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The dynamics of vibrational excitations on surfaces: CO on Ru(001)

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Bonn,  Mischa
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Hess,  Christian
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Wolf,  Martin
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Bonn, M., Hess, C., & Wolf, M. (2001). The dynamics of vibrational excitations on surfaces: CO on Ru(001). Journal of Chemical Physics, 115(16), 7725-7735. doi:10.1063/1.1404986.


Cite as: http://hdl.handle.net/11858/00-001M-0000-0011-174C-4
Abstract
We present an experimental and theoretical study of vibrational excitation of the C–O stretch vibration of carbon monoxide adsorbed on a ruthenium Ru(001) surface with ultrashort femtosecond infrared laser pulses. After broadband excitation leading to transfer of a significant fraction of the CO molecules to their first (~15%) and second (~5%) vibrationally excited states, we observe a competition between vibrational energy relaxation and energy delocalization through dipole–dipole coupling. We reproduce the observed excited state spectra by solving the three-level Bloch equations and accounting for intermolecular vibrational energy transfer on a picosecond time scale. The rate of vibrational energy transfer, and its coverage-dependence, can be described by a Förster energy transfer mechanism. We discuss possibilities to optimize the degree of localized vibrational excitation of a specific bond of molecules at surfaces through chirped pulse IR excitation.