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Science 5 August 2005:
Vol. 309. no. 5736, pp. 914 - 917
DOI: 10.1126/science.1115808
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Reports

Characterization of Excess Electrons in Water-Cluster Anions by Quantum Simulations

László Turi,1 Wen-Shyan Sheu,2 Peter J. Rossky3*

Water-cluster anions can serve as a bridge to understand the transition from gaseous species to the bulk hydrated electron. However, debate continues regarding how the excess electron is bound in Formula, as an interior, bulklike, or surface electronic state. To address the uncertainty, the properties of Formula clusters with 20 to 200 water molecules have been evaluated by mixed quantum-classical simulations. The theory reproduces every observed energetic, spectral, and structural trend with cluster size that is seen in experimental photoelectron and optical absorption spectra. More important, surface states and interior states each manifest a characteristic signature in the simulation data. The results strongly support assignment of surface-bound electronic states to the water-cluster anions in published experimental studies thus far.

1 Eötvös Loránd University, Department of Physical Chemistry, Budapest 112, Post Office Box 32, H-1518, Hungary.
2 Department of Chemistry, Fu-Jen Catholic University, Taipei, Taiwan 242, ROC.
3 Department of Chemistry and Biochemistry, Institute for Theoretical Chemistry, University of Texas at Austin, Austin, TX 78712–1167, USA.

* To whom correspondence should be addressed. E-mail: rossky{at}mail.utexas.edu

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THIS ARTICLE HAS BEEN CITED BY OTHER ARTICLES:
Mass Spectrometry Special Feature: Nanocalorimetry in mass spectrometry: A route to understanding ion and electron solvation.
W. A. Donald, R. D. Leib, J. T. O'Brien, A. I. S. Holm, and E. R. Williams (2008)
PNAS 105, 18102-18107
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First-principles, quantum-mechanical simulations of electron solvation by a water cluster.
J. M. Herbert and M. Head-Gordon (2006)
PNAS 103, 14282-14287
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Cluster Chemistry And Dynamics Special Feature: Clusters: A bridge across the disciplines of physics and chemistry..
P. Jena and A. W. Castleman Jr. (2006)
PNAS 103, 10560-10569
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Corrections and Clarifications.
(2005)
Science 310, 1769
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Comment on "Characterization of Excess Electrons in Water-Cluster Anions by Quantum Simulations".
J. R. R. Verlet, A. E. Bragg, A. Kammrath, O. Cheshnovsky, and D. M. Neumark (2005)
Science 310, 1769b
   Abstract »    Full Text »    PDF »
Response to Comment on "Characterization of Excess Electrons in Water-Cluster Anions by Quantum Simulations".
L. Turi, W.-S. Sheu, and P. J. Rossky (2005)
Science 310, 1769c
   Abstract »    Full Text »    PDF »


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