Abstract
Measurement of the excitation-profile of the Raman scattering by an adsorbate on a smooth metal surface is a form of modulation spectroscopy which can provide information about the energies, widths and relative strengths of the valence electron excitations of the adsorbate-substrate complex that is formed, the underlying Raman scattering mechanisms, and the symmetry of the adsorbate-substrate complex, and about the deformations of the configuration coordinates in the excited state relative to the ground state. An overview is given of the electronic structure and electronic excitations of representative adsorbates on metal surfaces. The formulation of the various factors that determine the intensity of Raman scattering by adsorbates on smooth metals, and its dependence on the frequency of excitation, are discussed. The transition susceptibility for Raman scattering via two-step electronic excitation processes is formulated in terms of the nature of the electron level-vibration mode interaction. Finally, data on the Raman scattering excitation-profiles of crystal violet, malachite green and free-base phthalocyanine are presented as examples of the application of these ideas.
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