Atmospheric Chemistry and Physics, vol. 11, issue 17 (2011) pp. 9303-9322
Using a three-dimensional general circulation model with sulfur chemistry and sectional aerosol microphysics (WACCM/CARMA), we studied aerosol formation and microphysics in the upper troposphere and lower stratosphere (UTLS) as well as the middle and upper stratosphere based on three nucleation schemes (two binary homogeneous schemes and an ion-mediated scheme related to one of the binary schemes). Simulations suggest that ion-mediated nucleation rates in the UTLS are 25% higher than its related binary scheme, but that the rates predicted by the two binary schemes vary by two orders of magnitude. None of the nucleation schemes is superior at matching the limited observations available at the smallest sizes. However, it is found that coagulation, not nucleation, controls number concentration at sizes greater than approximately 10 nm. Therefore, based on this study, processes relevant to atmospheric chemistry and radiative forcing in the UTLS are not sensitive to the choice of nucleation schemes. The dominance of coagulation over other microphysical processes in the UTLS is consistent with other recent work using microphysical models. Simulations using all three nucleation schemes compare reasonably well to observations of size distributions, number concentration across latitude, and vertical profiles of particle mixing ratio in the UTLS. Interestingly, we find that we need to include Van der Waals forces in our coagulation scheme to match the UTLS aerosol concentrations. We conclude that this model can reasonably represent sulfate microphysical processes in the UTLS, and that the properties of particles at atmospherically relevant sizes appear to be insensitive to the details of the nucleation scheme. We also suggest that micrometeorites, which are not included in this model, dominate the aerosol properties in the upper stratosphere above about 30 km.
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