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.
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Dates
Type | When |
---|---|
Created | 23 years, 1 month ago (July 26, 2002, 8:45 a.m.) |
Deposited | 1 year, 6 months ago (Feb. 7, 2024, 1:24 p.m.) |
Indexed | 1 month, 3 weeks ago (July 11, 2025, 6:24 a.m.) |
Issued | 23 years, 10 months ago (Oct. 22, 2001) |
Published | 23 years, 10 months ago (Oct. 22, 2001) |
Published Print | 23 years, 10 months ago (Oct. 22, 2001) |
@article{Bonn_2001, title={The dynamics of vibrational excitations on surfaces: CO on Ru(001)}, volume={115}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.1404986}, DOI={10.1063/1.1404986}, number={16}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Bonn, Mischa and Hess, Christian and Wolf, Martin}, year={2001}, month=oct, pages={7725–7735} }