How Well Does Water Activity Determine Homogeneous Ice Nucleation Temperature in Aqueous Sulfuric Acid and Ammonium Sulfate Droplets?

Abstract

Frozen fraction measurements made using a droplet free-fall freezing tube apparatus are presented and used, along with other recent laboratory measurements, to evaluate how well both the water activity idea and the translated melting-point curve idea of Koop et al. predict homogeneous freezing-point temperatures for aqueous ammonium sulfate and sulfuric acid solution droplets. The new freezing-point temperature datasets agree with the previous lowest-temperature results for both solutes. The lowest measured freezing-point temperatures for aqueous ammonium sulfate solutions agree with a curve shaped like the translated melting-point curve. However, those for aqueous sulfuric acid solutions are significantly lower than predicted by the translated melting-point curve idea, and a single water activity freezing-point temperature curve does not represent the lowest-temperature freezing-point temperature data for both solutes. A linear extrapolation of the new aqueous sulfuric acid solution freezing data to low temperatures predicts that high critical supersaturations in cloud-free regions of the upper troposphere will occur when homogeneous ice nucleation in an aqueous sulfuric acid aerosol is the primary ice formation mechanism.