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Many-body dispersion effects in the binding of adsorbates on metal surfaces
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Maurer, Reinhard J., Ruiz, Victor G. and Tkatchenko, Alexandre (2015) Many-body dispersion effects in the binding of adsorbates on metal surfaces. Journal of Chemical Physics, 143 . 102808 . doi:10.1063/1.4922688
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Official URL: https://doi.org/10.1063/1.4922688
Abstract
A correct description of electronic exchange and correlation effects for molecules in contact with extended (metal) surfaces is a challenging task for first-principles modeling. In this work, we demonstrate the importance of collective van der Waals dispersion effects beyond the pairwise approximation for organic–inorganic systems on the example of atoms, molecules, and nanostructures adsorbed on metals. We use the recently developed many-body dispersion (MBD) approach in the context of density-functional theory [Tkatchenko et al., Phys. Rev. Lett. 108, 236402 (2012) and Ambrosetti et al., J. Chem. Phys. 140, 18A508 (2014)] and assess its ability to correctly describe the binding of adsorbates on metal surfaces. We briefly review the MBD method and highlight its similarities to quantum-chemical approaches to electron correlation in a quasiparticle picture. In particular, we study the binding properties of xenon, 3,4,9,10-perylene-tetracarboxylic acid, and a graphene sheet adsorbed on the Ag(111) surface. Accounting for MBD effects, we are able to describe changes in the anisotropic polarizability tensor, improve the description of adsorbate vibrations, and correctly capture the adsorbate–surface interaction screening. Comparison to other methods and experiment reveals that inclusion of MBD effects improves adsorption energies and geometries, by reducing the overbinding typically found in pairwise additive dispersion-correction approaches.
| Item Type: | Journal Article | |||||||||
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| Subjects: | Q Science > QD Chemistry | |||||||||
| Divisions: | Faculty of Science > Chemistry | |||||||||
| Library of Congress Subject Headings (LCSH): | Metals -- Surfaces, Adsorption, Xenon, Graphene | |||||||||
| Journal or Publication Title: | Journal of Chemical Physics | |||||||||
| Publisher: | American Institute of Physics | |||||||||
| ISSN: | 0021-9606 | |||||||||
| Official Date: | June 2015 | |||||||||
| Dates: |
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| Date of first compliant deposit: | 6 December 2017 | |||||||||
| Volume: | 143 | |||||||||
| Article Number: | 102808 | |||||||||
| DOI: | 10.1063/1.4922688 | |||||||||
| Status: | Peer Reviewed | |||||||||
| Publication Status: | Published | |||||||||
| Access rights to Published version: | Restricted or Subscription Access | |||||||||
| Funder: | European Research Council (ERC), United States. Department of Energy. Office of Basic Energy Sciences (OBES) | |||||||||
| RIOXX Funder/Project Grant: |
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