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Multipole moments of water molecules in clusters and ice Ih from first principles calculations

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.479897· OSTI ID:686442
 [1];  [2];  [3]
  1. Department of Physics, Box 351560, University of Washington, Seattle, Washington 98195-1560 (United States)
  2. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, 906 Battelle Boulevard, PO Box 999, MS K8-91, Richland, Washington 99352 (United States)
  3. Department of Chemistry, Box 351700, University of Washington, Seattle, Washington 98195-1700 (United States)

We have calculated {ital molecular} multipole moments for water molecules in clusters and in ice Ih by partitioning the charge density obtained from first principles calculations. Various schemes for dividing the electronic charge density among the water molecules were used. They include Bader{close_quote}s zero flux surfaces and Voronoi partitioning schemes. A comparison was also made with an induction model including dipole, dipole-quadrupole, quadrupole-quadrupole polarizability and first hyperpolarizability as well as fixed octopole and hexadecapole moments. We have found that the different density partitioning schemes lead to widely different values for the molecular multipoles, illustrating how poorly defined molecular multipoles are in clusters and condensed environments. For instance, the magnitude of the molecular dipole moment in ice Ih ranges between 2.3 D and 3.1 D depending on the partitioning scheme used. Within each scheme, though, the value for the molecular dipole moment in ice is larger than in the hexamer. The magnitude of the molecular dipole moment in the clusters shows a monotonic increase from the gas phase value to the one in ice Ih, with the molecular dipole moment in the water ring hexamer being smaller than the one in ice Ih for all the partitioning schemes used. {copyright} {ital 1999 American Institute of Physics.}

OSTI ID:
686442
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 13 Vol. 111; ISSN JCPSA6; ISSN 0021-9606
Country of Publication:
United States
Language:
English

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