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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 (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.
