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Ion specific outcomes at aqueous interfaces remain among the most enigmatic phenomena in interfacial chemistry. Here, charged fused silica/water interfaces have been probed by homodyne- and heterodyne-detected (HD) second harmonic generation (SHG) spectroscopy at pH 7 and 5.8 and for concentrations of LiCl, NaCl, NaBr, NaI, KCl, RbCl, and CsCl ranging from tens of micromolar to several hundred millimolar. For ionic strengths around 0.1-1 mM, SHG intensities increase reversibly by up to 15% compared to the condition of zero added salt because of optical phase matching and the electrical double layer. For ionic strengths above 1 mM, use of any combination of cations and anions produces decreases in SHG response by as much as 50%, trending with ion softness when compared to the condition of zero added salt. Gouy-Chapman model fits to homodyned SHG intensities for the alkali halides studied here show that charge densities increase significantly with decreasing cation size. HD-SHG measurements indicate diffuse layer properties probed by the SHG process are invariant with ion identity, while Stern layer properties, as reported by χ (2) , are subject to ion specificity for the ions surveyed in this work in the order of χ RbCl  (2) = 1 / 2 χ NaCl  (2) = 1 / 4 χ NaI  (2) .

Specifics about Specific Ion Adsorption from Heterodyne-Detected Second Harmonic Generation