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Title: Self-interaction-free electric dipole polarizabilities for atoms and their ions using the Fermi-Löwdin self-interaction correction

Journal Article · · Physical Review A
 [1];  [2];  [3];  [1];  [2];  [2];  [2];  [2];  [3];  [1];  [1]
  1. Central Michigan Univ., Mount Pleasant, MI (United States)
  2. Univ. of Texas, El Paso, TX (United States)
  3. Temple Univ., Philadelphia, PA (United States)
+ Show Author Affiliations

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 self-interaction 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 self-interaction-corrected (SIC) DFAs with experiment and with high-level quantum chemistry reference values. The SIC results are obtained using the Fermi-Löwdin orbital self-interaction correction (FLO-SIC) method. Removing self-interaction generally leads to smaller polarizabilities that agree significantly better with reference values. In conclusion, we find that FLO-SIC improves the performance of the local spin density approximation and the generalized gradient approximation (GGA) for polarizabilities to a quality that is comparable to so-called rung 4 functionals, but slightly degrades the performance of the strongly constrained and appropriately normed meta-GGA functional.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Complex Materials from First Principles (CCM); Central Michigan Univ., Mount Pleasant, MI (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
Contributing Organization:
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
Grant/Contract Number:
SC0018331; SC0012575; SC0006818; SC0002168
OSTI ID:
1532407
Alternate ID(s):
OSTI ID: 1546377
Journal Information:
Physical Review A, Vol. 100, Issue 1; ISSN 2469-9926
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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Cited By (4)

Importance of self-interaction-error removal in density functional calculations on water cluster anions journal January 2020
Fermi-Löwdin orbital self-interaction correction using the strongly constrained and appropriately normed meta-GGA functional journal October 2019
A step in the direction of resolving the paradox of Perdew-Zunger self-interaction correction journal December 2019
Importance of self-interaction-error removal in density functional calculations on water cluster anions text January 2020

Figures / Tables (6)

FIG. 1(p. 7)figure FIG. 1
FIG. 2(p. 8)figure FIG. 2
FIG. 3(p. 9)figure FIG. 3
TABLE I(p. 10)table TABLE I
TABLE II(p. 11)table TABLE II
TABLE III(p. 13)table TABLE III

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Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
self-interaction correction
density functional theory
polarizability