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- ItemFirst long-term study of particle number size distributions and new particle formation events of regional aerosol in the North China Plain(München : European Geopyhsical Union, 2011) Shen, X.J.; Sun, J.Y.; Zhang, Y.M.; Wehner, B.; Nowak, A.; Tuch, T.; Zhang, X.C.; Wang, T.T.; Zhou, H.G.; Zhang, X.L.; Dong, F.; Birmili, W.; Wiedensohler, A.Atmospheric particle number size distributions (size range 0.003–10 μm) were measured between March 2008 and August 2009 at Shangdianzi (SDZ), a rural research station in the North China Plain. These measurements were made in an attempt to better characterize the tropospheric background aerosol in Northern China. The mean particle number concentrations of the total particle, as well as the nucleation, Aitken, accumulation and coarse mode were determined to be 1.2 ± 0.9 × 104, 3.6 ± 7.9 × 103, 4.4 ± 3.4 × 103, 3.5 ± 2.8 × 103 and 2 ± 3 cm−3, respectively. A general finding was that the particle number concentration was higher during spring compared to the other seasons. The air mass origin had an important effect on the particle number concentration and new particle formation events. Air masses from northwest (i.e. inner Asia) favored the new particle formation events, while air masses from southeast showed the highest particle mass concentration. Significant diurnal variations in particle number were observed, which could be linked to new particle formation events, i.e. gas-to-particle conversion. During particle formation events, the number concentration of the nucleation mode rose up to maximum value of 104 cm−3. New particle formation events were observed on 36% of the effective measurement days. The formation rate ranged from 0.7 to 72.7 cm−3 s−1, with a mean value of 8.0 cm−3 s−1. The value of the nucleation mode growth rate was in the range of 0.3–14.5 nm h−1, with a mean value of 4.3 nm h−1. It was an essential observation that on many occasions the nucleation mode was able to grow into the size of cloud condensation nuclei (CCN) within a matter of several hours. Furthermore, the new particle formation was regularly followed by a measurable increase in particle mass concentration and extinction coefficient, indicative of a high abundance of condensable vapors in the atmosphere under study.
- 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%).