The kinetics and energetics of cloud droplet and aerosol formation in the atmosphere are strongly influenced by the evaporation and condensation rates of water, yet the magnitude and mechanism of evaporation remains incompletely characterized. Of particular import (and controversy) is the nature of interfacial water pH and its potential effects on evaporation rate and environmental reactivity. We have used Raman thermometry measurements of freely evaporating microdroplets to determine evaporation coefficients (Î) for two different hydrochloric acid solutions, both of which result in a significant deviation from Îwater. At 95% confidence, we find the evaporation coefficient for 1.0 M HCl to be 0.24 ± 0.04, a â-60% decrease relative to pure water, and for 0.1 M HCl to be 0.91 ± 0.08, a â-45% increase relative to pure water. These results suggest a large perturbation in the surface structure induced by either hydronium ions adsorbing to the water surface or by the presence of a Cl-···H3O+ ion-pair moiety in the interfacial region.