References

ACPD

Atmospheric Chemistry and Physics Discussions

ACPD

1680-7375

Copernicus GmbH

Göttingen, Germany

10.5194/acpd-11-24765-2011

Nucleation and growth of sulfate aerosol in coal-fired power plant plumes: sensitivity to background aerosol and meteorology

Stevens

R. G.

¹ Pierce

J. R.

¹ Brock

C. A.

² Reed

M. K.

³ Crawford

J. H.

⁴ Holloway

J. S.

² Ryerson

T. B.

² Huey

L. G.

⁵ Nowak

J. B.

² ⁶

Department of Physics and Atmospheric Science, Dalhousie University, Halifax, NS, Canada

NOAA Earth System Research Laboratory, Boulder, CO, USA

Tennessee Technological University, Cookeville, TN, USA

NASA Langley Research Center, Hampton, VA, USA

Department of Earth and Atmospheric Science, Georgia Institute of Technology, Atlanta, GA, USA

Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA

05 09 2011

11 9 24765 24812

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

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The full text article is available as a PDF file from http://www.atmos-chem-phys-discuss.net/11/24765/2011/acpd-11-24765-2011.pdf

New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulfur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10 s of kilometers and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this paper, we focus on sub-grid sulfate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. We have developed a modeling framework with aerosol microphysics in the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM). The model is evaluated against aircraft observations of new-particle formation in two different power-plant plumes and reproduces the major features of the observations. We show how the downwind plume aerosols can be greatly modified by both meteorological and background aerosol conditions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large pre-existing aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the amount of sunlight and NOx since both control OH concentrations. The results of this study highlight the importance for improved sub-grid particle formation schemes in regional and global aerosol models.

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