Atmos. Chem. Phys. Discuss., 12, 26503-26560, 2012
© Author(s) 2012. 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.
The size distribution and mixing state of black carbon aerosol over Europe
C. L. Reddington1, G. McMeeking2, G. W. Mann1, H. Coe3, M. G. Frontoso4, D. Liu3, M. Flynn3, D. V. Spracklen1, and K. S. Carslaw1
1Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, UK
2Department of Atmospheric Science, Colorado State University, Fort Collins, CO, USA
3School of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester, UK
4C2SM – ETH Zürich, Zürich, Switzerland

Abstract. Black carbon-containing aerosol particles play an important role in the direct and indirect radiative forcing of climate. However, the magnitude and sign of the net radiative effect is strongly dependent on the physical properties of the black carbon (BC) component of the particles, such as mass, number concentration and size distribution. Here we use a global aerosol model combined with aircraft measurements of BC particle number and size from the Single Particle Soot Photometer (SP2) to assess the realism with which these physical properties are predicted by global models. The comparison reveals a substantial mismatch between the measured and modelled BC size distribution over the size range of the SP2 instrument (90–400 nm BC diameter). The model predicts BC particle number concentrations a factor ~3.5–5.7 higher than measured and a mode diameter that is 40–65 nm smaller than observed. More than 90% of the model particles in the SP2 size range contain BC, while the observations suggest only 21%. These model-observation biases in the BC properties are considerably greater than for the overall particle distribution, suggesting that the discrepancy is associated with model assumptions about the size and mixing state of the emitted carbonaceous particles. We expect the discrepancy in BC size distribution to be common among most global aerosol models, with implications for model estimates of absorption optical depth and direct radiative forcing.

Citation: Reddington, C. L., McMeeking, G., Mann, G. W., Coe, H., Frontoso, M. G., Liu, D., Flynn, M., Spracklen, D. V., and Carslaw, K. S.: The size distribution and mixing state of black carbon aerosol over Europe, Atmos. Chem. Phys. Discuss., 12, 26503-26560, doi:10.5194/acpd-12-26503-2012, 2012.
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