The self-interaction error (SIE) is one of the major drawbacks of practical exchange-correlation functionals for Kohn-Sham density functional theory. Despite this, the use of methods that explicitly remove SIE from approximate density functionals is scarce in the literature due to their relatively high computational cost and lack of consistent improvement over standard modern functionals. Here, we assess the performance of a novel approach recently proposed by Pederson, Ruzsinszky, and Perdew for performing self-interaction free calculations in density functional theory based on Fermi-orbitals. To this end, we employ test sets consisting of reaction energies that are considered particularly sensitive to SIE. We found that the parameter-free Fermi-Löwdin orbital self-interaction correction method combined with standard local spin density approximation (LSDA) and Perdew-Burke-Ernzerhof (PBE) functionals gives a much better estimate of reaction energies compared to their parent LSDA and PBE functionals for most of the reactions in these two sets. They also perform on par with the global PBE0 and range-separated LC-ωPBE hybrids, which partially eliminate the SIE by including Hartree-Fock exchange. This shows the potential of the Fermi-Löwdin orbital self-interaction corrected (FLOSIC) method for practical density functional calculations without SIE.
Sharkas, Kamal, et al. "Shrinking Self-Interaction Errors with the Fermi–Löwdin Orbital Self-Interaction-Corrected Density Functional Approximation." Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, vol. 122, no. 48, Nov. 2018. https://doi.org/10.1021/acs.jpca.8b09940
Sharkas, Kamal, Li, Lin, Trepte, Kai, Withanage, Kushantha K., Joshi, Rajendra P., Zope, Rajendra R., Baruah, Tunna, Johnson, J. Karl, Jackson, Koblar A., & Peralta, Juan E. (2018). Shrinking Self-Interaction Errors with the Fermi–Löwdin Orbital Self-Interaction-Corrected Density Functional Approximation. Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, 122(48). https://doi.org/10.1021/acs.jpca.8b09940
Sharkas, Kamal, Li, Lin, Trepte, Kai, et al., "Shrinking Self-Interaction Errors with the Fermi–Löwdin Orbital Self-Interaction-Corrected Density Functional Approximation," Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory 122, no. 48 (2018), https://doi.org/10.1021/acs.jpca.8b09940
@article{osti_1781806,
author = {Sharkas, Kamal and Li, Lin and Trepte, Kai and Withanage, Kushantha K. and Joshi, Rajendra P. and Zope, Rajendra R. and Baruah, Tunna and Johnson, J. Karl and Jackson, Koblar A. and Peralta, Juan E.},
title = {Shrinking Self-Interaction Errors with the Fermi–Löwdin Orbital Self-Interaction-Corrected Density Functional Approximation},
annote = {The self-interaction error (SIE) is one of the major drawbacks of practical exchange-correlation functionals for Kohn-Sham density functional theory. Despite this, the use of methods that explicitly remove SIE from approximate density functionals is scarce in the literature due to their relatively high computational cost and lack of consistent improvement over standard modern functionals. Here, we assess the performance of a novel approach recently proposed by Pederson, Ruzsinszky, and Perdew for performing self-interaction free calculations in density functional theory based on Fermi-orbitals. To this end, we employ test sets consisting of reaction energies that are considered particularly sensitive to SIE. We found that the parameter-free Fermi-Löwdin orbital self-interaction correction method combined with standard local spin density approximation (LSDA) and Perdew-Burke-Ernzerhof (PBE) functionals gives a much better estimate of reaction energies compared to their parent LSDA and PBE functionals for most of the reactions in these two sets. They also perform on par with the global PBE0 and range-separated LC-ωPBE hybrids, which partially eliminate the SIE by including Hartree-Fock exchange. This shows the potential of the Fermi-Löwdin orbital self-interaction corrected (FLOSIC) method for practical density functional calculations without SIE.},
doi = {10.1021/acs.jpca.8b09940},
url = {https://www.osti.gov/biblio/1781806},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
issn = {ISSN 1089-5639},
number = {48},
volume = {122},
place = {United States},
publisher = {American Chemical Society},
year = {2018},
month = {11}}
Central Michigan Univ., Mount Pleasant, MI (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231; SC0018331
OSTI ID:
1781806
Alternate ID(s):
OSTI ID: 1543639
Journal Information:
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Journal Name: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory Journal Issue: 48 Vol. 122; ISSN 1089-5639