Abstract

The lifetime broadening of the frustrated translation (T) mode parallel to the surface of isolated CO molecules [≲6% of a c(2×2) coverage] chemisorbed on Cu(001) has been studied with high resolution inelastic helium atom scattering as a function of the surface temperature and the parallel momentum transfer. The T excitation peak shows a temperature dependent peak shift and a broadening. The latter is attributed to a quartic anharmonic potential contribution described by a spectroscopic constant χe=−0.0085±0.0008. The extrapolated TS=0 K peak broadening is then γ0=85±5 μeV, corresponding to a vibrational lifetime τ=8±1 ps. We attribute this lifetime to substrate phonon mediated damping and electronic damping.

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