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Volume 16, issue 12 | Copyright
Atmos. Chem. Phys., 16, 7709-7724, 2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 24 Jun 2016

Research article | 24 Jun 2016

The evolution of biomass-burning aerosol size distributions due to coagulation: dependence on fire and meteorological details and parameterization

Kimiko M. Sakamoto1, James R. Laing2, Robin G. Stevens3, Daniel A. Jaffe2,4, and Jeffrey R. Pierce1,5 Kimiko M. Sakamoto et al.
  • 1Department of Atmospheric Science, Colorado State University, Fort Collins, CO, USA
  • 2School of Science and Technology, University of Washington-Bothell, Bothell, WA, USA
  • 3School of Earth and Environment, University of Leeds, Leeds, UK
  • 4Department of Atmospheric Science, University of Washington, Seattle, WA, USA
  • 5Department of Physics and Atmospheric Science, Dalhousie University, Halifax, NS, Canada

Abstract. Biomass-burning aerosols have a significant effect on global and regional aerosol climate forcings. To model the magnitude of these effects accurately requires knowledge of the size distribution of the emitted and evolving aerosol particles. Current biomass-burning inventories do not include size distributions, and global and regional models generally assume a fixed size distribution from all biomass-burning emissions. However, biomass-burning size distributions evolve in the plume due to coagulation and net organic aerosol (OA) evaporation or formation, and the plume processes occur on spacial scales smaller than global/regional-model grid boxes. The extent of this size-distribution evolution is dependent on a variety of factors relating to the emission source and atmospheric conditions. Therefore, accurately accounting for biomass-burning aerosol size in global models requires an effective aerosol size distribution that accounts for this sub-grid evolution and can be derived from available emission-inventory and meteorological parameters.

In this paper, we perform a detailed investigation of the effects of coagulation on the aerosol size distribution in biomass-burning plumes. We compare the effect of coagulation to that of OA evaporation and formation. We develop coagulation-only parameterizations for effective biomass-burning size distributions using the SAM-TOMAS large-eddy simulation plume model. For the most-sophisticated parameterization, we use the Gaussian Emulation Machine for Sensitivity Analysis (GEM-SA) to build a parameterization of the aged size distribution based on the SAM-TOMAS output and seven inputs: emission median dry diameter, emission distribution modal width, mass emissions flux, fire area, mean boundary-layer wind speed, plume mixing depth, and time/distance since emission. This parameterization was tested against an independent set of SAM-TOMAS simulations and yields R2 values of 0.83 and 0.89 for Dpm and modal width, respectively. The size distribution is particularly sensitive to the mass emissions flux, fire area, wind speed, and time, and we provide simplified fits of the aged size distribution to just these input variables. The simplified fits were tested against 11 aged biomass-burning size distributions observed at the Mt. Bachelor Observatory in August 2015. The simple fits captured over half of the variability in observed Dpm and modal width even though the freshly emitted Dpm and modal widths were unknown. These fits may be used in global and regional aerosol models. Finally, we show that coagulation generally leads to greater changes in the particle size distribution than OA evaporation/formation does, using estimates of OA production/loss from the literature.

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We determine how various meteorological and fire factors contribute to shaping the aged biomass-burning particle size distribution through coagulation. The mass emissions flux, fire area, and wind speed are dominant factors controlling the aged size distribution. We parameterize the aged size distribution for global/regional aerosol models. We estimate that the aged biomass-burning particle size distribution may be more sensitive to variability in coagulation than SOA formation.
We determine how various meteorological and fire factors contribute to shaping the aged...