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Journal Article

Optimizing Vibrational Population Transfer at Surfaces through Infrared Excitation

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Bonn, M., & Wolf, M. (2002). Optimizing Vibrational Population Transfer at Surfaces through Infrared Excitation. Bulletin of the Chemical Society of Japan, 75(5), 1005-1010. doi:10.1246/bcsj.75.1005.

Cite as: https://hdl.handle.net/21.11116/0000-000E-28BF-F
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 (IR) laser pulses. Broadband IR excitation leads to the transfer of a significant fraction of the CO molecules to their first (∼15%) and second (∼5%) vibrationally excited states. We reproduce the observed excited state spectra by solving the three-level Bloch equations and discuss possibilities to optimize the degree of localized vibrational excitation of a specific bond of surface molecules through IR excitation by tuning the pulse duration and central frequency.