Comment on “Additional Insights Between Fermi-Löwdin Orbital SIC and the Localization Equation Constraints in SIC-DFT”
In a recent Letter, Aquino and Wong (AW) analyze the connection between the Fermi-Löwdin orbital self-interaction correction (FLO-SIC) and the traditional Perdew– Zunger self-interaction correction (PZ-SIC) methods. In this work, the authors present a derivation of the conditions required to minimize the SIC density functional theory (DFT) total energy in FLO-SIC. These involve the gradient of the energy with respect to parameters known as Fermi-orbital descriptors (FODs) (called orbital “centroids” in ref 1) that are used together with the total charge density to determine the Fermi- Löwdin orbitals (FLOs). AW state that the conditions, the vanishing of the FOD gradient components, “resemble” the localization equations (LE), the minimum energy conditions in traditional PZ-SIC. The LE involve the equality of certain off-diagonal matrix elements of different orbital-dependent Hamiltonians. While AW are careful to say that their equations do not prove the mathematical equivalence of the two methods, the discussion in the text and the graphical table of contents figure suggest that vanishing FOD gradients imply satisfaction of the LE and vice versa, and hence that the methods are equivalent. We believe this ambiguity clouds an important issue, rather than clarifying it.
- Research Organization:
- Central Michigan Univ., Mount Pleasant, MI (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Grant/Contract Number:
- SC0018331
- OSTI ID:
- 1781828
- Journal Information:
- Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Vol. 123, Issue 19; ISSN 1089-5639
- Publisher:
- American Chemical SocietyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
Web of Science
Similar Records
Fermi–Löwdin orbital self-interaction correction of adsorption energies on transition metal ions
Density Matrix Implementation of the Fermi–Löwdin Orbital Self-Interaction Correction Method