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We present an ``orbital'' free density functional theory for computing the quantum ground state of atomic clusters and liquids. Our approach combines the Bohm hydrodynamical description of quantum mechanics with an information theoretical…

Soft Condensed Matter · Physics 2016-08-31 Sean W. Derrickson , Eric R. Bittner

The ground state energy of a system of electrons and nuclei is proven to be a variational functional of the conditional electronic density $n_R(\mathbf{r})$, the nuclear wavefunction $\chi(R)$ and an induced vector potential $A_{\mu}(R)$…

Chemical Physics · Physics 2016-11-08 Ryan Requist , E. K. U. Gross

Degenerate perturbation theory from quantum mechanics is inadequate in density functional theory (DFT) because of nonlinearity in the Kohn-Sham potential. Herein, we develop the fully general perturbation theory for open-shell, degenerate…

Materials Science · Physics 2017-07-19 Mark C. Palenik , Brett I. Dunlap

Ground-state Kohn-Sham density functional theory provides, in principle, the exact ground-state energy and electronic spin-densities of real interacting electrons in a static external potential. In practice, the exact density functional for…

Chemical Physics · Physics 2022-07-11 Aaron D. Kaplan , Mel Levy , John P. Perdew

Alchemical transformations showed that perturbation theory can be applied also to changes in the atomic nuclear charges of a molecule. The alchemical path that connects two different chemical species involves the conceptualization of a…

Chemical Physics · Physics 2024-03-27 Giorgio Domenichini

Density functional theory (DFT) is a widespread and effective tool in electronic structure calculations for ground-state electron systems. Its success has prompted exploration into the use of DFT for non-collective excited states. The delta…

Chemical Physics · Physics 2025-08-12 Ethan Pollack , Rohan Maniar , John P. Perdew

Standard approximations for the exchange-correlation (XC) functional in Kohn-Sham density functional theory (KS-DFT) typically lead to unacceptably large errors when applied to strongly-correlated electronic systems. Partition-DFT (PDFT) is…

Chemical Physics · Physics 2023-09-12 Yi Shi , Yuming Shi , Adam Wasserman

Density functional theory (DFT) is an exact alternative formulation of quantum mechanics, in which it is possible to calculate the total energy, the spin and the charge density of many-electron systems in the ground state. In practice, it…

Atomic Physics · Physics 2014-03-25 Uri Argaman , Guy Makov , Eli Kraisler

An explicitly orbital-dependent correlation energy functional is proposed, which is to be used in combination with the orbital-dependent exchange energy functional in energy-band calculations. It bears a close resemblance to the…

Strongly Correlated Electrons · Physics 2009-11-10 Masahiko Higuchi , Hiroshi Yasuhara

High-entropy alloys (HEAs) exhibit exceptional catalytic performance due to their complex surface structures. However, the vast number of active binding sites in HEAs, as opposed to conventional alloys, presents a significant computational…

Materials Science · Physics 2024-08-22 Mohamed Hendy , Okan K. Orhan , Homin Shin , Ali Malek , Mauricio Ponga

The thorough treatment of electron-lattice interactions from first principles is one of the main goals in condensed matter physics. While the commonly applied adiabatic Born-Oppenheimer approximation is sufficient for describing many…

Modern density functional approximations achieve moderate accuracy at low computational cost for many electronic structure calculations. Some background is given relating the gradient expansion of density functional theory to the WKB…

Chemical Physics · Physics 2021-01-27 Kieron Burke

For orbital-free {\it ab initio} molecular dynamics, especially on systems in extreme thermodynamic conditions, we provide the first pseudo-potential-adapted generalized gradient approximation (GGA) functional for the non-interacting free…

Chemical Physics · Physics 2020-02-19 Kai Luo , Valentin V. Karasiev , S. B. Trickey

We survey approaches to nonrelativistic density functional theory (DFT) for nuclei using progress toward ab initio DFT for Coulomb systems as a guide. Ab initio DFT starts with a microscopic Hamiltonian and is naturally formulated using…

Nuclear Theory · Physics 2009-12-04 J. E. Drut , R. J. Furnstahl , L. Platter

The universal functional of Hohenberg-Kohn is given as a coupling-constant integral over the density as a functional of the potential. Conditions are derived under which potential-functional approximations are variational. Construction via…

Other Condensed Matter · Physics 2011-06-13 Attila Cangi , Donghyung Lee , Peter Elliott , Kieron Burke , E. K. U. Gross

We develop an ensemble density functional theory for the fractional quantum Hall effect using a local density approximation. Model calculations for edge reconstructions of a spin-polarized quantum dot give results in good agreement with…

Condensed Matter · Physics 2009-10-28 O. Heinonen , M. I. Lubin , M. D. Johnson

We derive the second-order approximation (PT2) to the ensemble correlation energy functional by applying the G\"{o}rling-Levy perturbation theory on the ensemble density-functional theory (EDFT). Its performance is checked by calculating…

Computational Physics · Physics 2021-11-17 Zeng-hui Yang

A very specific ensemble of ground and excited states is shown to yield an exact formula for any excitation energy as a simple correction to the energy difference between orbitals of the Kohn-Sham ground state. This alternative scheme…

Chemical Physics · Physics 2017-07-26 Zeng-hui Yang , Aurora Pribram-Jones , Kieron Burke , Carsten A. Ullrich

We introduce new and robust decompositions of mean-field Hartree-Fock (HF) and Kohn-Sham density functional theory (KS-DFT) relying on the use of localized molecular orbitals and physically sound charge population protocols. The new…

Chemical Physics · Physics 2020-12-04 Janus J. Eriksen

A density functional theory (DFT) framework is presented that links functional derivatives of free-energy functionals to non-linear static density response functions in quantum many-body systems. Within this framework, explicit expressions…

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