Self-Interaction and Strong Correlation in DFTB

B. Hourahine, S. Sanna, B. Aradi, C. Kohler, T. Niehaus, T. Frauenheim

Research output: Contribution to journalArticle

27 Citations (Scopus)

Abstract

The density functional based tight-binding (DFTB) method can benefit substantially from a number of developments in density functional theory (DFT) while also providing a simple analytical proving ground for new extensions. This contribution begins by demonstrating the variational nature of charge-self-consistent DFTB (SCC-DFTB), proving the presence of a defined ground-state in this class of methods. Because the ground state of the SCC-DFTB method itself can be qualitatively incorrect for some systems, suitable forms of the recent LDA+U functionals for SCC-DFTB are also presented. This leads to both a new semilocal self-interaction correction scheme and a new physical argument for the choice of parameters in the LDA+U method. The locality of these corrections can only partly repair the HOMO-LUMO gap and chemical potential discontinuity, hence a novel method for introducing this further physics into the method is also presented, leading to exact derivative discontinuities in this theory at low computational cost. The prototypical system NiO is used as an illustration for these developments.
LanguageEnglish
Pages5671-5677
Number of pages6
JournalJournal of Physical Chemistry A
Volume111
Issue number26
DOIs
Publication statusPublished - 6 Jul 2007

Fingerprint

Ground state
Chemical potential
Density functional theory
Repair
Physics
interactions
Derivatives
discontinuity
ground state
Costs
functionals
density functional theory
costs
physics

Keywords

  • density
  • tight-binding
  • DFTB
  • nanoscience
  • applied physics

Cite this

Hourahine, B., Sanna, S., Aradi, B., Kohler, C., Niehaus, T., & Frauenheim, T. (2007). Self-Interaction and Strong Correlation in DFTB. Journal of Physical Chemistry A, 111(26), 5671-5677. https://doi.org/10.1021/jp070173b
Hourahine, B. ; Sanna, S. ; Aradi, B. ; Kohler, C. ; Niehaus, T. ; Frauenheim, T. / Self-Interaction and Strong Correlation in DFTB. In: Journal of Physical Chemistry A. 2007 ; Vol. 111, No. 26. pp. 5671-5677.
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Hourahine, B, Sanna, S, Aradi, B, Kohler, C, Niehaus, T & Frauenheim, T 2007, 'Self-Interaction and Strong Correlation in DFTB' Journal of Physical Chemistry A, vol. 111, no. 26, pp. 5671-5677. https://doi.org/10.1021/jp070173b

Self-Interaction and Strong Correlation in DFTB. / Hourahine, B.; Sanna, S.; Aradi, B.; Kohler, C.; Niehaus, T.; Frauenheim, T.

In: Journal of Physical Chemistry A, Vol. 111, No. 26, 06.07.2007, p. 5671-5677.

Research output: Contribution to journalArticle

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Hourahine B, Sanna S, Aradi B, Kohler C, Niehaus T, Frauenheim T. Self-Interaction and Strong Correlation in DFTB. Journal of Physical Chemistry A. 2007 Jul 6;111(26):5671-5677. https://doi.org/10.1021/jp070173b