PyFLOSIC: OpenSource Implementation of the Fermi-Löwdin-Orbital Self-Interaction-Correction for use in PySCF

• Applicant: Professor Dr. Jens Kortus
• Subject Area: Theoretical Condensed Matter Physics
• Term: from 2019 to 2023
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 421663657

• Final Report Year: 2023

Final Report Abstract

All modern density functional approximations (DFAs) utilized in everyday density functional theory (DFT) calculations suffer from the self-interaction error (SIE). We implemented the novel Fermi-Löwdin orbital self-interaction correction (FLO-SIC) method, i.e., a method encountering SIE in an orbital-by-orbital formulation, on top of the PYSCF electronic structure package as Open-Source package entitled Python-based Fermi–Löwdin orbital selfinteraction correction (PyFLOSIC). Utilizing our PYFLOSIC code, we were able to show, that Fermi-orbital descriptors (FODs) – needed for each FLO-SIC calculation – carry chemical information that agrees in many cases with commonly known Lewis theory (LT) of bonding. In this context, we revived the nearly forgotten Linnett’s double-quartet (LDQ) theory, as for some molecules FODs following LDQ give the lowest energy in FLO-SIC. With our contributions, we are the first who established, used, compared, and analyzed LDQ-FLO-SIC. We designed, implemented, and tested various methods for the generation of FODs, which find common usage in FLO-SIC calculations. With our Psi-k supported workshop Quo vadis Self-InteractionCorrection (QVSIC)? we brought together the experts of the field and may revived also the interest of the people in the self-interaction correction (SIC) method.

Publications

• Interpretation and Automatic Generation of Fermi‐Orbital Descriptors. Journal of Computational Chemistry, 40(32), 2843-2857.
  Schwalbe, Sebastian; Trepte, Kai; Fiedler, Lenz; Johnson, Alex I.; Kraus, Jakob; Hahn, Torsten; Peralta, Juan E.; Jackson, Koblar A. & Kortus, Jens
  
• Stretched or noded orbital densities and self-interaction correction in density functional theory. The Journal of Chemical Physics, 150(17).
  Shahi, Chandra; Bhattarai, Puskar; Wagle, Kamal; Santra, Biswajit; Schwalbe, Sebastian; Hahn, Torsten; Kortus, Jens; Jackson, Koblar A.; Peralta, Juan E.; Trepte, Kai; Lehtola, Susi; Nepal, Niraj K.; Myneni, Hemanadhan; Neupane, Bimal; Adhikari, Santosh; Ruzsinszky, Adrienn; Yamamoto, Yoh; Baruah, Tunna; Zope, Rajendra R. & Perdew, John P.
  
• PyFLOSIC: Python-based Fermi–Löwdin orbital self-interaction correction. The Journal of Chemical Physics, 153(8).
  Schwalbe, Sebastian; Fiedler, Lenz; Kraus, Jakob; Kortus, Jens; Trepte, Kai & Lehtola, Susi
  
• Chemical bonding theories as guides for self-interaction corrected solutions: Multiple local minima and symmetry breaking. The Journal of Chemical Physics, 155(22).
  Trepte, Kai; Schwalbe, Sebastian; Liebing, Simon; Schulze, Wanja T.; Kortus, Jens; Myneni, Hemanadhan; Ivanov, Aleksei V. & Lehtola, Susi
  
• Testing Self‐Interaction Correction for Molecules in Solution. Advanced Engineering Materials, 24(2).
  Kraus, Jakob; Schwalbe, Sebastian; Trepte, Kai & Kortus, Jens
  
• Effect of Molecular and Electronic Geometries on the Electronic Density in FLO-SIC. Springer Proceedings in Physics, 167-186. Springer International Publishing.
  Liebing, Simon; Trepte, Kai & Schwalbe, Sebastian
  
• How good are recent density functionals for ground and excited states of one-electron systems?. The Journal of Chemical Physics, 157(17).
  Schwalbe, Sebastian; Trepte, Kai & Lehtola, Susi