Abstract
The study of the relaxation of internalstretch vibrations of diatomics at metal surfaces has been an area of intense interest. Using ultrafast laser techniques, several groups1,2 have recently performed elegant vibrational-relaxation measurements that reveal short (of the order of 1 ps) T, lifetimes. This strong coupling has been attributed to excitation of electron-hole pairs in the substrate. We present here the results of a reverse vibrational-relaxation experiment. Rather than excite the adsorbate internal mode and time-resolve the decay of the vibrational energy due to damping, we create high transient electronic temperatures and measure the flow of energy to the adsorbate vibration through the vibrational distributions of molecules that desorb. This experiment provides a direct demonstration of the strong coupling between electrons and the adsorbate vibrational excitation.
© 1993 Optical Society of America
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