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Direct observation of vibrational energy delocalization on surfaces: CO on Ru(001)

We report the experimental observation of the gradual transition from a local oscillator to a two-dimensional delocalized phonon, observed for the CO-stretch vibration of carbon monoxide adsorbed on a Ru(001) surface by means of broadband-infrared saturation sum-frequency spectroscopy. The data are theoretically reproduced by an exchange model with residence times of the excitation down to 2.5 ps.