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We present a method to perform fully selfconsistent density-functional calculations, which scales linearly with the system size and which is well suited for very large systems. It uses strictly localized pseudoatomic orbitals as basis…

Condensed Matter · Physics 2009-10-28 Pablo Ordejon , Emilio Artacho , Jose M. Soler

One-electron self-interaction and an incorrect asymptotic behavior of the Kohn-Sham exchange-correlation potential are among the most prominent limitations of many present-day density functionals. However, a one-electron…

Chemical Physics · Physics 2016-07-06 Tobias Schmidt , Eli Kraisler , Leeor Kronik , Stephan Kümmel

The precise energy level alignment between a metal electrode and an organic semiconductor is required to reduce contact resistance and enhance the efficiency of organic-semiconductor-based devices. One of the ways is to include interlayers…

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

We consider a massless and minimally coupled self interacting quantum scalar field theory in the inflationary de Sitter background of dimension four. The self interaction potential is taken to be either quartic, $\lambda \phi^4/4!$, or…

High Energy Physics - Theory · Physics 2024-08-13 Sourav Bhattacharya , Sudesh Kumar

A method for increasing the accuracy of configuration interaction (CI) calculations of molecules and other electronic systems is proposed. The energy defect of a given calculation is associated with the electron pair origin of…

Chemical Physics · Physics 2025-11-18 Jerry L. Whitten

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

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

Natural orbital functional (NOF) theory offers a promising approach for studying strongly correlated systems at an affordable computational cost, with an accuracy comparable to highly demanding wavefunction-based methods. However, its…

Strongly Correlated Electrons · Physics 2025-01-31 Juan Felipe Huan Lew-Yee , Jorge M. del Campo , Mario Piris

Iron-sulfur clusters comprise an important functional motif of the catalytic centers of biological systems, capable of enabling important chemical transformations at ambient conditions. This remarkable capability derives from a notoriously…

We derive an automatic procedure for generating a set of highly localized, non-orthogonal orbitals for linear scaling quantum Monte Carlo calculations. We demonstrate the advantage of these orbitals in calculations of the total energy of…

Materials Science · Physics 2007-05-23 F. A. Reboredo , A. J. Williamson

An improved algorithm to evaluate the nonrelativistic three-electron Hylleraas-Configuration Interaction (Hy-CI) kinetic energy integrals over Slater orbitals and the Hamiltonian in Hylleraas coordinates is shown. The resulting analytical…

Atomic Physics · Physics 2016-01-29 Maria Belen Ruiz

Functionals that strive to correct for such self-interaction errors, such as those obtained by imposing the Perdew-Zunger self-interaction correction or the generalized Koopmans' condition, become orbital dependent or orbital-density…

Materials Science · Physics 2011-08-30 Cheol-Hwan Park , Andrea Ferretti , Ismaila Dabo , Nicolas Poilvert , Nicola Marzari

Spin-orbit coupling (SOC) is a relativistic effect, where an electron moving in an electric field experiences an effective magnetic field in its rest frame. In crystals without inversion symmetry, it lifts the spin degeneracy and leads to…

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

The Fermi-L\"owdin orbital (FLO) approach to the Perdew-Zunger self-interaction correction (PZ-SIC) to density functional theory (DFT) is described and an improved approach to the problem of optimizing the Fermi-orbitals in order to…

Chemical Physics · Physics 2019-10-24 K. A. Jackson , J. E. Peralta , R. P. Joshi , K. P. Withanage , K. Trepte , K. Sharkas , A. I. Johnson

Self-interactions (SIs) are a major problem in density functional approximations and the source of serious divergence from experimental results. Here, we propose to optimize density functional total energies in terms of the effective local…

Other Condensed Matter · Physics 2012-06-20 Nikitas I. Gidopoulos , Nektarios N. Lathiotakis

In this work, we develop a mathematical framework for a Selected Configuration Interaction (SCI) algorithm within a bi-orthogonal basis for transcorrelated (TC) calculations. The bi-orthogonal basis used here serves as the equivalent of the…

Chemical Physics · Physics 2023-06-22 Abdallah Ammar , Anthony Scemama , Emmanuel Giner

We study the effect of self-interaction errors on the barrier heights of chemical reactions. For this purpose we use the well-known Perdew-Zunger [J. P. Perdew and A. Zunger, Phys. Rev. B, {\bf 23}, 5048 (1981)] self-interaction-correction…

We propose a simplification of the full "2 sets" Time dependent Self Interaction Correction (TD-SIC) method, applying the Optimized Effective Potential (OEP) method. The new resulting scheme is called time-dependent "Generalized SIC-OEP". A…

Quantum Physics · Physics 2009-11-05 J. Messud , P. M. Dinh , P. -G. Reinhard , E. Suraud
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