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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…

Chemical Physics · Physics 2024-10-30 Priya , Mainak Sadhukhan

To construct an N-representable time-dependent density-functional theory, a generalization to the time domain of the Levy-Lieb (LL) constrained search algorithm is required. That the action is only stationary in the Dirac-Frenkel…

Other Condensed Matter · Physics 2009-11-10 Morrel H. Cohen , Adam Wasserman

Orbital-free density functional theory promises to deliver linear-scaling electronic structure calculations. This requires the knowledge of the non-interacting kinetic-energy density functional (KEDF), which should be accurate and must…

Materials Science · Physics 2024-12-12 Michael A. J. Mitchell , Teresa Del Aguila Ferrandis , Stefano Sanvito

The non-interacting kinetic energy functional, $T_{KS}(\rho)$, plays a fundamental role in Density Functional Theory (DFT), but its explicit form remains unknown for arbitrary $N$-representable densities. Although it can, in principle, be…

Chemical Physics · Physics 2025-11-19 Dharamveer Kumar , Amuthan A. Ramabathiran

The one-particle reduced density-matrix (1-RDM) functional theory is a promising alternative to density-functional theory (DFT) that uses the 1-RDM rather than the electronic density as a basic variable. However, long-standing challenges…

Quantum Physics · Physics 2024-08-20 Matthieu Vladaj , Quentin Marécat , Bruno Senjean , Matthieu Saubanère

Kohn-Sham (KS) formalism of Density Functional Theory is modified to include the systems with strong non-dynamic electron correlation. Unlike in extended KS and broken symmetry unrestricted KS formalisms, cases of both singlet-triplet and…

Chemical Physics · Physics 2007-05-23 Artem Masunov

We explore a new formalism to study the nonlinear electronic density response based on Kohn-Sham density functional theory (KS-DFT) at partially and strongly quantum degenerate regimes. It is demonstrated that the KS-DFT calculations are…

Plasma Physics · Physics 2022-05-10 Zhandos Moldabekov , Jan Vorberger , Tobias Dornheim

A relativistic density-functional theory based on a Fock-space effective quantum-electrodynamics (QED) Hamiltonian using the Coulomb or Coulomb-Breit two-particle interaction is developed. This effective QED theory properly includes the…

Chemical Physics · Physics 2021-05-03 Julien Toulouse

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

The density-functional approach to quantum electrodynamics is extending traditional density-functional theory and opens the possibility to describe electron-photon interactions in terms of effective Kohn-Sham potentials. In this work, we…

Quantum Physics · Physics 2016-02-17 Johannes Flick , Michael Ruggenthaler , Heiko Appel , Angel Rubio

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

We visualize the Kohn-Sham kinetic energy density (KED), and the ingredients -- the electron density, its gradient and Laplacian -- used to construct orbital-free models of it, for the AE6 test set of molecules. These are compared to…

Chemical Physics · Physics 2016-03-01 Antonio C. Cancio , Dane Stewart , Aeryk I. Kuna

This article generalizes the notion of the local density of a many-body system to introduce collective coordinates as explicit degrees of freedom. It is shown that the energy of the system can be expressed as a functional of this object.…

Nuclear Theory · Physics 2014-04-23 Thomas Lesinski

Orbital-free density functional theory (OF-DFT) holds the promise to compute ground state molecular properties at minimal cost. However, it has been held back by our inability to compute the kinetic energy as a functional of the electron…

Chemical Physics · Physics 2023-10-25 Roman Remme , Tobias Kaczun , Maximilian Scheurer , Andreas Dreuw , Fred A. Hamprecht

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

The dissociation of molecules, even the most simple hydrogen molecule, cannot be described accurately within density functional theory because none of the currently available functionals accounts for strong on-site correlation. This problem…

Strongly Correlated Electrons · Physics 2011-01-14 N. Helbig , I. V. Tokatly , A. Rubio

Last year, at least 30,000 scientific papers used the Kohn-Sham scheme of density functional theory to solve electronic structure problems in a wide variety of scientific fields, ranging from materials science to biochemistry to…

Computational Physics · Physics 2018-02-07 Felix Brockherde , Leslie Vogt , Li Li , Mark E. Tuckerman , Kieron Burke , Klaus-Robert Müller

The Kohn-Sham scheme of density functional theory is one of the most widely used methods to solve electronic structure problems for a vast variety of atomistic systems across different scientific fields. While the method is fast relative to…

We present a density difference based analysis for a range of orbital--dependent Kohn--Sham functionals. Results for atoms, some members of the neon isoelectronic series and small molecules are reported and compared with ab initio…

Chemical Physics · Physics 2015-01-22 I. Grabowski , A. M. Teale , E. Fabiano , S. Smiga , A. Buksztel , F. Della Sala

Density functional theory is generalized to incorporate electron-phonon coupling. A Kohn-Sham equation yielding the electronic density $n_U(\mathbf{r})$, a conditional probability density depending parametrically on the phonon normal mode…

Materials Science · Physics 2019-04-25 Ryan Requist , C. R. Proetto , E. K. U. Gross