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Published Online September 16, 2004
Science DOI: 10.1126/science.1102792

Reports

Submitted on July 15, 2004
Accepted on August 20, 2004

How Do Small Water Clusters Bind an Excess Electron?

Nathan I. Hammer 1, Joong-Won Shin 1, Jeffrey M. Headrick 1, Eric G. Diken 1, Joseph R. Roscioli 1, Gary H. Weddle 1{dagger}, Mark A. Johnson 1*

1 Sterling Chemistry Laboratory, Yale University, Post Office Box 208107, New Haven, CT 06520, USA.

* To whom correspondence should be addressed.
Mark A. Johnson , E-mail: mark.johnson{at}yale.edu

{dagger}Present address: Department of Chemistry, Fairfield University, Fairfield, CT 06430, USA.

The arrangement of water molecules around a hydrated electron has eluded explanation for more than forty years. Here we report sharp vibrational bands for small gas phase water cluster anions, (H2O)4-6- and (D2O)4-6-. Analysis of these bands reveals a detailed picture of the diffuse electron binding site. The electron is closely associated with a single water molecule attached to the supporting network through a double H-bond acceptor motif. The local OH stretching bands of this molecule are dramatically distorted in the pentamer and smaller clusters because the excited vibrational 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 remarkably fast, with the symmetric stretching mode surviving for less than ten vibrational periods (50 fs in (H2O)4-).


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