Atmos. Chem. Phys. Discuss., 10, 27695-27723, 2010
www.atmos-chem-phys-discuss.net/10/27695/2010/
doi:10.5194/acpd-10-27695-2010
© Author(s) 2010. This work is distributed
under the Creative Commons Attribution 3.0 License.
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Sensitivity of global cloud condensation nuclei concentrations to primary sulfate emissions parameterizations
G. Luo and F. Yu
Atmospheric Sciences Research Center, State University of New York, 251 Fuller Road, Albany, New York 12203, USA

Abstract. The impact of primary sulfate emissions on cloud condensation nuclei (CCN) concentrations, one of the major uncertainties in global CCN predictions, depends on the fraction of sulfur mass emitted as primary sulfate particles (fsulfate), the fraction of primary sulfate mass distributed into the nucleation mode particles (fnucl), and the nucleation and growth process in the ambient atmosphere. Here, we use a global size-resolved aerosol microphysics model recently developed to study how the different parameterizations of primary sulfate emission affect particle properties and CCN abundance. Different from previous studies, we use the ion-mediated nucleation scheme to calculate tropospheric particle formation and explicitly simulate the condensation of low volatile secondary organic gas (in addition to H2SO4 gas) on nucleated particles. Our simulations show a compensation effect of nucleation to primary sulfate emission. We find that the change of fnucl from 5% to 15% has a more significant impact on the simulated particle number budget than that of fsulfate within the range of 2.5–5%. An increase of fsulfate from 0% to 2.5% (with fnucl = 5%) does not improve the agreement between simulated and observed annual mean number concentrations of particles >10 nm at 21 stations but further increase of either fsulfate from 2.5% to 5% (with fnucl = 5%) or fnucl from 5% to 15% (with fsulfate = 2.5%) substantially deteriorates the agreement. For fsulfate of 2.5%–5% and fnucl of 5%, our simulations indicate that the global CCN at supersaturation of 0.2 increases by 8–11% in the boundary layer and 3–5% in the whole troposphere (compared to the case with fsulfate = 0). Our derived impact of primary sulfate emission on global CCN abundance is about a factor of ∼3–7 smaller than those found in previous studies.

Citation: Luo, G. and Yu, F.: Sensitivity of global cloud condensation nuclei concentrations to primary sulfate emissions parameterizations, Atmos. Chem. Phys. Discuss., 10, 27695-27723, doi:10.5194/acpd-10-27695-2010, 2010.
 
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