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Science 9 November 2001:
Vol. 294. no. 5545, pp. 1322 - 1325
DOI: 10.1126/science.1064916
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Reports

Bulk-Like Features in the Photoemission Spectra of Hydrated Doubly Charged Anion Clusters

Xue-Bin Wang,12 Xin Yang,12 John B. Nicholas,3 Lai-Sheng Wang12*

We produced gaseous hydrated clusters of sulfate and oxalate anions [SO42--(H2O)n and C2O42-(H2O)n, where n = 4 to 40]. Photoelectron spectra of these clusters revealed that the solute dianions were in the center of the water cluster, (H2O)n. For small clusters, these spectra were characteristic of the respective solutes, but beyond the first solvation shell (n approx  12), features in the spectra from the solutes were diminished and a new feature from ionization of water emerged, analogous to bulk aqueous solutions. For large clusters with dimensions greater than 1 nanometer, the solute photoemission features disappeared and the spectra were dominated by the ionization of water as the solvent coverage increased. A smooth transition from gas-phase clusters to behavior of electrolyte solutions was clearly revealed, and the large solvated clusters can be used as molecular models to investigate the photophysics and chemistry of aqueous electrolyte solutions.

1 Department of Physics, Washington State University, 2710 University Drive, Richland, WA 99352, USA.
2 W. R. Wiley Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Mail Stop K8-88, Post Office Box 999, Richland, WA 99352, USA.
3 Genentech Inc., 1 DNA Way, South San Francisco, CA 94080, USA.
*   To whom correspondence should be addressed. E-mail: ls.wang{at}pnl.gov

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THIS ARTICLE HAS BEEN CITED BY OTHER ARTICLES:
Partitioning of atmospherically relevant ions between bulk water and the water/vapor interface.
L. M. Pegram and M. T. Record Jr. (2006)
PNAS 103, 14278-14281
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