Activation Energies and Potentials of Mean Force for Water Cluster Evaporation
Activation energies for water cluster evaporation are of interest in many areas of chemical physics. We present the first computation of activation energies for small waters clusters using the formalism of Dynamical Nucleation Theory (DNT). To this end, individual evaporation rate constants are computed for water clusters (H2O)i, where i = 2 to 10 for temperatures ranging from 243 to 333K. These calculations employ a parallel sampling technique utilizing the Global Arrays Toolkit developed at PNNL. The resulting evaporation rate constants for each cluster are then fit to Arrhenius equations to obtain activation energies. We discuss DNT evaporation rate constants and their relation to potentials of mean force, activation energies, and how to account for non-separability of the reaction coordinate in the reactant state partition function. This work was supported by the PNNL Computational Science and Engineering LDRD Program and the Chemical and Material Sciences Division, Office of Basic Energy Sciences, Department of Energy. The Pacific Northwest National Laboratory is operated by Battelle for the US Department of Energy.
- Research Organization:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- AC05-76RL01830
- OSTI ID:
- 927278
- Report Number(s):
- PNNL-SA-56857; JCPSA6; KC0301020; TRN: US200811%%17
- Journal Information:
- Journal of Chemical Physics, 128(6):Art. No. 064306, Vol. 128, Issue 6; ISSN 0021-9606
- Country of Publication:
- United States
- Language:
- English
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