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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
Atmos. Chem. Phys., 17, 3605-3617, 2017
https://doi.org/10.5194/acp-17-3605-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
Research article
14 Mar 2017
Composition, size and cloud condensation nuclei activity of biomass burning aerosol from northern Australian savannah fires
Marc D. Mallet1, Luke T. Cravigan1, Andelija Milic1, Joel Alroe1, Zoran D. Ristovski1, Jason Ward2, Melita Keywood2, Leah R. Williams3, Paul Selleck2, and Branka Miljevic1 1School of Chemistry, Physics and Mechanical Engineering, Queensland University of Technology, Queensland, Brisbane, 4001, Australia
2CSIRO Oceans and Atmosphere Flagship, Aspendale, Victoria, 3195, Australia
3Aerodyne Research, Inc., Billerica, Massachusetts, 01821, USA
Abstract. The vast majority of Australia's fires occur in the tropical north of the continent during the dry season. These fires are a significant source of aerosol and cloud condensation nuclei (CCN) in the region, providing a unique opportunity to investigate the biomass burning aerosol (BBA) in the absence of other sources. CCN concentrations at 0.5 % supersaturation and aerosol size and chemical properties were measured at the Australian Tropical Atmospheric Research Station (ATARS) during June 2014. CCN concentrations reached over 104 cm−3 when frequent and close fires were burning – up to 45 times higher than periods with no fires. Both the size distribution and composition of BBA appeared to significantly influence CCN concentrations. A distinct diurnal trend in the proportion of BBA activating to cloud droplets was observed, with an activation ratio of 40 ± 20 % during the night and 60 ± 20 % during the day. BBA was, on average, less hygroscopic during the night (κ = 0. 04 ± 0.03) than during the day (κ =  0.07 ± 0.05), with a maximum typically observed just before midday. Size-resolved composition of BBA showed that organics comprised a constant 90 % of the aerosol volume for aerodynamic diameters between 100 and 200 nm. While this suggests that the photochemical oxidation of organics led to an increase in the hygroscopic growth and an increase in daytime activation ratios, it does not explain the decrease in hygroscopicity after midday. Modelled CCN concentrations assuming typical continental hygroscopicities produced very large overestimations of up to 200 %. Smaller, but still significant, overpredictions up to  ∼  100 % were observed using aerosol mass spectrometer (AMS)- and hygroscopicity tandem differential mobility analyser (H-TDMA)-derived hygroscopicities as well as campaign night and day averages. The largest estimations in every case occurred during the night, when the small variations in very weakly hygroscopic species corresponded to large variations in the activation diameters. Trade winds carry the smoke generated from these fires over the Timor Sea, where aerosol–cloud interactions are likely to be sensitive to changes in CCN concentrations, perturbing cloud albedo and lifetime. Dry season fires in northern Australia are therefore potentially very important in cloud processes in this region.

Citation: Mallet, M. D., Cravigan, L. T., Milic, A., Alroe, J., Ristovski, Z. D., Ward, J., Keywood, M., Williams, L. R., Selleck, P., and Miljevic, B.: Composition, size and cloud condensation nuclei activity of biomass burning aerosol from northern Australian savannah fires, Atmos. Chem. Phys., 17, 3605-3617, https://doi.org/10.5194/acp-17-3605-2017, 2017.
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Short summary
This paper presents data on the size, composition and concentration of aerosol particles emitted from north Australian savannah fires and how these properties influence cloud condensation nuclei (CCN) concentrations. Both the size and composition of aerosol were found to be important in determining CCN. Despite large CCNc enhancements during periods of close biomass burning, the aerosol was very weakly hygroscopic which should be accounted for in climate models to avoid large CCNc overestimates.
This paper presents data on the size, composition and concentration of aerosol particles emitted...
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