We show that vibrational spectra of molecules chemisorbed on metal surfaces can be affected by anharmonicity much more than usually estimated if various vibrational coordinates are coupled by non-diagonal terms. The strong coverage dependence of the linewidth of the adsorbate-metal vibrations of CO adsorbed on Pt(111) can be attributed to the multiphonon decay, enhanced by a strong coupling of the adsorbate motion to the in-plane displacement of the surrounding surface atoms. © 1995.
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