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Ab initio molecular dynamics simulation of a medium-sized water cluster anion: From an interior to a surface-located excess electron via a delocalized state


Frigato, T; VandeVondele, J; Schmidt, B; Schuette, C; Jungwirth, P (2008). Ab initio molecular dynamics simulation of a medium-sized water cluster anion: From an interior to a surface-located excess electron via a delocalized state. Journal of Physical Chemistry. A, 112(27):6125-6133.

Abstract

We present a computational study of the structure and dynamics of an excess electron in a medium-sized water cluster aimed at addressing the question of interior vs exterior solvation. Ab initio Born - Oppenheimer molecular dynamics simulations were performed within the DFT framework, employing a hybrid Gaussian and plane-wave formalism together with the PBE exchange-correlation functional and norm-conserving pseudopotentials. Analysis of a 15-ps trajectory allowed us to reach the following conclusions: (i) the excess electron is predominantly located at the cluster surface (even if it is initially placed in the interior), (ii) the computed electron binding energies correlate with the electron localization rather than with its bulk vs surface location, and (iii) a dynamical interconversion between two different H-bond patterns around the electron occurs. The computed electron binding energies and tile most relevant features of the IR spectrum are in a very good agreement with results of previous experimental studies.

We present a computational study of the structure and dynamics of an excess electron in a medium-sized water cluster aimed at addressing the question of interior vs exterior solvation. Ab initio Born - Oppenheimer molecular dynamics simulations were performed within the DFT framework, employing a hybrid Gaussian and plane-wave formalism together with the PBE exchange-correlation functional and norm-conserving pseudopotentials. Analysis of a 15-ps trajectory allowed us to reach the following conclusions: (i) the excess electron is predominantly located at the cluster surface (even if it is initially placed in the interior), (ii) the computed electron binding energies correlate with the electron localization rather than with its bulk vs surface location, and (iii) a dynamical interconversion between two different H-bond patterns around the electron occurs. The computed electron binding energies and tile most relevant features of the IR spectrum are in a very good agreement with results of previous experimental studies.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Date:12 June 2008
Deposited On:20 Oct 2008 08:29
Last Modified:05 Apr 2016 12:27
Publisher:American Chemical Society
ISSN:1089-5639
Publisher DOI:10.1021/jp711545s
Permanent URL: http://doi.org/10.5167/uzh-3458

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