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The strong boundary normalized condition of wavefunction for fully occupied semicore 3d orbitals leads the linear response DFT+U on such metal oxide to have an insurmountable obstacle in Hubbard U determination. We treated the orbital…

Strongly Correlated Electrons · Physics 2015-11-17 Bolong Huang

We present a fully variational generalization of the pseudo self-interaction correction (VPSIC) approach previously presented in two implementations based on plane-waves and atomic orbital basis set, known as PSIC and ASIC, respectively.…

Materials Science · Physics 2015-05-28 A. Filippetti , C. D. Pemmaraju , P. Delugas , D. Puggioni , V. Fiorentini , S. Sanvito

The recently developed localized orbital scaling correction (LOSC) method shows the ability to systematically and size-consistently reduce the delocalization error existing in conventional density functional approximations (DFAs). Applying…

Chemical Physics · Physics 2020-10-19 Yuncai Mei , Zehua Chen , Weitao Yang

In the present letter, it is demonstrated how full configuration interaction (FCI) results in extended basis sets may be obtained to within sub-kJ/mol accuracy by decomposing the energy in terms of many-body expansions in the virtual…

Chemical Physics · Physics 2017-09-15 Janus J. Eriksen , Filippo Lipparini , Jürgen Gauss

The most widely-used density functionals for the exchange-correlation energy are inexact for one-electron systems. Their self-interaction errors can be severe in some applications. The problem is not only to correct the self-interaction…

Chemical Physics · Physics 2009-11-10 Stephan Kümmel , John P. Perdew

We study several approaches to orbital optimization in selected configuration interaction plus perturbation theory (SCI+PT) methods, and test them on the ground and excited states of three molecules using the semistochastic heatbath…

Chemical Physics · Physics 2021-07-14 Yuan Yao , C. J. Umrigar

Incremental full configuration interaction (iFCI) closely approximates the FCI limit with polynomial cost through a many-body expansion of the correlation energy, providing highly accurate total energies within a given basis set. To extend…

Chemical Physics · Physics 2025-02-26 Jeffrey Hatch , Paul M. Zimmerman

Self-interaction is a fundamental flaw of practical Kohn-Sham Density Functional Theory (KS DFT) approximations responsible for numerous qualitative and even catastrophic shortcomings. Whereas self-interaction is easy to characterize in…

Chemical Physics · Physics 2024-07-16 Samuel A. Slattery , Edward F. Valeev

The accurate prediction of electronic response properties of extended molecular systems has been a challenge for conventional, explicit density functionals. We demonstrate that a self-interaction correction implemented rigorously within…

Materials Science · Physics 2009-11-13 T. Körzdörfer , M. Mundt , S. Kümmel

A direct orbital optimization method is presented for density functional calculations of excited electronic states using either a real space grid or a plane wave basis set. The method is variational, provides atomic forces in the excited…

Computational Physics · Physics 2022-11-09 Aleksei V. Ivanov , Gianluca Levi , Elvar Ö. Jónsson , Hannes Jónsson

Density functional theory offers accurate structure prediction at acceptable computational cost, but commonly used approximations suffer from delocalization error; this results in inaccurate predictions of quantities such as energy band…

Materials Science · Physics 2022-08-17 Aaron Mahler , Jacob Z. Williams , Neil Qiang Su , Weitao Yang

It is demonstrated that the commonly applied self interaction correction (SIC) used in density functional theory does not remove all self interaction. We present as an alternative a novel method which, by construction, is totally free from…

Materials Science · Physics 2007-05-23 Urban Lundin , Olle Eriksson

In approximate Kohn-Sham density-functional theory, self-interaction manifests itself as the dependence of the energy of an orbital on its fractional occupation. This unphysical behavior translates into qualitative and quantitative errors…

Materials Science · Physics 2010-09-28 Ismaila Dabo , Andrea Ferretti , Nicolas Poilvert , Yanli Li , Nicola Marzari , Matteo Cococcioni

The general procedure underlying Hartree-Fock and Kohn-Sham density functional theory calculations consists in optimizing orbitals for a self-consistent solution of the Roothaan-Hall equations in an iterative process. It is often ignored…

Chemical Physics · Physics 2017-03-16 Alain C. Vaucher , Markus Reiher

We present the scheme that allows for efficient calculations of forces in the framework of pseudopotential self-interaction corrected (pSIC) formulation of the density functional theory. The scheme works with norm conserving and also with…

Strongly Correlated Electrons · Physics 2015-06-03 Malgorzata Wierzbowska , Jacek A. Majewski

A one-electron Schroedinger equation based on special one-electron potentials for atoms is shown to exist that produces orbitals for an arbitrary molecule that are sufficiently accurate to be used without modification to construct single-…

Chemical Physics · Physics 2022-05-16 Jerry L. Whitten

Local-spin-density functional calculations may be affected by severe errors when applied to the study of magnetic and strongly-correlated materials. Some of these faults can be traced back to the presence of the spurious self-interaction in…

Materials Science · Physics 2009-11-10 Alessio Filippetti , Nicola Spaldin

In effective single-electron theories, self-interaction manifests itself through the unphysical dependence of the energy of an electronic state as a function of its occupation, which results in important deviations from the ideal Koopmans…

Materials Science · Physics 2009-01-20 I. Dabo , M. Cococcioni , N. Marzari

Density functional theory calculations of electronic transport based on local exchange and correlation functionals contain self-interaction errors. These originate from the interaction of an electron with the potential generated by itself…

Mesoscale and Nanoscale Physics · Physics 2009-11-11 C. Toher , S. Sanvito

Linear scaling methods for density-functional theory (DFT) simulations are formulated in terms of localised orbitals in real-space, rather than the delocalised eigenstates of conventional approaches. In local-orbital methods, relative to…

Materials Science · Physics 2011-05-30 N. D. M. Hine , M. Robinson , P. D. Haynes , C. -K. Skylaris , M. C. Payne , A. A. Mostofi