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- ItemCloud 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 weakly CCN-active soot particles(München : European Geopyhsical Union, 2011) 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.; Pöschl, U.Size-resolved chemical composition, mixing state, and cloud condensation nucleus (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 (forg, finorg) determined by the AMS: κa,p=κorg·forg + κinorg·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 weakly CCN-active 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 particles including weakly CCN-active particles (κt) could be parameterized as a function of κa,p and the number fraction of low volatility particles determined by VTDMA (φLV): κt,p=κa,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). Overall, the results confirm that on a global and climate modeling scale 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 regional and 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%).
- ItemAerosol particle number size distributions and particulate light absorption at the ZOTTO tall tower (Siberia), 2006–2009(München : European Geopyhsical Union, 2011) Heintzenberg, J.; Birmili, W.; Otto, R.; Andreae, M.O.; Mayer, J.-C.; Chi, X.; Panov, A.This paper analyses aerosol particle number size distributions, particulate absorption at 570 nm wavelength and carbon monoxide (CO) measured between September 2006 and January 2010 at heights of 50 and 300 m at the Zotino Tall Tower Facility (ZOTTO) in Siberia (60.8° N; 89.35° E). Average number, surface and volume concentrations are broadly comparable to former studies covering shorter observation periods. Fits of multiple lognormal distributions yielded three maxima in probability distribution of geometric mean diameters in the Aitken and accumulation size range and a possible secondary maximum in the nucleation size range below 25 nm. The seasonal cycle of particulate absorption shows maximum concentrations in high winter (December) and minimum concentrations in mid-summer (July). The 90th percentile, however, indicates a secondary maximum in July/August that is likely related to forest fires. The strongly combustion derived CO shows a single winter maximum and a late summer minimum, albeit with a considerably smaller seasonal swing than the particle data due to its longer atmospheric lifetime. Total volume and even more so total number show a more complex seasonal variation with maxima in winter, spring, and summer. A cluster analysis of back trajectories and vertical profiles of the pseudo-potential temperature yielded ten clusters with three levels of particle number concentration: Low concentrations in Arctic air masses (400–500 cm−3), mid-level concentrations for zonally advected air masses from westerly directions between 55° and 65° N (600–800 cm−3), and high concentrations for air masses advected from the belt of industrial and population centers in Siberia and Kazakhstan (1200 cm−3). The observational data is representative for large parts of the troposphere over Siberia and might be particularly useful for the validation of global aerosol transport models.
- ItemA synthesis of cloud condensation nuclei counter (CCNC) measurements within the EUCAARI network(München : European Geopyhsical Union, 2015) Paramonov, M.; Kerminen, V.-M.; Gysel, M.; Aalto, P.P.; Andreae, M.O.; Asmi, E.; Baltensperger, U.; Bougiatioti, A.; Brus, D.; Frank, G.P.; Good, N.; Gunthe, S.S.; Hao, L.; Irwin, M.; Jaatinen, A.; Jurányi, Z.; King, S.M.; Kortelainen, A.; Kristensson, A.; Lihavainen, H.; Kulmala, M.; Lohmann, U.; Martin, S.T.; McFiggans, G.; Mihalopoulos, N.; Nenes, A.; O'Dowd, C.D.; Ovadnevaite, J.; Petäjä, T.; Pöschl, U.; Roberts, G.C.; Rose, D.; Svenningsson, B.; Swietlicki, E.; Weingartner, E.; Whitehead, J.; Wiedensohler, A.; Wittbom, C.; Sierau, B.Cloud condensation nuclei counter (CCNC) measurements performed at 14 locations around the world within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) framework have been analysed and discussed with respect to the cloud condensation nuclei (CCN) activation and hygroscopic properties of the atmospheric aerosol. The annual mean ratio of activated cloud condensation nuclei (NCCN) to the total number concentration of particles (NCN), known as the activated fraction A, shows a similar functional dependence on supersaturation S at many locations – exceptions to this being certain marine locations, a free troposphere site and background sites in south-west Germany and northern Finland. The use of total number concentration of particles above 50 and 100 nm diameter when calculating the activated fractions (A50 and A100, respectively) renders a much more stable dependence of A on S; A50 and A100 also reveal the effect of the size distribution on CCN activation. With respect to chemical composition, it was found that the hygroscopicity of aerosol particles as a function of size differs among locations. The hygroscopicity parameter κ decreased with an increasing size at a continental site in south-west Germany and fluctuated without any particular size dependence across the observed size range in the remote tropical North Atlantic and rural central Hungary. At all other locations κ increased with size. In fact, in Hyytiälä, Vavihill, Jungfraujoch and Pallas the difference in hygroscopicity between Aitken and accumulation mode aerosol was statistically significant at the 5 % significance level. In a boreal environment the assumption of a size-independent κ can lead to a potentially substantial overestimation of NCCN at S levels above 0.6 %. The same is true for other locations where κ was found to increase with size. While detailed information about aerosol hygroscopicity can significantly improve the prediction of NCCN, total aerosol number concentration and aerosol size distribution remain more important parameters. The seasonal and diurnal patterns of CCN activation and hygroscopic properties vary among three long-term locations, highlighting the spatial and temporal variability of potential aerosol–cloud interactions in various environments.