Atmos. Chem. Phys. Discuss., 10, 26841-26890, 2010
www.atmos-chem-phys-discuss.net/10/26841/2010/
doi:10.5194/acpd-10-26841-2010
© Author(s) 2010. This work is distributed
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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.
Cloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China – Part 2: Size-resolved aerosol chemical composition, diurnal cycles, and externally mixed CCN-inactive soot particles
D. Rose1, S. S. Gunthe1, H. Su1, R. M. Garland1, H. Yang1, M. Berghof2, Y. F. Cheng2, B. Wehner2, P. Achtert2, A. Nowak2, A. Wiedensohler2, N. Takegawa3, Y. Kondo3, M. Hu4, Y. Zhang4, M. O. Andreae1, and U. Pöschl1
1Biogeochemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
2Leibniz Institute for Tropospheric Research, Leipzig, Germany
3RCAST, University of Tokyo, Tokyo, Japan
4State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing, China

Abstract. Size-resolved chemical composition, mixing state, and CCN activity of aerosol particles in polluted mega-city air and biomass burning smoke were measured during the PRIDE-PRD2006 campaign near Guangzhou, China, using an aerosol mass spectrometer (AMS), a volatility tandem differential mobility analyzer (VTDMA), and a continuous-flow CCN counter (DMT-CCNC).

The size-dependence and temporal variations of the effective average hygroscopicity parameter for CCN-active particles (κa) could be parameterized as a function of organic and inorganic mass fractions determined by AMS: κa,porg·forginorg·finorg. The characteristic κ values of organic and inorganic components were similar to those observed in other continental regions of the world: κorg≈0.1 and κinorg≈0.6. The campaign average κa values increased with particle size from ~0.25 at ~50 nm to ~0.4 at ~200 nm, while forg decreased with particle size. At ~50 nm, forg was on average 60% and increased to almost 100% during a biomass burning event.

The VTDMA results and complementary aerosol optical data suggest that the large fractions of CCN-inactive particles observed at low supersaturations (up to 60% at S≤0.27%) were externally mixed soot particles with low volatility (diameter reduction <5% at 300 °C) and effective hygroscopicity parameters around κlv≈0.01. A proxy for the effective average hygroscopicity of the total ensemble of CCN-active and -inactive particles (κt) could be parameterized as a function of κa,p and the number fraction of low volatility particles determined by VTDMA (φlv): κt,pa,p−φlv·(κa,p−κlv).

Based on κ values derived from AMS and VTDMA data, the observed CCN number concentrations (NCCN,S≈102–104 cm−3 at S=0.068–0.47%) could be efficiently predicted from the measured particle number size distribution. The mean relative deviations between observed and predicted CCN concentrations were ~10% when using κt,p, and they increased to ~20% when using only κa,p. The mean relative deviations were not higher (~20%) when using an approximate continental average value of κ≈0.3, although the constant κ value cannot account for the observed temporal variations in particle composition and mixing state (diurnal cycles and biomass burning events).

The results confirm that an average value of κ≈0.3 can be used for approximate predictions of CCN number concentrations in continental boundary layer air when aerosol size distribution data are available without information about chemical composition. Bulk or size-resolved data on aerosol chemical composition enable improved CCN predictions resolving temporal variations, but the composition data need to be highly accurate and complemented by information about particle mixing state to achieve high precision (relative deviations <20%).


Citation: Rose, D., Gunthe, S. S., Su, H., Garland, R. M., Yang, H., Berghof, M., Cheng, Y. F., Wehner, B., Achtert, P., Nowak, A., Wiedensohler, A., Takegawa, N., Kondo, Y., Hu, M., Zhang, Y., Andreae, M. O., and Pöschl, U.: Cloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China – Part 2: Size-resolved aerosol chemical composition, diurnal cycles, and externally mixed CCN-inactive soot particles, Atmos. Chem. Phys. Discuss., 10, 26841-26890, doi:10.5194/acpd-10-26841-2010, 2010.
 
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