Self-consistent self-interaction corrected density functional theory calculations for atoms using Fermi-Löwdin orbitals: Optimized Fermi-orbital descriptors for Li-Kr

Der-You Kao; Kushantha Withanage; Torsten Hahn; Javaria Batool; Jens Kortus; Koblar Jackson

doi:10.1063/1.4996498

Self-consistent self-interaction corrected density functional theory calculations for atoms using Fermi-Löwdin orbitals: Optimized Fermi-orbital descriptors for Li-Kr

J Chem Phys. 2017 Oct 28;147(16):164107. doi: 10.1063/1.4996498.

Authors

Der-You Kao¹, Kushantha Withanage¹, Torsten Hahn², Javaria Batool³, Jens Kortus², Koblar Jackson¹

Affiliations

¹ Physics Department and Science of Advanced Materials Ph.D. Program, Central Michigan University, Mt Pleasant, Michigan 48859, USA.
² Institute of Theoretical Physics, TU Bergakademie Freiberg, 09596 Freiberg, Germany.
³ Department of Chemistry, The Johns Hopkins University, Baltimore, Maryland 21218, USA.

PMID: 29096512
DOI: 10.1063/1.4996498

Abstract

In the Fermi-Löwdin orbital method for implementing self-interaction corrections (FLO-SIC) in density functional theory (DFT), the local orbitals used to make the corrections are generated in a unitary-invariant scheme via the choice of the Fermi orbital descriptors (FODs). These are M positions in 3-d space (for an M-electron system) that can be loosely thought of as classical electron positions. The orbitals that minimize the DFT energy including the SIC are obtained by finding optimal positions for the FODs. In this paper, we present optimized FODs for the atoms from Li-Kr obtained using an unbiased search method and self-consistent FLO-SIC calculations. The FOD arrangements display a clear shell structure that reflects the principal quantum numbers of the orbitals. We describe trends in the FOD arrangements as a function of atomic number. FLO-SIC total energies for the atoms are presented and are shown to be in close agreement with the results of previous SIC calculations that imposed explicit constraints to determine the optimal local orbitals, suggesting that FLO-SIC yields the same solutions for atoms as these computationally demanding earlier methods, without invoking the constraints.