Selfinteractionfree electric dipole polarizabilities for atoms and their ions using the FermiLöwdin selfinteraction correction
Abstract
The static electric dipole polarizability of a system is a measure of the binding of its electrons. In density functional theory calculations, this binding is weakened by the presence of unphysical selfinteraction in the density functional approximation (DFA), leading to overestimates of polarizabilities. In this work, to investigate this systematically we compare polarizabilities for the atoms from H to Ar and their anions and cations calculated in several DFAs and the corresponding selfinteractioncorrected (SIC) DFAs with experiment and with highlevel quantum chemistry reference values. The SIC results are obtained using the FermiLöwdin orbital selfinteraction correction (FLOSIC) method. Removing selfinteraction generally leads to smaller polarizabilities that agree significantly better with reference values. In conclusion, we find that FLOSIC improves the performance of the local spin density approximation and the generalized gradient approximation (GGA) for polarizabilities to a quality that is comparable to socalled rung 4 functionals, but slightly degrades the performance of the strongly constrained and appropriately normed metaGGA functional.
 Authors:

 Central Michigan Univ., Mount Pleasant, MI (United States)
 Univ. of Texas, El Paso, TX (United States)
 Temple Univ., Philadelphia, PA (United States)
 Publication Date:
 Research Org.:
 Central Michigan Univ., Mount Pleasant, MI (United States)
 Sponsoring Org.:
 USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC22). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES)
 Contributing Org.:
 Central Michigan University, the University of Texas at El Paso, Temple University, NERSC, the Texas Advanced Computing Center, and the Michigan State University High Performance Computing Center
 OSTI Identifier:
 1532407
 Alternate Identifier(s):
 OSTI ID: 1546377
 Grant/Contract Number:
 SC0018331; SC0012575; SC0006818; SC0002168
 Resource Type:
 Accepted Manuscript
 Journal Name:
 Physical Review A
 Additional Journal Information:
 Journal Volume: 100; Journal Issue: 1; Journal ID: ISSN 24699926
 Publisher:
 American Physical Society (APS)
 Country of Publication:
 United States
 Language:
 English
 Subject:
 74 ATOMIC AND MOLECULAR PHYSICS; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; selfinteraction correction; density functional theory; polarizability
Citation Formats
Withanage, Kushantha P. K., Akter, Sharmin, Shahi, Chandra, Joshi, Rajendra P., Diaz, Carlos, Yamamoto, Yoh, Zope, Rajendra, Baruah, Tunna, Perdew, John P., Peralta, Juan E., and Jackson, Koblar A. Selfinteractionfree electric dipole polarizabilities for atoms and their ions using the FermiLöwdin selfinteraction correction. United States: N. p., 2019.
Web. doi:10.1103/PhysRevA.100.012505.
Withanage, Kushantha P. K., Akter, Sharmin, Shahi, Chandra, Joshi, Rajendra P., Diaz, Carlos, Yamamoto, Yoh, Zope, Rajendra, Baruah, Tunna, Perdew, John P., Peralta, Juan E., & Jackson, Koblar A. Selfinteractionfree electric dipole polarizabilities for atoms and their ions using the FermiLöwdin selfinteraction correction. United States. doi:10.1103/PhysRevA.100.012505.
Withanage, Kushantha P. K., Akter, Sharmin, Shahi, Chandra, Joshi, Rajendra P., Diaz, Carlos, Yamamoto, Yoh, Zope, Rajendra, Baruah, Tunna, Perdew, John P., Peralta, Juan E., and Jackson, Koblar A. Mon .
"Selfinteractionfree electric dipole polarizabilities for atoms and their ions using the FermiLöwdin selfinteraction correction". United States. doi:10.1103/PhysRevA.100.012505. https://www.osti.gov/servlets/purl/1532407.
@article{osti_1532407,
title = {Selfinteractionfree electric dipole polarizabilities for atoms and their ions using the FermiLöwdin selfinteraction correction},
author = {Withanage, Kushantha P. K. and Akter, Sharmin and Shahi, Chandra and Joshi, Rajendra P. and Diaz, Carlos and Yamamoto, Yoh and Zope, Rajendra and Baruah, Tunna and Perdew, John P. and Peralta, Juan E. and Jackson, Koblar A.},
abstractNote = {The static electric dipole polarizability of a system is a measure of the binding of its electrons. In density functional theory calculations, this binding is weakened by the presence of unphysical selfinteraction in the density functional approximation (DFA), leading to overestimates of polarizabilities. In this work, to investigate this systematically we compare polarizabilities for the atoms from H to Ar and their anions and cations calculated in several DFAs and the corresponding selfinteractioncorrected (SIC) DFAs with experiment and with highlevel quantum chemistry reference values. The SIC results are obtained using the FermiLöwdin orbital selfinteraction correction (FLOSIC) method. Removing selfinteraction generally leads to smaller polarizabilities that agree significantly better with reference values. In conclusion, we find that FLOSIC improves the performance of the local spin density approximation and the generalized gradient approximation (GGA) for polarizabilities to a quality that is comparable to socalled rung 4 functionals, but slightly degrades the performance of the strongly constrained and appropriately normed metaGGA functional.},
doi = {10.1103/PhysRevA.100.012505},
journal = {Physical Review A},
number = 1,
volume = 100,
place = {United States},
year = {2019},
month = {7}
}
Web of Science
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