Response of Observables for Cold Anionic Water Clusters to Cluster Thermal History

Madarász, Ádám and Rossky, Peter and Turi, László (2010) Response of Observables for Cold Anionic Water Clusters to Cluster Thermal History. Journal of Physical Chemistry A, 114 (6). pp. 2331-2337. ISSN 1520-5215

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Abstract

We have used mixed quantum-classical molecular dynamics simulations to explore the role of structural relaxation when binding an excess electron to neutral water clusters. The structural and spectral properties of the water cluster anions were investigated as a function of the size (n=45 and 104), nominal temperature (Tnom=50, 100 and 150 K) and the preparation method of the parent neutral clusters. In particular, we consider two different protocols for preparing the initial neutral clusters, which differ markedly in their thermal history. In the first, warm equilibrium neutral clusters are gradually quenched to increasingly lower temperature. In the second, neutral clusters are formed spontaneously at ~0 K and then warmed to the same target temperatures, yielding inherently metastable, non-equilibrium structures. Electron attachment to these alternative sets of clusters shows that below a critical temperature (~200K), the metastable water clusters bind a surface state excess electron significantly more strongly than the quenched, equilibrium clusters. The structural analysis indicates that these cluster anions with larger vertical detachment energies (VDE) more frequently stabilize the electron by double acceptor-type water molecules, and exhibit a weak temperature dependence of the VDE, compared to the quenched clusters. These results suggest that the alternative classes of cluster anions seen experimentally may reflect differences in thermal history of such clusters.

Item Type:	Article
Subjects:	Q Science / természettudomány > QD Chemistry / kémia > QD02 Physical chemistry / fizikai kémia
Depositing User:	Dr. Túri László
Date Deposited:	28 Jan 2013 13:47
Last Modified:	01 Mar 2013 12:46
URI:	http://real.mtak.hu/id/eprint/4032

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• Response of Observables for Cold Anionic Water Clusters to Cluster Thermal History. (deposited 13 Apr 2012 18:03)
  • Response of Observables for Cold Anionic Water Clusters to Cluster Thermal History. (deposited 28 Jan 2013 13:47) [Currently Displayed]

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