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
*now at: EWRE Division, Department of Civil Engineering, Indian Institute of Technology Madras, Chennai, India
**now at: Natural Resources and the Environment, Council for Scientific and Industrial Research, Pretoria, South Africa
***now at: School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts, USA
Received: 02 Feb 2011 – Published in Atmos. Chem. Phys. Discuss.: 25 Mar 2011
Abstract. Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate. CCN properties were measured and characterized during the CAREBeijing-2006 campaign at a regional site south of the megacity of Beijing, China. Size-resolved CCN efficiency spectra recorded for a supersaturation range of S=0.07% to 0.86% yielded average activation diameters in the range of 190 nm to 45 nm. The corresponding effective hygroscopicity parameters (κ) exhibited a strong size dependence ranging from ~0.25 in the Aitken size range to ~0.45 in the accumulation size range. The campaign average value (κ =0.3 ± 0.1) was similar to the values observed and modeled for other populated continental regions.
Revised: 18 Oct 2011 – Accepted: 25 Oct 2011 – Published: 08 Nov 2011
The hygroscopicity parameters derived from the CCN measurements were consistent with chemical composition data recorded by an aerosol mass spectrometer (AMS) and thermo-optical measurements of apparent elemental and organic carbon (EC and OC). The CCN hygroscopicity and its size dependence could be parameterized as a function of only AMS based organic and inorganic mass fractions (forg, finorg) using the simple mixing rule κp ≈ 0.1 · forg + 0.7 · finorg.
When the measured air masses originated from the north and passed rapidly over the center of Beijing (fresh city pollution), the average particle hygroscopicity was reduced (κ = 0.2 ± 0.1), which is consistent with enhanced mass fractions of organic compounds (~50%) and EC (~30%) in the fine particulate matter (PM1). Moreover, substantial fractions of externally mixed weakly CCN-active particles were observed at low supersaturation (S=0.07%), which can be explained by the presence of freshly emitted soot particles with very low hygroscopicity (κ < 0.1). Particles in stagnant air from the industrialized region south of Beijing (aged regional pollution) were on average larger and more hygroscopic, which is consistent with enhanced mass fractions (~60%) of soluble inorganic ions (mostly sulfate, ammonium, and nitrate). Accordingly, the number concentration of CCN in aged air from the megacity region was higher than in fresh city outflow ((2.5–9.9) × 103 cm−3 vs. (0.4–8.3) × 103 cm−3 for S=0.07–0.86%) although the total aerosol particle number concentration was lower (1.2 × 104 cm−3 vs. 2.3 × 104 cm−3). A comparison with related studies suggests that the fresh outflow from Chinese urban centers generally may contain more, but smaller and less hygroscopic aerosol particles and thus fewer CCN than the aged outflow from megacity regions.
Citation: Gunthe, S. S., Rose, D., Su, H., Garland, R. M., Achtert, P., Nowak, A., Wiedensohler, A., Kuwata, M., Takegawa, N., Kondo, Y., Hu, M., Shao, M., Zhu, T., Andreae, M. O., and Pöschl, U.: Cloud condensation nuclei (CCN) from fresh and aged air pollution in the megacity region of Beijing, Atmos. Chem. Phys., 11, 11023-11039, doi:10.5194/acp-11-11023-2011, 2011.