Abstract
The textbook view of the liquid electrolyte surfaces as being devoid of ions have recently been challenged by molecular dynamics simulations, which predict a surface enhancement of highly polarizable anions. Here we present the first direct experimental verification of this prediction. Enhanced azide ( N 3 - ) concentrations were measured at the liquid surface by femtosecond second harmonic generation (SHG) experiments exploiting the charge-transfer-to-solvent (CTTS) resonance of N 3 - , yielding a surface excess free energy of −9.9 ± 0.3 kJ/mole. Such surface-enhanced concentrations of anions could have important consequences for the chemical reactions taking place on atmospheric aerosols and at the ocean-air interface.
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