The area of in situ spectroscopy at quasi-perfect Pt(111) single-crystal facet|aqueous electrolyte interfaces is herein reviewed. Illustrations are provided of the simultaneous application of differential reflectance spectroscopy and second-harmonic generation as static and dynamic probes of ionic and molecular adsorbates. Attention is focused on quantitative studies of bisulfate adsorption as well as of the dynamics of phase transitions and reactivity of carbon monoxide adlayers and their dependence on the applied potential. Also discussed are current limitations of these techniques, as well as possible means to improve their temporal and spatial resolution.
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