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A. E. Bragg,1J. R. R. Verlet,1A. Kammrath,1O. Cheshnovsky,2D. M. Neumark1,3*
The electronic relaxation dynamics of size-selected (H2O)n–/(D2O)n[25n 50] clusters have been studied with time-resolved photoelectronimaging. The excess electron () was excited through the transition with an ultrafast laser pulse, with subsequent evolution of the excited statemonitored with photodetachment and photoelectron imaging. Allclusters exhibited p-state population decay with concomitants-state repopulation (internal conversion) on time scales rangingfrom 180 to 130 femtoseconds for (H2O)n– and 400 to 225femtoseconds for (D2O)n–; the lifetimes decrease withincreasing cluster sizes. Our results support the "nonadiabaticrelaxation" 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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First-principles, quantum-mechanical simulations of electron solvation by a water cluster.
n 
) 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. 
