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By systematically changing the salt concentration and comparing HD-VSFG spectra with simulated spectra, we show that the formation of an EDL cannot account for the HD-VSFG spectra of the sodium halide salts and other electrolytes, the only exceptions among the considered electrolytes being HCl and NaClO 4 , for which the hydrated proton and the perchlorate have very high surface propensity

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