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Originally published in Science Express on 16 September 2004
Science 22 October 2004:
Vol. 306. no. 5696, pp. 669 - 671
DOI: 10.1126/science.1103527
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Reports

Hydrated Electron Dynamics: From Clusters to Bulk

A. E. Bragg,1 J. R. R. Verlet,1 A. Kammrath,1 O. Cheshnovsky,2 D. M. Neumark1,3*

The electronic relaxation dynamics of size-selected (H2O)n–/(D2O)n[25 ≤ n ≤ 50] clusters have been studied with time-resolved photoelectron imaging. The excess electron () was excited through the transition with an ultrafast laser pulse, with subsequent evolution of the excited state monitored with photodetachment and photoelectron imaging. All clusters exhibited p-state population decay with concomitant s-state repopulation (internal conversion) on time scales ranging from 180 to 130 femtoseconds for (H2O)n– and 400 to 225 femtoseconds for (D2O)n–; the lifetimes decrease with increasing cluster sizes. Our results support the "nonadiabatic relaxation" mechanism for the bulk hydrated electron (), which invokes a 50-femtosecond internal conversion lifetime.

1 Department of Chemistry, University of California, Berkeley, CA 94720, USA.
2 School of Chemistry, The Sackler Faculty of Exact Sciences, Tel-Aviv University, 69978 Israel.
3 Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.

* To whom correspondence should be addressed. E-mail: dan{at}radon.cchem.berkeley.edu

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