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Many-Body Dispersion in Molecular Clusters
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    Many-Body Dispersion in Molecular Clusters
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    • Melisa Alkan
      Melisa Alkan
      Department of Chemistry, Iowa State University, Ames, Iowa 50011, United States
      Ames Laboratory, Ames, Iowa 50011, United States
      More by Melisa Alkan
    • Peng Xu
      Peng Xu
      Department of Chemistry, Iowa State University, Ames, Iowa 50011, United States
      Ames Laboratory, Ames, Iowa 50011, United States
      More by Peng Xu
    • Mark S. Gordon*
      Mark S. Gordon
      Department of Chemistry, Iowa State University, Ames, Iowa 50011, United States
      Ames Laboratory, Ames, Iowa 50011, United States
      *(M.S.G.) E-mail: [email protected]
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    The Journal of Physical Chemistry A

    Cite this: J. Phys. Chem. A 2019, 123, 39, 8406–8416
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    https://doi.org/10.1021/acs.jpca.9b05977
    Published September 9, 2019
    Copyright © 2019 American Chemical Society

    Abstract

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    Many-body dispersion has gained considerable attention over the past decade, particularly for condensed phase systems. However, quantitatively accurate studies of many-body dispersion have only recently become feasible due to challenges in reliability and accuracy. Currently available methodologies for calculating many-body dispersion have been challenged, with recent evidence suggesting, for example, that dispersion-corrected density functional theory (DFT) schemes cannot consistently predict many-body dispersion accurately. This study evaluates many-body dispersion energies using a composite approach that employs singles and doubles coupled cluster theory with perturbative/noniterative triples, CCSD(T), combined with an extrapolation to the complete basis set (CBS) limit. The combined CCSD(T)/CBS approach is applied to Arn and (H2O)n, n = 3–10, clusters, and a new data set called S22(3), which includes trimers generated based on the S22 data set. In these systems, the many-body dispersion provides a very small contribution to the total interaction energy of all of the systems studied, generally 3% or less of the total interaction energy. Two-body dispersion is the dominant dispersion contribution and many-body dispersion contributes no more than 5.7% of the total dispersion energy, generally staying below 2%.

    Copyright © 2019 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpca.9b05977.

    • Cartesian coordinates of all of the structures studied in this work, support for choosing appropriate level of theory and basis set for geometry optimization, list of S22(3) trimers, a table of energy differences comparing the MP2-optimized structures with either HF-D3- or B3LYP-D3-optimized structures, and a figure showing nonequilibrium S22(3) structures (PDF)

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    This article is cited by 21 publications.

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    The Journal of Physical Chemistry A

    Cite this: J. Phys. Chem. A 2019, 123, 39, 8406–8416
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpca.9b05977
    Published September 9, 2019
    Copyright © 2019 American Chemical Society

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