We report the first azimuthally resolved measurements of the effect of an adsorbed gas on optical second-harmonic generation (SHG) from a clean, well-ordered metal surface. The second-harmonic intensity from Ni(111) decreases rapidly upon hydrogen adsorption; however, the threefold symmetry with sample rotation about the surface normal is retained. The β₁ and β₂ adsorption states are clearly resolved and their contributions to the second-order susceptibility are determined. For this system, SHG is highly sensitive to local site symmetry and little affected by long-range ordering of adsorbates.
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Anderson et al. (1988) studied this question.
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