Abstract
A theoretical study of the vibrational relaxation of the adbond between a physisorbed molecule and a crystalline substrate is presented. The bond between the admolecule and the substrate is described as a one-dimensional Morse oscillator. Using standard perturbation theory, expressions for the relaxation of the vibrational adbond due to its interaction with the substrate lattice vibrations are derived. Both energy relaxation and pure dephasing are considered. A numerical evaluation of the resulting expressions for the relaxation constants is given for a Debye spectrum for the phonons and for a surface phonon spectrum. The relative importance of pure dephasing and energy relaxation in determining the absorption linewidth is derived as a function of the fundamental frequency of the active mode.
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