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We formulate a time-dependent density functional theory for the coupled dynamics of electrons and nuclei that goes beyond the Born-Oppenheimer (BO) approximation. We prove that the time-dependent marginal nuclear probability density…

Chemical Physics · Physics 2025-11-14 Chen Li , Ryan Requist , E. K. U. Gross

On the basis of the zero-temperature grand canonical ensemble generalization of the energy E[N,N_s,v,B] for fractional particle N and spin N_s numbers, the energy surface over the (N,N_s) plane is displayed and analyzed in the case of…

Atomic Physics · Physics 2010-11-10 T. Gal , P. Geerlings

Using a simplified one-dimensional model of a diatomic molecule, the associated interacting density and corresponding Kohn-Sham potential have been obtained analytically for all fractional molecule occupancies $N$ between 0 and 2. For the…

Atomic Physics · Physics 2016-11-15 A. Benitez , C. R. Proetto

In this article, we consider the extended Kohn-Sham model for atoms subjected to cylindrically-symmetric external potentials. The variational approximation of the model and the construction of appropriate discretization spaces are detailed…

Mathematical Physics · Physics 2018-07-04 Eric Cancès , Nahia Mourad

By extrapolating the energies of non-relativistic atoms and their ions with up to 3000 electrons within Kohn-Sham density functional theory, we find that the ionization potential remains finite and increases across a row, even as…

Materials Science · Physics 2015-05-19 Lucian A. Constantin , John C. Snyder , John P. Perdew , Kieron Burke

We discuss the usefulness of Born-Oppenheimer potential surfaces for nuclear dynamics for molecules strongly coupled to metal surfaces. A simple model demonstrating the construction of such surface for a molecular junction is discussed.

Mesoscale and Nanoscale Physics · Physics 2009-09-07 Michael Galperin , Abraham Nitzan , Mark A. Ratner

Accurate local Kohn-Sham potentials have been constructed for the ground $1s^2 ^1S$ state and, in particular, for the lowest triplet $1s2s ^{3}S$ state of the helium atom, using electron densities from many-body calculations and the…

Atomic Physics · Physics 2016-08-16 I. Lindgren , S. Salomonson , F. Möller

Basics of the Born-Oppenheimer (B-O) approximation are reviewed. Assuming the domain of applicability of B-O approximation is limited to 4 significant digits (s.d.) in energy spectrum, where mass, relativistic and QED corrections do NOT…

Atomic Physics · Physics 2025-04-10 Horacio Olivares-Pilon , Alexander V Turbiner

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…

Strongly Correlated Electrons · Physics 2009-11-13 Jeng-Da Chai , John D Weeks

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…

Chemical Physics · Physics 2015-06-15 M. Mendoza , S. Succi , H. J. Herrmann

The near nucleus behavior of the exchange-correlation potential $v_{xc}({\bf r})$ in Hohenberg-Kohn-Sham density functional theory is investigated. It is shown that near the nucleus the linear term of $O(r)$ of the spherically averaged…

Materials Science · Physics 2009-11-13 Zhixin Qian

The Born-Oppenheimer potential for the $^1\Sigma_g^+$ state of H$_2$ is obtained in the range of 0.1 -- 20 au, using analytic formulas and recursion relations for two-center two-electron integrals with exponential functions. For small…

Chemical Physics · Physics 2015-05-19 Krzysztof Pachucki

The exchange-correlation energy in Kohn-Sham density functional theory is expressed as a functional of the electronic density and the Kohn-Sham orbitals. An alternative to Kohn-Sham theory is to express the energy as a functional of the…

Computational Physics · Physics 2009-10-31 S. Goedecker , C. Umrigar

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…

Materials Science · Physics 2021-01-15 Jack Wetherell , Matthew Hodgson , Leopold Talirz , Rex Godby

Polymer self-consistent field theory techniques are used to derive quantum density functional theory without the use of the theorems of density functional theory. Instead, a free energy is obtained from a partition function that is…

Chemical Physics · Physics 2022-11-29 Russell B. Thompson

The atomization energies of molecules from first-principles density functional approximations improve from the local spin-density approximation (LSDA) to the Perdew-Burke-Ernzerhof (PBE)) generalized gradient approximation (GGA) to the…

Chemical Physics · Physics 2024-06-19 Shah Tanvir ur Rahman Chowdhury , John P. Perdew

The Hohenberg-Kohn theorem and the Kohn-Sham equations, which are at the basis of the Density Functional Theory, are reformulated in terms of a particular many-body density, which is translational invariant and therefore is relevant for…

Nuclear Theory · Physics 2021-09-29 A. Kievsky , G. Orlandini , M. Gattobigio

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

For the $S$ states of two-electron atoms, we introduce an exact and unique factorization of the internal eigenfunction in terms of a marginal amplitude, which depends functionally on the electron-nucleus distances $r_1$ and $r_2$, and a…

Atomic Physics · Physics 2017-02-08 L. D. Salas , J. C. Arce

We present a new theory for partitioning simulations of periodic and solid-state systems into physically sound atomic contributions at the level of Kohn-Sham density functional theory. Our theory is based on spatially localized linear…

Chemical Physics · Physics 2024-10-01 Luna Zamok , Janus J. Eriksen
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