-orbitals of the implied singlet many-body wave function and their joint occupation probabilities. The…

Chemical Physics · Physics 2015-06-23 Ralph Gebauer , Morrel H. Cohen , Roberto Car

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.…

Mesoscale and Nanoscale Physics · Physics 2015-06-05 J. D. Ramsden , R. W. Godby

We resolve a fundamental issue associated with the conventional Kohn-Sham formulation of real-time time-dependent density functional theory. We show that unphysical multielectron excitations, generated during time propagation of the…

Computational Physics · Physics 2020-01-16 Xiaoning Zang , Udo Schwingenschlogl , Mark T. Lusk

Density Functional Theory's Kohn-Sham (KS) potential emerges as the minimizing effective potential in an unconstrained variational scheme that does not involve fixing the unknown single-electron density. The physical content behind the…

Other Condensed Matter · Physics 2007-05-23 N. I. Gidopoulos

Stochastic density functional theory (sDFT) is becoming a valuable tool for studying ground state properties of extended materials. The computational complexity of describing the Kohn-Sham orbitals is replaced by introducing a set of random…

Chemical Physics · Physics 2021-06-16 Ming Chen , Roi Baer , Daniel Neuhauser , Eran Rabani

We calculate ground-state energies and densities of a helium atom confined in an impenetrable spherical box within density functional theory. These calculations are performed by variationally solving Kohn-Sham equation with the ground-state…

Atomic Physics · Physics 2010-06-24 Subhajit Waugh , Avijit Chowdhury , Arup Banerjee

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…

Chemical Physics · Physics 2014-11-07 Nektarios N. Lathiotakis , Nicole Helbig , Angel Rubio , Nikitas I. Gidopoulos

Quantum computers hold promise to enable efficient simulations of the properties of molecules and materials; however, at present they only permit ab initio calculations of a few atoms, due to a limited number of qubits. In order to harness…

Materials Science · Physics 2020-07-07 He Ma , Marco Govoni , Giulia Galli

Quantum embedding theories are promising approaches to investigate strongly-correlated electronic states of active regions of large-scale molecular or condensed systems. Notable examples are spin defects in semiconductors and insulators. We…

Materials Science · Physics 2021-12-14 He Ma , Nan Sheng , Marco Govoni , Giulia Galli

We introduce a spectral density functional theory which can be used to compute energetics and spectra of real strongly--correlated materials using methods, algorithms and computer programs of the electronic structure theory of solids. The…

Strongly Correlated Electrons · Physics 2009-11-10 S. Y. Savrasov , G. Kotliar

A novel low complexity method to perform self-consistent electronic-structure calculations using the Kohn-Sham formalism of density functional theory is presented. Localization constraints are neither imposed nor required thereby allowing…

Computational Physics · Physics 2007-05-23 M. J. Rayson