Fermi-Löwdin orbital self-interaction correction using the strongly constrained and appropriately normed meta-GGA...

Area of Science:

• Computational Chemistry
• Materials Science
• Quantum Mechanics

Background:

• Density functional approximations (DFAs) are vital for electronic property calculations.
• Self-interaction errors (SIEs) in widely used DFAs limit their accuracy.
• The Strongly Constrained and Appropriately Normed (SCAN) meta-generalized gradient approximation is a popular DFA.

Purpose of the Study:

• To investigate the impact of removing SIEs from the SCAN approximation using the Fermi-Löwdin Orbital Self-Interaction Correction (FLOSIC) method.
• To evaluate the performance of FLOSIC-SCAN for various material properties.
• To explore the DFA@FLOSIC-DFA approach for enhanced accuracy.

Main Methods:

• Implementation of the Fermi-Löwdin Orbital Self-Interaction Correction (FLOSIC) method with the SCAN functional.
• Careful treatment of numerical details and integration grids for FLOSIC-SCAN calculations.
• Application of the DFA@FLOSIC-DFA approach, using the self-consistent FLOSIC-SCAN density within the SCAN functional.

Main Results:

• FLOSIC-SCAN generally outperforms FLOSIC-LDA and FLOSIC-PBE.
• FLOSIC-SCAN shows improved predictions for orbital and dissociation energies compared to pure SCAN.
• Total energies and atomization energies were worsened by FLOSIC-SCAN, but improved by the DFA@FLOSIC-DFA approach.
• The DFA@FLOSIC-DFA approach yielded better results than self-consistent SCAN calculations.

Conclusions:

• FLOSIC-SCAN offers improved accuracy over the parent SCAN functional for properties dominated by SIEs.
• The DFA@FLOSIC-DFA approach enhances results even when SIEs are not dominant.
• FLOSIC-SCAN represents a significant advancement in accurate electronic property prediction using DFAs.