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Study of the stabilization energies of halide-water clusters: An application of first-principles interaction potentials based on a polarizable and flexible model

 

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dc.creator Ayala, Regla es
dc.creator Martínez Fernández, José Manuel es
dc.creator Pappalardo, Rafael R. es
dc.creator Sánchez Marcos, Enrique es
dc.date.accessioned 2016-10-28T10:19:53Z
dc.date.available 2016-10-28T10:19:53Z
dc.date.issued 2004
dc.identifier.citation Ayala, R., Martínez Fernández, J.M., Pappalardo, R.R. y Sánchez Marcos, E. (2004). Study of the stabilization energies of halide-water clusters: An application of first-principles interaction potentials based on a polarizable and flexible model. The Journal of chemical physics, 121 (15), 7269-7275.
dc.identifier.issn 0021-9606 es
dc.identifier.uri http://hdl.handle.net/11441/48329
dc.description.abstract The aim of this work is to compute the stabilization energy Estab(n) of [ X(H2O)n ]- (X=F, Br, and I for n=1 – 60) clusters from Monte Carlo simulations using first-principles ab initio potentials. Stabilization energy of [ X(H2O)n ]- clusters is defined as the difference between the vertical photodeachment energy of the cluster and the electron affinity of the isolated halide. On one hand, a study about the relation between cluster structure and the Estab(n) value, as well as the dependence of the latter with temperature is performed, on the other hand, a test on the reliability of our recently developed first-principles halide ion-water interaction potentials is carried out. Two different approximations were applied: (1) the Koopmans’ theorem and (2) calculation of the difference between the interaction energy of [ X(H2O)n ]- and [ X(H2O)n ] clusters using the same ab initio interaction potentials. The developed methodology allows for using the same interaction potentials in the case of the ionic and neutral clusters with the proviso that the charge of the halide anion was switched off in the latter. That is, no specific parametrization of the interaction potentials to fit the magnitude under study was done. The good agreement between our predicted Estab(n) and experimental data allows us to validate the first-principles interaction potentials developed elsewhere and used in this study, and supports the fact that this magnitude is mainly determined by electrostatic factors, which can be described by our interaction potentials. No relation between the value of Estab(n) and the structure of clusters has been found. The diversity of Estab(n) values found for different clusters with similar interaction energy indicates the need for statistical information to properly estimate the stabilization energy of the halide anions. The effect of temperature in the prediction of the Estab(n) is not significant as long as it was high enough to avoid cluster trapping into local equilibrium configurations which guarantees an appropriate sampling of the configurational space. Parallel tempering method was applied in particular cases to guarantee satisfactory sampling of clusters at low temperature es
dc.description.sponsorship Dirección General de Investigaciones Científicas y Técnicas BQU2002- 02217 es
dc.format application/pdf es
dc.language.iso eng es
dc.publisher American Institute of Physics (AIP) es
dc.relation.ispartof The Journal of chemical physics, 121 (15), 7269-7275.
dc.rights Attribution-NonCommercial-NoDerivatives 4.0 Internacional *
dc.rights Attribution-NonCommercial-NoDerivatives 4.0 Internacional *
dc.rights.uri http://creativecommons.org/licenses/by-nc-nd/4.0/ *
dc.title Study of the stabilization energies of halide-water clusters: An application of first-principles interaction potentials based on a polarizable and flexible model es
dc.type info:eu-repo/semantics/article es
dc.type.version info:eu-repo/semantics/publishedVersion es
dc.rights.accessrights info:eu-repo/semantics/openAccess es
dc.contributor.affiliation Universidad de Sevilla. Departamento de Química Física es
dc.relation.projectID BQU2002- 02217 es
dc.relation.publisherversion http://dx.doi.org/10.1063/1.1788660 es
dc.identifier.doi 10.1063/1.1788660 es
idus.format.extent 7 p. es
dc.journaltitle The Journal of chemical physics es
dc.publication.volumen 121 es
dc.publication.issue 15 es
dc.publication.initialPage 7269 es
dc.publication.endPage 7275 es
dc.identifier.idus https://idus.us.es/xmlui/handle/11441/48329
dc.contributor.funder Ministerio de Ciencia y Tecnología (MCYT). España
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