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Density functional theory (DFT) is the de facto approach for predicting self-consistent-field electronic structures of ground-state configurations of complex atoms, molecules, and solids and providing their property data for materials…

Materials Science · Physics 2024-01-30 Zi-Kui Liu

We show that the energy of a perturbed system can be fully recovered from the unperturbed system's electron density. We derive an alchemical integral transform by parametrizing space in terms of transmutations, the chain rule and…

Chemical Physics · Physics 2022-10-28 Simon León Krug , Guido Falk von Rudorff , O. Anatole von Lilienfeld

This chapter presents the development of a density functional theory (DFT)-based method for accurate, reliable treatment of various resonances in atoms. Many of these are known to be notorious for their strong correlation, proximity to more…

Chemical Physics · Physics 2019-04-19 Amlan K. Roy

An approximate solution to the time-dependent density functional theory (TDDFT) response equations for finite systems is developed, yielding corrections to the single-pole approximation. These explain why allowed Kohn-Sham transition…

Materials Science · Physics 2009-11-07 H. Appel , E. K. U. Gross , K. Burke

Time-dependent density-functional theory (TDDFT) is widely used to describe electronic excitations in complex finite systems with large numbers of atoms, such as biomolecules and nanocrystals. The first part of this paper will give a simple…

Materials Science · Physics 2008-08-15 C. A. Ullrich , V. Turkowski

In the recent work of S. Sharma \emph{et al.}, (arxiv.org: arxiv:0912.1118), a single-electron spectrum associated with the natural orbitals was defined as the derivative of the total energy with respect to the occupation numbers at half…

Chemical Physics · Physics 2012-03-07 E. N. Zarkadoula , S. Sharma , J. K. Dewhurst , E. K. U. Gross , N. N. Lathiotakis

In this work we explore the performance of approximations to electron correlation in reduced density-matrix functional theory (RDMFT) and of approximations to the observables calculated within this theory. Our analysis focuses on the…

Strongly Correlated Electrons · Physics 2015-02-26 Stefano Di Sabatino , Jan A. Berger , Lucia Reining , Pina Romaniello

Density functional theory (DFT) has transformed our ability to investigate and understand electronic ground states. In its original formulation, however, DFT is not suited to addressing (e.g.) degenerate ground states, mixed states with…

Chemical Physics · Physics 2025-10-30 Tim Gould , Leeor Kronik , Stefano Pittalis

Koopmans-compliant functionals emerge naturally from extending the constraint of piecewise linearity of the total energy as a function of the number of electrons to each fractional orbital occupation. When applied to approximate…

Materials Science · Physics 2015-06-19 Giovanni Borghi , Andrea Ferretti , Ngoc Linh Nguyen , Ismaila Dabo , Nicola Marzari

The recent non-empirical semi-local exchange functional of Armiento and K\"ummel, the AK13 [PRL 111, 036402 (2013)] incorporates a number of features reproduced by higher-order theory. The AK13 potential behaves analogously with the…

Chemical Physics · Physics 2016-11-02 A. Lindmaa , R. Armiento

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 showcase the advantages of orbital-free density-potential functional theory (DPFT), a more flexible variant of Hohenberg-Kohn density functional theory. DPFT resolves the usual trouble with the gradient-expanded kinetic energy functional…

Quantum Gases · Physics 2021-06-16 Martin-Isbjörn Trappe , Jun Hao Hue , Berthold-Georg Englert

It is shown here that Kohn-Sham equations cannot be derived from Hohenberg-Kohn theory without an additional postulate. Assuming that a functional derivative with respect to total electron density exists leads in general to a theory…

Condensed Matter · Physics 2007-05-23 R. K. Nesbet

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…

Chemical Physics · Physics 2015-06-03 Jeng-Da Chai

Density functional theory is the workhorse of modern electronic structure calculations, with wide-ranging applications in chemistry, physics, materials science, and machine learning. At its heart lies the exchange-correlation functional, a…

Chemical Physics · Physics 2026-02-20 Fabien Tran , Susi Lehtola , Stefano Pittalis , Miguel A. L. Marques

The treatment of atomic anions with Kohn-Sham density functional theory (DFT) has long been controversial since the highest occupied molecular orbital (HOMO) energy, $E_{HOMO}$, is often calculated to be positive with most approximate…

Chemical Physics · Physics 2019-03-20 Lindsey N. Anderson , M. Belén Oviedo , Bryan M. Wong

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

Recent advances in X-ray free-electron laser diagnostics have enabled direct probing of the electronic structure under extreme pressures and temperatures, such as those encountered in stellar interiors and inertial confinement fusion…

Reduced density-matrix functional theory (RDMFT) is a promising alternative approach to the problem of electron correlation. Like standard density functional theory, it contains an unknown exchange-correlation functional, for which several…

Chemical Physics · Physics 2017-03-03 N. N. Lathiotakis , Miguel A. L. Marques

We show an $\textit{ab initio}$ construction of the energy density functional (EDF) for electron systems using the functional renormalization group. The correlation energies of the homogeneous electron gas given in our framework reproduce…

Strongly Correlated Electrons · Physics 2021-08-03 Takeru Yokota , Tomoya Naito