Self-Interaction Correction in F-Electron Systems

Approximations to density functional theory typically overestimate the electronic coulomb energy in quantum systems and the origin of this overestimate leads to especially large self-interaction errors in rare earth containing molecules and materials. For example, in the Ln row, DFT often underestimates the number of f-electrons in the neutral atom compared to experiment. The self-interaction correction (SIC) cures the prevalent self-interaction error in DFT calculations and is known to localize orbitals. Calculations addressing the role of the self-interaction correction for correcting the electronic valence configuration in the elements of the lanthanide series are presented using the Fermi-Löwdin Orbital Self Interaction Correction (FLOSIC) methodology.[1] The work presented here utilized a newly developed tool for algorithmic parallelization of the solution of Poisson’s equation, and for selecting FODs within the Naval Research Laboratory Molecular Orbital Library (NRLMOL).
[1] M.R. Pederson, A. Ruzsinszky and J. P. Perdew, J. Chem. Phys. 140 121103 (2014).