The changes of the nonlinear optical response by single atoms adsorbed on free-electron-like metal surfaces are calculated in the low-frequency limit. Density-functional theory and an extension of the atom+jellium chemisorption model by Lang and Williams allowing for the presence of an external static field is used. The results enable a detailed discussion of the mechanisms responsible for the characteristic effects of adsorbates on second-harmonic generation as evident from recent experiments on metal surfaces.
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Kuchler et al. (1993) studied this question.
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