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Journal Article

Effects of Coadsorbed Oxygen on the Infrared Driven Decomposition of N2O on isolated Rh5+ Clusters

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Harding,  Daniel J.
Molecular Physics, Fritz Haber Institute, Max Planck Society;

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Kerpal,  Christian
Molecular Physics, Fritz Haber Institute, Max Planck Society;

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Meijer,  Gerard
Molecular Physics, Fritz Haber Institute, Max Planck Society;

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Fielicke,  André
Molecular Physics, Fritz Haber Institute, Max Planck Society;

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Citation

Hermes, A. C., Hamilton, S. M., Hopkins, W. S., Harding, D. J., Kerpal, C., Meijer, G., et al. (2011). Effects of Coadsorbed Oxygen on the Infrared Driven Decomposition of N2O on isolated Rh5+ Clusters. The Journal of Physical Chemistry Letters, 2(24), 3053-3057. doi:10.1021/jz2012963.


Cite as: http://hdl.handle.net/11858/00-001M-0000-0012-3E60-2
Abstract
The thermally induced decomposition of nitrous oxide on isolated Rh5+ and Rh5O+ clusters has been investigated using mid-infrared multiple photon dissociation spectroscopy. The presence of a single co-adsorbed oxygen atom is observed to have a profound effect on the cluster surface processes which ensue following infrared heating of the cluster. Exciting the infrared active N2O bending transition in Rh5N2O+ results predominantly (≥ 85%) in molecular desorption of the N2O moiety whilst the same excitation in Rh5ON2O+ leads instead to N2O dissociation on the cluster surface producing Rh5O2+ (≥ 85%). Calculations of the reaction pathway using density functional theory indicate that the change in branching ratio arises from a 0.4 eV greater binding energy of N2O to Rh5O+ compared with Rh5+ taking the desorption threshold above the reaction barrier for the surface reaction channel whose energy is unchanged.