Evaluating the role of NAT, NAD, and liquid H2SO4/H2O/HNO3 solutions in Antarctic polar stratospheric cloud aerosol: Observations and implications

• Published in: Journal of Geophysical Research: Atmospheres 1997-06, Vol.102 (D11), p.13255-13282
• Main Authors: Del Negro, L. A., Fahey, D. W., Donnelly, S. G., Gao, R. S., Keim, E. R., Wamsley, R. C., Woodbridge, E. L., Dye, J. E., Baumgardner, D., Gandrud, B. W., Wilson, J. C., Jonsson, H. H., Loewenstein, M., Podolske, J. R., Webster, C. R., May, R. D., Worsnop, D. R., Tabazadeh, A., Tolbert, M. A., Kelly, K. K., Chan, K. R.
• Format: Article
• Language: English
• ISSN: 0148-0227; 2156-2202
• DOI: 10.1029/97JD00764

Airborne measurements of total reactive nitrogen (NOy) and polar stratospheric cloud (PSC) aerosol particles were made in the Antarctic (68°S) as part of the NASA Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft (ASHOE/MAES A) campaign in late July 1994. As found in both polar regions during previous studies, substantial PSC aerosol volume containing NOy was observed at temperatures above the frost point, confirming the presence of particles other than water ice. The composition of the aerosol particles is evaluated using equilibrium expressions for nitric acid trihydrate (NAT), nitric acid dihydrate (NAD), and the supercooled ternary solution (STS) composed of nitric acid (HNO3), sulfuric acid (H2SO4), and water (H2O). The equilibrium abundance of condensed HNO3 is calculated for each phase and compared to estimates made using observations of aerosol volume and NOy. The best agreement is found for STS composition, using criteria related to the onset and abundance of aerosol volume along the flight track. Throughout the PSC region, a comparison of the number of particles between 0.4 and 4.0 μm diameter with the number of available nuclei indicates that a significant fraction of the background aerosol number participates in PSC growth. Modeled STS size distributions at temperatures below 191 K compare favorably with measured size distributions of PSC aerosol. Calculations of the heterogeneous loss of chlorine nitrate (ClONO2) show that the reactivity of the observed PSC surface area is 30 to 300% greater with STS than with NAT composition for temperatures less than 195 K. The total volume of STS PSCs is shown to be more sensitive than NAT to increases in H2O, HNO3, and H2SO4 from supersonic aircraft fleet emissions. Using the current observations and perturbations predicted by the current aircraft assessments, an increase of 50 to 260% in STS aerosol volume is expected at the lowest observed temperatures (190 to 192 K), along with an extension of significant PSC activity to regions ∼0.7 K higher in temperature. These results improve our understanding of PSC aerosol formation in polar regions while strengthening the requirement to include STS aerosols in studies of polar ozone loss and the effects of aircraft emissions.