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Title: Communication: Charge-population based dispersion interactions for molecules and materials

We introduce a system-independent method to derive effective atomic C 6 coefficients and polarizabilities in molecules and materials purely from charge population analysis. This enables the use of dispersion-correction schemes in electronic structure calculations without recourse to electrondensity partitioning schemes and expands their applicability to semi-empirical methods and tightbinding Hamiltonians. We then show that the accuracy of our method is en par with established electrondensity partitioning based approaches in describing intermolecular C 6 coefficients as well as dispersion energies of weakly bound molecular dimers, organic crystals, and supramolecular complexes. We showcase the utility of our approach by incorporation of the recently developed many-body dispersion method [Tkatchenko et al., Phys. Rev. Lett. 108, 236402 (2012)] into the semi-empirical density functional tight-binding method and propose the latter as a viable technique to study hybrid organic-inorganic interfaces.
Authors:
ORCiD logo [1] ;  [2] ;  [3] ;  [2] ; ORCiD logo [3]
  1. Yale Univ., New Haven, CT (United States). Dept. of Chemistry; Technical Univ. of Munich, Garching (Germany). Dept. of Chemistry
  2. Technical Univ. of Munich, Garching (Germany). Dept. of Chemistry
  3. Yale Univ., New Haven, CT (United States). Dept. of Chemistry
Publication Date:
Grant/Contract Number:
FG02-05ER15677
Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 144; Journal Issue: 15; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Research Org:
Yale Univ., New Haven, CT (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 74 ATOMIC AND MOLECULAR PHYSICS; optical fibers; electron density; numerical linear algebra; density-functional tight-binding; dispersion; density functional theory; polarizability; electronic structure methods; intermolecular forces; crystalline solids
OSTI Identifier:
1470763
Alternate Identifier(s):
OSTI ID: 1248058

Stöhr, Martin, Michelitsch, Georg S., Tully, John C., Reuter, Karsten, and Maurer, Reinhard J.. Communication: Charge-population based dispersion interactions for molecules and materials. United States: N. p., Web. doi:10.1063/1.4947214.
Stöhr, Martin, Michelitsch, Georg S., Tully, John C., Reuter, Karsten, & Maurer, Reinhard J.. Communication: Charge-population based dispersion interactions for molecules and materials. United States. doi:10.1063/1.4947214.
Stöhr, Martin, Michelitsch, Georg S., Tully, John C., Reuter, Karsten, and Maurer, Reinhard J.. 2016. "Communication: Charge-population based dispersion interactions for molecules and materials". United States. doi:10.1063/1.4947214. https://www.osti.gov/servlets/purl/1470763.
@article{osti_1470763,
title = {Communication: Charge-population based dispersion interactions for molecules and materials},
author = {Stöhr, Martin and Michelitsch, Georg S. and Tully, John C. and Reuter, Karsten and Maurer, Reinhard J.},
abstractNote = {We introduce a system-independent method to derive effective atomic C6 coefficients and polarizabilities in molecules and materials purely from charge population analysis. This enables the use of dispersion-correction schemes in electronic structure calculations without recourse to electrondensity partitioning schemes and expands their applicability to semi-empirical methods and tightbinding Hamiltonians. We then show that the accuracy of our method is en par with established electrondensity partitioning based approaches in describing intermolecular C6 coefficients as well as dispersion energies of weakly bound molecular dimers, organic crystals, and supramolecular complexes. We showcase the utility of our approach by incorporation of the recently developed many-body dispersion method [Tkatchenko et al., Phys. Rev. Lett. 108, 236402 (2012)] into the semi-empirical density functional tight-binding method and propose the latter as a viable technique to study hybrid organic-inorganic interfaces.},
doi = {10.1063/1.4947214},
journal = {Journal of Chemical Physics},
number = 15,
volume = 144,
place = {United States},
year = {2016},
month = {4}
}