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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
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Volume 14, issue 24 | Copyright
Atmos. Chem. Phys., 14, 13661-13679, 2014
https://doi.org/10.5194/acp-14-13661-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 20 Dec 2014

Research article | 20 Dec 2014

The contribution of plume-scale nucleation to global and regional aerosol and CCN concentrations: evaluation and sensitivity to emissions changes

R. G. Stevens1,2 and J. R. Pierce1,2 R. G. Stevens and J. R. Pierce
  • 1Department of Physics and Atmospheric Science, Dalhousie University, Halifax, NS, Canada
  • 2Department of Atmospheric Science, Colorado State University, Fort Collins, CO, USA

Abstract. We implement the Predicting Particles Produced in Power-Plant Plumes (P6) sub-grid sulphate parameterization for the first time into a global chemical-transport model with online aerosol microphysics, the GEOS-Chem-TOMAS model. Compared to simulations using two other previous treatments of sub-grid sulphate, simulations using P6 sub-grid sulphate predicted similar or smaller increases (depending on other model assumptions) in globally, annually averaged concentrations of particles larger than 80 nm (N80). We test in simulations using P6 sub-grid sulphate the sensitivity of particle number concentrations to changes in SO2 or NOx emissions to represent recent emissions control changes. For global increases of 50% in emissions of either SO2 or NOx, or both SO2 and NOx, we find that globally, annually averaged N80 increase by 9.00, 1.47, or 10.24% respectively. However, both sub-grid and grid-resolved processes contribute to these changes. Finally, we compare the model results against observations of particle number concentrations. Compared with previous treatments of sub-grid sulphate, use of the P6 parameterization generally improves correlation with observed particle number concentrations. The P6 parameterization is able to resolve spatial heterogeneity in new-particle formation and growth that cannot be resolved by any constant assumptions about sub-grid sulphate. However, the differences in annually averaged aerosol size distributions due to the treatment of sub-grid sulphate at the measurement sites examined here are too small to unambiguously establish P6 as providing better agreement with observations.

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We implement a parameterization of sub-grid new-particle formation in sulfur-rich plumes (P6) for the first time into a global chemical-transport model with online aerosol microphysics. Compared with previous treatments of sub-grid particle formation, use of the P6 parameterization limits sub-grid particle formation in polluted or low-sunlight regions. We also test the sensitivity of sub-grid particle formation to changes in SO2 or NOx emissions due to emissions controls.
We implement a parameterization of sub-grid new-particle formation in sulfur-rich plumes (P6)...
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