Structural data about water at the air/water interface of sulfuric acid solutions have been obtained with sum frequency generation spectroscopy. Sulfuric acid significantly affects the orientation of water at the interface. With as little as 0.01 x (mole fraction) sulfuric acid, water is more highly oriented compared with the pure water surface. Surface water with one hydrogen free of hydrogen bonding, a “free OH”, decreases in concentration as the sulfuric acid concentration is increased. Finally, there are no sulfuric acid free OH groups projecting out of the surface for solutions from 0.01 x to 0.9 x sulfuric acid. Observations of the structure of water are consistent with the fact that sulfuric acid/water solutions change from ionic in nature at low concentrations (<0.01 x ) to ion pair complexes/hydrates at high concentrations (>0.4 x ).
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Baldelli et al. (1997) studied this question.
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