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We introduce a novel energy functional for ground-state electronic-structure calculations. Its fundamental variables are the natural spin-orbitals of the implied singlet many-body wave function and their joint occupation probabilities. The…

Chemical Physics · Physics 2015-06-23 Ralph Gebauer , Morrel H. Cohen , Roberto Car

New ways to treat electron correlation in electronic structure problems are discussed in the context of many-electron theory. The present work focuses primarily on static correlation. In related work, a method for including dynamical…

Chemical Physics · Physics 2018-09-05 Jerry L. Whitten

A framework for developing new approximate electronic structure methods is presented, in which the correlation energy of a many-electron system in the ground state is computed as in the single-reference second-order many-body perturbation…

Chemical Physics · Physics 2011-06-15 Dimitri Laikov

We introduce an energy functional for ground-state electronic structure calculations. Its variables are the natural spin-orbitals of singlet many-body wave functions and their joint occupation probabilities deriving from controlled…

Chemical Physics · Physics 2016-12-04 Ralph Gebauer , Morrel H. Cohen , Roberto Car

The account of electron correlation and its efficient separation into dynamic and nondynamic parts plays a key role in the development of computational methods. In this paper we suggest a physically-sound matrix formulation to split…

Chemical Physics · Physics 2016-08-16 Eloy Ramos-Cordoba , Pedro Salvador , Eduard Matito

Methods based on propagation of the one-body reduced density-matrix hold much promise for the simulation of correlated many-electron dynamics far from equilibrium, but difficulties with finding good approximations for the interaction term…

Chemical Physics · Physics 2016-02-12 Peter Elliott , Neepa T. Maitra

The current work presents a new single-reference method for capturing at the same time the static and dynamic electron correlation. The starting-point is a determinant wavefunction formed with natural orbitals obtained from a new…

Chemical Physics · Physics 2017-08-16 Mario Piris

Quantitatively accurate electronic structure calculations rely on the proper description of electron correlation. A judicious choice of the approximate quantum chemistry method depends upon the importance of dynamic and nondynamic…

Chemical Physics · Physics 2019-05-09 Eloy Ramos-Cordoba , Eduard Matito

Multi-configurational approaches yield universal wave function parameterizations that can qualitatively well describe electronic structures along reaction pathways. For quantitative results, multi-reference perturbation theory is required…

Chemical Physics · Physics 2016-09-08 Christopher J. Stein , Vera von Burg , Markus Reiher

The multilayer multiconfiguration time-dependent Hartree theory within second quantization representation of the Fock space is applied to study correlated electron transport in models of single-molecule junctions. Extending previous work,…

Mesoscale and Nanoscale Physics · Physics 2015-06-12 Haobin Wang , Michael Thoss

In this perspective, the various measures of electron correlation used in wavefunction theory, density functional theory and quantum information theory are briefly reviewed. We then focus on a more traditional metric based on dominant…

Chemical Physics · Physics 2023-04-07 Róbert Izsák , Aleksei V Ivanov , Nick S. Blunt , Nicole Holzmann , Frank Neese

A new method to determine electron correlation energy is described. This method is based on a better representation of the potential due to interacting electrons that is obtained by specifying both the average and standard deviation. The…

Materials Science · Physics 2007-05-23 T. R. S. Prasanna

We present two methods of calculating the spatial entanglement of an interacting electron system within the framework of density-functional theory. These methods are tested on the model system of Hooke's atom for which the spatial…

Quantum Physics · Physics 2015-03-13 J. P. Coe , A. Sudbery , I. D'Amico

Multi-configurational electronic structure theory delivers the most versatile approximations to many-electron wavefunctions, flexible enough to deal with all sorts of transformations, ranging from electronic excitations, to open-shell…

Chemical Physics · Physics 2024-05-07 Kalman Szenes , Maximilian Moerchen , Paul Fischill , Markus Reiher

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

New models of the Fock space sector corresponding to some fixed number of electrons are introduced. These models originate from the representability theory and their practical implementation may lead to essential reduction of dimensions of…

Chemical Physics · Physics 2016-09-08 A. I. Panin

The concept of electronic correlations plays an important role in modern condensed matter physics. It refers to interaction effects which cannot be explained within a static mean-field picture as provided by Hartree-Fock theory. Electronic…

Strongly Correlated Electrons · Physics 2015-03-17 Dieter Vollhardt

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

It is shown that the electron density functional correlation functional satisfies an equation that links the N-electron and (N-1)-electron densities of the same adiabatically scaled Hamiltonian of the interacting electron system.

Materials Science · Physics 2012-04-01 Daniel P. Joubert

Density functional theory can be extended to excited states by means of a unified variational approach for passive state ensembles. This extension overcomes the restriction of the typical density functional approach to ground states, and…

Chemical Physics · Physics 2019-07-10 Tim Gould , Stefano Pittalis
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