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We present a wide-reaching revamp of the generalized many-body expanded full configuration interaction (MBE-FCI) method. First, we outline how to automatize the selection of reference active spaces whereby the inherent bias introduced…

Chemical Physics · Physics 2024-06-18 Jonas Greiner , Jürgen Gauss , Janus J. Eriksen

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

We use our recently developed functional bosonization approach to bosonize interacting fermions in arbitrary dimension $d$ beyond the Gaussian approximation. Even in $d=1$ the finite curvature of the energy dispersion at the Fermi surface…

Condensed Matter · Physics 2016-08-31 Peter Kopietz , Joachim Hermisson , Kurt Schoenhammer

Accurate description of the excess charge in water cluster anions is challenging for standard semi-local and (global) hybrid density functional approximations (DFAs). Using the recent unitary invariant implementation of the Perdew-Zunger…

Chemical Physics · Physics 2020-02-11 Jorge Vargas , Peter Ufondu , Tunna Baruah , Yoh Yamamoto , Koblar A. Jackson , Rajendra R. Zope

Effective field theory (EFT) methods are applied to density functional theory (DFT) as part of a program to systematically go beyond mean-field approaches to medium and heavy nuclei. A system of fermions with short-range, natural…

Nuclear Theory · Physics 2007-05-23 S. J. Puglia , A. Bhattacharyya , R. J. Furnstahl

Plane-wave electronic-structure predictions based upon orbital-dependent density-functional theory (OD-DFT) approximations, such as hybrid density-functional methods and self-interaction density-functional corrections, are severely affected…

Materials Science · Physics 2011-10-19 Yanli Li , Ismaila Dabo

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

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

We describe the behavior of the Perdew-Zunger self-interaction-corrected local density approximation (SIC-LDA) functional when implemented in a plane-wave pseudopotential formalism with Wannier functions. Prototypical semiconductors and…

Other Condensed Matter · Physics 2011-03-03 Massimiliano Stengel , Nicola A. Spaldin

Orbital-free density functional theory (OFDFT) is a quantum chemistry formulation that has a lower cost scaling than the prevailing Kohn-Sham DFT, which is increasingly desired for contemporary molecular research. However, its accuracy is…

Machine Learning · Statistics 2024-03-12 He Zhang , Siyuan Liu , Jiacheng You , Chang Liu , Shuxin Zheng , Ziheng Lu , Tong Wang , Nanning Zheng , Bin Shao

Methods for correcting residual energy errors of configuration interaction (CI) calculations of molecules and other electronic systems are discussed based on the assumption that the energy defect can be mapped onto atomic regions. The…

Chemical Physics · Physics 2022-10-05 Jerry L. Whitten

By combining the Self-Interaction Correction (SIC) with pseudopotential perturbation theory, the role of self-interaction errors inherent to the Local Density Approximation (LDA) to Density Functional Theory is estimated in the…

mtrl-th · Physics 2009-10-28 Jorge M. Pacheco , Walter Ekardt , Wolf-Dieter Schoene

Late transition-metal oxides with small charge-transfer energy $\Delta$ raise issues for state-of-the-art correlated electronic structure schemes such as the combination of density functional theory (DFT) with dynamical mean-field theory…

Strongly Correlated Electrons · Physics 2019-09-17 Frank Lechermann , Wolfgang Körner , Daniel F. Urban , Christian Elsässer

We conduct a detailed investigation of the polaron self-interaction (pSI) error in standard approximations to the exchange-correlation (XC) functional within density-functional theory (DFT). The pSI leads to delocalization error in the…

Materials Science · Physics 2020-08-03 Babak Sadigh , Paul Erhart , Daniel Åberg

Facilitated by a rigorous partitioning of a molecular system's orbital basis into two fundamental subspaces - a reference and an expansion space, both with orbitals of unspecified occupancy - we generalize our recently introduced many-body…

Chemical Physics · Physics 2019-12-12 Janus J. Eriksen , Jürgen Gauss

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 large anisotropy in the electronic properties across a structural transition in several correlated systems has been identified as the key manifestation of electronic nematic order, breaking rotational symmetry. In this context, FeSe is…

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

The Perdew-Zunger (PZ) self-interaction correction (SIC) is an established tool to correct unphysical behavior in density functional approximations. Yet, PZ-SIC is well-known to sometimes break molecular symmetries. An example of this is…

Chemical Physics · Physics 2024-10-28 Sebastian Schwalbe , Wanja Timm Schulze , Kai Trepte , Susi Lehtola

In the past decade, natural orbital functional (NOF) approximations have emerged as prominent tools for characterizing electron correlation. Despite their effectiveness, these approaches, which rely on natural orbitals and their associated…

Chemical Physics · Physics 2024-04-19 Ion Mitxelena , Mario Piris