AAAR 32nd Annual Conference
September 30 - October 4, 2013
Oregon Convention Center
Portland, Oregon, USA
Abstract View
Weak Global Sensitivity of Cloud Condensation Nuclei and the Aerosol Indirect Effect to Criegee+SO2 Chemistry
JEFFREY PIERCE, Mat Evans, Catherine Scott, Stephen D'Andrea, Delphine Farmer, Erik Swietlicki, Dominick Spracklen, Colorado State University
Abstract Number: 41 Working Group: Aerosols, Clouds, and Climate
Abstract H2SO4 vapor is important for the nucleation of atmospheric aerosols and the growth of ultrafine particles to cloud condensation nuclei (CCN) sizes with important roles in the global aerosol budget and hence planetary radiative forcing. Recent studies have found that reactions of stabilized Criegee intermediates (CIs, formed from the ozonolysis of alkenes) with SO2 may be an important source of H2SO4 that has been missing from atmospheric aerosol models. We investigate the impact of this new source of H2SO4 in the atmosphere. We use the chemical transport model, GEOS-Chem, with the online aerosol microphysics module, TOMAS, to estimate the possible impact of CIs on present-day H2SO4, CCN, and the cloud-albedo aerosol indirect effect (AIE). We extend the standard GEOS-Chem chemistry with CI-forming reactions from the Master Chemical Mechanism. H2SO4 concentrations increase by over 100% in forested tropical boundary layers and by over 10-25% in forested NH boundary layers (up to 100% in July) due to CI+SO2 chemistry, but the change is generally negligible elsewhere. The predicted changed in CCN were strongly dampened to the CI+SO2 changes in H2SO4 in these regions: less than 15% in tropical forests and less than 2% in most mid-latitude locations. The global-mean CCN change was less than 1% both in the boundary layer and the free troposphere. The associated cloud-albedo AIE change was less than 0.03 W/m^2. The model global sensitivity of CCN and the AIE to CI+SO2 chemistry is significantly (approximately one order-of-magnitude) smaller than the sensitivity of CCN and AIE to other uncertain model inputs, such as nucleation mechanisms, primary emissions, SOA and deposition. We conclude that improvement in the modeled CI+SO2 chemistry would not likely to lead to significant improvements in present-day CCN and AIE predictions.