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Structure and bonding in ionized water clusters.

Hainam Do1, Nicholas A Besley

  • 1School of Chemistry, University of Nottingham, University Park, Nottingham, NG7 2RD, UK.

The Journal of Physical Chemistry. A
|June 7, 2013
PubMed
Summary
This summary is machine-generated.

Investigating ionized water clusters ((H2O)(n)(+), n=3-9) reveals proton transfer to H3O+ and OH radicals as the most stable structures. A novel hemibonded motif was observed in larger clusters.

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Area of Science:

  • Physical Chemistry
  • Computational Chemistry
  • Spectroscopy

Background:

  • Ionized water clusters are fundamental in atmospheric and solution chemistry.
  • Understanding their structure and bonding is crucial for various chemical processes.
  • Previous studies have explored smaller clusters, but larger systems present computational challenges.

Purpose of the Study:

  • To determine the stable structures and bonding configurations of ionized water clusters (H2O)(n)(+) for n = 3–9.
  • To investigate the role of proton transfer and radical formation in cluster stability.
  • To compare computational results with experimental infrared spectra.

Main Methods:

  • Basin hopping search algorithm for initial isomer generation.
  • Density functional theory (DFT) for preliminary calculations.
  • Second-order Møller–Plesset perturbation theory (MP2) and coupled cluster theory (e.g., CCSD(T)) for high-level energy refinement.
  • Infrared spectroscopy for comparison with experimental data.

Main Results:

  • The most stable isomers involve proton transfer, forming hydronium ions (H3O+) and hydroxyl radicals (OH).
  • These proton-transferred structures are more stable than those with hemibonded hydrazine-like fragments.
  • Calculated infrared spectra align well with experimental observations.
  • A new structural motif with a hemibonded OH radical was identified in (H2O)(9)(+).

Conclusions:

  • Proton transfer is a dominant stabilizing mechanism in ionized water clusters.
  • Computational methods accurately predict the structures and spectra of these systems.
  • The identified novel motif in larger clusters offers new insights into water cluster chemistry.