Particle size distributions in Arctic polar stratospheric clouds, growth and freezing of sulfuric acid droplets, and implications for cloud formation

Abstract

Particle size and volume measurements obtained with the forward scattering spectrometer probe (FSSP), model 300 during January and February 1989 in the Airborne Arctic Stratospheric Experiment are presented and used to study processes important in the formation and growth of polar stratospheric cloud (PSC) particles. Comparisons of the observations with expected sulfuric acid droplet deliquescence suggest that in the Arctic a major fraction of the sulfuric acid droplets remain liquid until temperatures at least as low as 193 K. Arguments are presented to suggest that homogeneous freezing of the sulfuric acid droplets might occur near 190 K and might play a role in the formation of PSCs. The first suggestion of nitric acid trihydrate (NAT) particles appears near saturation ratios of HNO3 with respect to NAT of 1 (about 195 K) as an enhancement, of the large particles on the tail of the sulfuric acid droplet size distribution. The major increases in number and volume indicative of the main body of the NAT cloud are not seen in these Arctic investigations until 191 to 192 K, which corresponds to an apparent saturation ratio of HNO3 with respect to NAT of about 10, unlike the Antarctic where clouds were encountered at saturation ratios near 1. A decrease in the number of particles was observed in regions in which the airmass was denitrified, i.e. NOy, the sum of all reactive nitrogen species, was reduced. This was especially true for the larger particles on the upper tail of the sulfate size distribution. The loss of these largest particles supports the idea that denitrification may be the result of the preferential nucleation and growth of NAT on only the largest sulfate particles, which then sediment out of the airmass.