Implementation and benchmark of a long-range corrected functional in the density functional based tight-binding method

Bridging the gap between first principles methods and empirical schemes, the density functional based tight-binding method (DFTB) has become a versatile tool in predictive atomistic simulations over the past years. One of the major restrictions of this method is the limitation to local or gradient c...

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Bibliographic Details
Published in:The Journal of chemical physics 2015-11, Vol.143 (18), p.184107-184107
Main Authors: Lutsker, V, Aradi, B, Niehaus, T A
Format: Article
Language:English
Subjects:
AFFINITY
BENCHMARKS
Binding
COMPARATIVE EVALUATIONS
Computer simulation
Cures
DENSITY FUNCTIONAL METHOD
Density functional theory
Dependence
ELECTRIC FIELDS
First principles
FUNCTIONALS
IMPLEMENTATION
INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
IONIZATION POTENTIAL
Ionization potentials
MOLECULES
Organic chemistry
THERMOCHEMICAL DIAGRAMS
THERMOCHEMICAL PROCESSES
Thermochemistry
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Summary:Bridging the gap between first principles methods and empirical schemes, the density functional based tight-binding method (DFTB) has become a versatile tool in predictive atomistic simulations over the past years. One of the major restrictions of this method is the limitation to local or gradient corrected exchange-correlation functionals. This excludes the important class of hybrid or long-range corrected functionals, which are advantageous in thermochemistry, as well as in the computation of vibrational, photoelectron, and optical spectra. The present work provides a detailed account of the implementation of DFTB for a long-range corrected functional in generalized Kohn-Sham theory. We apply the method to a set of organic molecules and compare ionization potentials and electron affinities with the original DFTB method and higher level theory. The new scheme cures the significant overpolarization in electric fields found for local DFTB, which parallels the functional dependence in first principles density functional theory (DFT). At the same time, the computational savings with respect to full DFT calculations are not compromised as evidenced by numerical benchmark data.
ISSN:0021-9606
1089-7690
DOI:10.1063/1.4935095