Simplification of the Fermi–Löwdin Self‐Interaction Correction Method for Efficient Self‐Interaction‐Free Density Functional Calculations
Year: 2025
Type: article
Abstract: Fermi–Löwdin orbital self‐interaction‐correction (FLOSIC) method uses symmetric orthogonalized Fermi orbitals as localized orbitals in one‐electron SIC schemes. In FLOSIC, a set of Fermi orbital descriptors (FOD) defines the FLOs and is obtained by energy minimization. Determination of optimal FODs is a computationally very demanding task. Herein, simplification of the FLOSIC calculations by removing self‐interaction error from a set of selected orbitals of interest (SOSIC) is proposed. This approach is illustrated by choosing a set of valence orbitals as active orbitals. The results of a wide range of properties obtained using the valence SOSIC (vSOSIC) scheme are compared against the Perdew–Zunger SIC results. The two methods agree within a few percent for the majority of the properties. The mean absolute error in the vertical detachment energy of water cluster anions with vSOSIC‐Perdew–Burke–Ernzerhof (PBE) against benchmark CCSD(T) results is only 15 meV making vSOSIC‐PBE an excellent alternative to the CCSD(T) for the case. The calculation on the [CuCl]2− complex demonstrates that the FOD optimization in vSOSIC is substantially smoother and faster. Assessment of the performance of SIC‐rSCAN shows that it performs similarly to the SIC‐Strongly Constrained and Appropriately Normed functional (SCAN) for most properties, but for atomization energies, SIC‐rSCAN outperforms SIC‐SCAN.
Source: ChemPhysChem
Institution: The University of Texas at El Paso
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: green
OpenAlex ID: W4413106986