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How Do Small Water Clusters Bind an Excess Electron?
Nathan I. Hammer,Joong-Won Shin,Jeffrey M. Headrick,Eric G. Diken,Joseph R. Roscioli,Gary H. Weddle,*Mark A. Johnson
The arrangement of water molecules around a hydrated electronhas eluded explanation for more than 40 years. Here we reportsharp vibrational bands for small gas-phase water cluster anions,(H2O)4-6– and (D2O)4-6–. Analysis of these bandsreveals a detailed picture of the diffuse electron-binding site.The electron is closely associated with a single water moleculeattached to the supporting network through a double H-bond acceptormotif. The local OH stretching bands of this molecule are dramaticallydistorted in the pentamer and smaller clusters because the excitedvibrational levels are strongly coupled to the electron continuum.The vibration–to–electronic energy transfer rates,as revealed by line shape analysis, are mode-specific and remarkablyfast, with the symmetric stretching mode surviving for lessthan 10 vibrational periods [50 fs in (H2O)4–].
Sterling Chemistry Laboratory, Yale University, Post Office Box 208107, New Haven, CT 06520, USA.
* Present address: Department of Chemistry, Fairfield University,Fairfield, CT 06430, USA.
To whom correspondence should be addressed. E-mail: mark.johnson{at}yale.edu
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A. E. Bragg, J. R. R. Verlet, A. Kammrath, O. Cheshnovsky, and D. M. Neumark (22 October 2004) Science306 (5696), 669.
[DOI: 10.1126/science.1103527] |Abstract »|Full Text »|PDF »
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[DOI: 10.1126/science.1104678] |Summary »|Full Text »|PDF »
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[DOI: 10.1126/science.1102827] |Abstract »|Full Text »|PDF »
THIS ARTICLE HAS BEEN CITED BY OTHER ARTICLES:
First-principles, quantum-mechanical simulations of electron solvation by a water cluster.
To whom correspondence should be addressed. E-mail: 
