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Standard density functional approximations often give questionable results for odd-electron radical complexes, with the error typically attributed to self-interaction. In density corrected density functional theory (DC-DFT), certain classes…

Chemical Physics · Physics 2015-06-19 Min-Cheol Kim , Eunji Sim , Kieron Burke

The self consistent version of the density functional theory (DFT) is presented, which allows to calculate the ground state and dynamic properties of finite multi-electron systems such as atoms, molecules and clusters. The exact functional…

Condensed Matter · Physics 2007-05-23 M. Ya. Amusia , V. R. Shaginyan

Recently, an approximate theoretical framework was introduced, called local reduced density matrix functional theory (local-RDMFT), where functionals of the one-body reduced density matrix (1-RDM) are minimized under the additional…

Electrons in zero external magnetic field can be studied with density functional theory (DFT) or with spin-DFT (SDFT). The latter is normally used for open shell systems because its approximations appear to model better the exchange and…

Chemical Physics · Physics 2022-04-06 Timothy Callow , Benjamin Pearce , Nikitas Gidopoulos

The effective potential of electron--electron interaction and the two-particle \textquotedblleft density--density\textquotedblright\ correlation function have been calculated for a simple semiinfinite metal making allowance for the…

Mesoscale and Nanoscale Physics · Physics 2015-03-29 B. M. Markovych , I. M. Zadvorniak

This work explores the use of joint density-functional theory, a new form of density-functional theory for the ab initio description of electronic systems in thermodynamic equilibrium with a liquid environment, to describe electrochemical…

Materials Science · Physics 2015-06-05 Kendra Letchworth-Weaver , T. A. Arias

This paper aims at introducing the formal foundations of the application of reduced density-matrix theory and Green's function theory to the analysis of molecular electronic transitions. For this sake, their mechanics, applied to specific…

Chemical Physics · Physics 2022-08-09 Thibaud Etienne

Based on standard perturbation theory, we present a full quantum derivation of the formula for the orbital magnetization in periodic systems. The derivation is generally valid for insulators with or without a Chern number, for metals at…

Mesoscale and Nanoscale Physics · Physics 2009-11-13 Junren Shi , G. Vignale , Di Xiao , Qian Niu

We introduce a new functional for simulating ground-state and time-dependent electronic systems within density-functional theory. The functional combines an expression for the exact Kohn-Sham (KS) potential in the limit of complete electron…

Mesoscale and Nanoscale Physics · Physics 2021-01-15 M. J. P. Hodgson , J. D. Ramsden , T. R. Durrant , R. W. Godby

In this paper, we investigate the energy minimization model of the ensemble Kohn-Sham density functional theory for metallic systems, in which a pseudo-eigenvalue matrix and a general smearing approach are involved. We study the invariance…

Numerical Analysis · Mathematics 2022-01-19 Xiaoying Dai , Stefano de Gironcoli , Bin Yang , Aihui Zhou

Density functional theory (DFT), the most widely adopted method in modern computational chemistry, fails to describe accurately the electronic structure of strongly correlated systems. Here we show that DFT can be formally and practically…

Chemical Physics · Physics 2022-04-18 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

Reduced density matrix functional theory for the case of solids is presented and a new exchange correlation functional based on a fractional power of the density matrix is introduced. We show that compared to other functionals, this…

Materials Science · Physics 2009-11-13 S. Sharma , J. K. Dewhurst , N. N. Lathiotakis , E. K. U. Gross

Using the optimized effective potential method in conjunction with the semi-analytical approximation due to Krieger, Li and Iafrate, we have performed fully self-consistent exact exchange-only density-functional calculations for diatomic…

chem-ph · Physics 2008-02-03 T. Grabo , E. K. U. Gross

Two electrons at the threshold of ionization represent a severe test case for electronic structure theory. A pseudospectral method yields a very accurate density of the two-electron ion with nuclear charge close to the critical value.…

Chemical Physics · Physics 2014-08-12 Paul E. Grabowski , Kieron Burke

We derive an exact representation of the exchange-correlation energy within density functional theory (DFT) which spawns a class of approximations leading to correct long-range asymptotic behavior. In what amounts to be the simplest…

Materials Science · Physics 2009-11-10 Roi Baer , Daniel Neuhauser

The current work presents a natural orbital functional (NOF) for electronic systems with any spin value independent of the external potential being considered, that is, a global NOF (GNOF). It is based on a new two-index reconstruction of…

Chemical Physics · Physics 2021-12-07 Mario Piris

We present an exact single-electron picture that describes the correlated electron dynamics in strong laser fields. Our approach is based on the factorization of the electronic wavefunction as a product of a marginal and a conditional…

Chemical Physics · Physics 2017-04-26 Axel Schild , E. K. U. Gross

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

Ab initio electronic structure methods give accurate results for small systems, but do not scale well to large systems. Chemical insight tells us that molecular functional groups will behave approximately the same way in all molecules,…

Chemical Physics · Physics 2007-05-23 Benjamin G. Janesko , David Yaron

The practical success of density functional theory (DFT) is largely credited to the Kohn-Sham approach, which enables the exact calculation of the non-interacting electron kinetic energy via an auxiliary noninteracting system. Yet, the…

Computational Physics · Physics 2025-03-21 Sangita Majumdar , Zekun Shi , Giovanni Vignale