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Title: Combining molecular dynamics and ab initio quantum-chemistry to describe electron transfer reactions in electrochemical environments
Author: Domínguez-Ariza, David
Hartnig, Christoph
Sousa Romero, Carmen
Illas i Riera, Francesc
Keywords: Dinàmica molecular
Química quàntica
Molecular dynamics
Quantum chemistry
Issue Date: 24-Jun-2004
Publisher: American Institute of Physics
Abstract: A theoretical model is presented aimed to provide a detailed microscopic description of the electron transfer reaction in an electrochemical environment. The present approach is based on the well-known two state model extended by the novelty that the energy of the two states involved in the electron transfer reaction is computed quantum mechanically as a function of the solvent coordinate, as defined in the Marcus theory, and of the intensity of an external electric field. The solvent conformations defining the reaction coordinate are obtained from classical molecular dynamics and then transferred to the quantum mechanical model. The overall approach has been applied to the electron transfer between a chloride anion and a single crystal Cu(100) electrode. It is found that the solvent exerts a strong influence on the equilibrium geometry of the halide and hence on the relative energy of the two states involved in the electron transfer reaction. Finally, both solvent fluctuations and external field facilitate the electron transfer although solvent effects have a stronger influence.
Note: Reproducció del document publicat a:
It is part of: Journal of Chemical Physics, 2004, vol. 121, num. 2, p. 1066-1073
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ISSN: 0021-9606
Appears in Collections:Articles publicats en revistes (Ciència dels Materials i Química Física)

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