Size-resolved cloud condensation nuclei (CCN) spectra measured for various aerosol types at a non-urban site in Germany showed that CCN concentrations are mainly determined by the aerosol number size distribution. Distinct variations of CCN activation with particle chemical composition were observed but played a secondary role. When the temporal variation of chemical effects on CCN activation is neglected, variation in the size distribution alone explains 84 to 96% of the variation in CCN concentrations. Understanding that particles' ability to act as CCN is largely controlled by aerosol size rather than composition greatly facilitates the treatment of aerosol effects on cloud physics in regional and global models.

In recent years, severe haze events often occurred in China, causing serious environmental problems. The mechanisms responsible for the haze formation, however, are still not well understood, hindering the forecast and mitigation of haze pollution. Our study of the 2012–13 winter haze events in Beijing shows that atmospheric water vapour plays a critical role in enhancing the heavy haze events. Under weak solar radiation and stagnant moist meteorological conditions in winter, air pollutants and water vapour accumulate in a shallow planetary boundary layer (PBL). A positive feedback cycle is triggered resulting in the formation of heavy haze: (1) the dispersal of water vapour is constrained by the shallow PBL, leading to an increase in relative humidity (RH); (2) the high RH induces an increase of aerosol particle size by enhanced hygroscopic growth and multiphase reactions to increase particle size and mass, which results in (3) further dimming and decrease of PBL height, and thus further depressing of aerosol and water vapour in a very shallow PBL. This positive feedback constitutes a self-amplification mechanism in which water vapour leads to a trapping and massive increase of particulate matter in the near-surface air to which people are exposed with severe health hazards.

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[1] In a forested near-urban location in central Germany, the CCN efficiency of particles smaller than 100 nm decreases significantly during periods of new particle formation. This results in an increase of average activation diameters, ranging from 5 to 8% at supersaturations of 0.33% and 0.74%, respectively. At the same time, the organic mass fraction in the sub-100-nm size range increases from approximately 2/3 to 3/4. This provides evidence that secondary organic aerosol (SOA) components are involved in the growth of new particles to larger sizes, and that the reduced CCN efficiency of small particles is caused by the low hygroscopicity of the condensing material. The observed dependence of particle hygroscopicity (k) on chemical composition can be parameterized as a function of organic and inorganic mass fractions (f org , f inorg ) determined by aerosol mass spectrometry: k = k org f org + k inorg f inorg . The obtained value of k org % 0.1 is characteristic for SOA, and k inorg % 0.7 is consistent with the observed mix of ammonium, sulfate and nitrate ions. Citation: Dusek, U., G. P. Frank, J. Curtius, F. Drewnick, J. Schneider, A. Kürten, D. Rose, M. O. Andreae, S. Borrmann, and U. Pö schl (2010), Enhanced organic mass fraction and decreased hygroscopicity of cloud condensation nuclei (CCN) during new particle formation events, Geophys.

Light-absorbing organic carbon (i.e., brown carbon or BrC) in the atmospheric aerosol has significant contribution to light absorption and radiative forcing. However, the link between BrC optical properties and chemical composition remains poorly constrained. In this study, we combine spectrophotometric measurements and chemical analyses of BrC samples collected from July 2008 to June 2009 in urban Xi'an, Northwest China. Elevated BrC was observed in winter (5 times higher than in summer), largely due to increased emissions from wintertime domestic biomass burning. The light absorption coefficient of methanol-soluble BrC at 365 nm (on average approximately twice that of water-soluble BrC) was found to correlate strongly with both parent polycyclic aromatic hydrocarbons (parent-PAHs, 27 species) and their carbonyl oxygenated derivatives (carbonyl-OPAHs, 15 species) in all seasons ( r > 0.61). These measured parent-PAHs and carbonyl-OPAHs account for on average ∼1.7% of the overall absorption of methanol-soluble BrC, about 5 times higher than their mass fraction in total organic carbon (OC, ∼0.35%). The fractional solar absorption by BrC relative to element carbon (EC) in the ultraviolet range (300-400 nm) is significant during winter (42 ± 18% for water-soluble BrC and 76 ± 29% for methanol-soluble BrC), which may greatly affect the radiative balance and tropospheric photochemistry and therefore the climate and air quality.

Abstract. We investigate the CCN activity of freshly emitted biomass burning particles and their hygroscopic growth at a relative humidity (RH) of 85 %. The particles were produced in the Mainz combustion laboratory by controlled burning of various wood types. The water uptake at sub-and supersaturations is parameterized by the hygroscopicity parameter, κ (c.f. Petters and Kreidenweis, 2007). For the wood burns, κ is low, generally around 0.06. The main emphasis of this study is a comparison of κ derived from measurements at sub-and supersaturated conditions (κ G and κ CCN ), in order to see whether the water uptake at 85 % RH can predict the CCN properties of the biomass burning particles. Differences in κ G and κ CCN can arise through solution nonidealities, the presence of slightly soluble or surface active compounds, or non-spherical particle shape. We find that κ G and κ CCN agree within experimental uncertainties (of around 30 %) for particle sizes of 100 and 150 nm; only for 50 nm particles is κ CCN larger than κ G by a factor of 2. The magnitude of this difference and its dependence on particle size is consistent with the presence of surface active organic compounds. These compounds mainly facilitate the CCN activation of small particles, which form the most concentratedCorrespondence to: U. Dusek (u.dusek@uu.nl) solution droplets at the point of activation. The 50 nm particles, however, are only activated at supersaturations higher than 1 % and are therefore of minor importance as CCN in ambient clouds. By comparison with the actual chemical composition of the biomass burning particles, we estimate that the hygroscopicity of the water-soluble organic carbon (WSOC) fraction can be represented by a κ WSOC value of approximately 0.2. The effective hygroscopicity of a typical wood burning particle can therefore be represented by a linear mixture of an inorganic component with κ ∼ = 0.6, a WSOC component with κ ∼ = 0.2, and an insoluble component with κ = 0.

The CCN (cloud condensation nucleus) activation of pure and coated carbon black particles was investigated using the University of Vienna cloud condensation nuclei counter (Giebl, H.; Berner, A.; Reischl, G.; Puxbaum, H.; Kasper-Giebl, A.; Hitzenberger, R. J. Aerosol Sci. 2002, 33, 1623-1634). The particles were produced by nebulizing an aqueous suspension of carbon black in a Collison atomizer. The activation of pure carbon black particles was found to require higher supersaturations than predicted by calculations representing the particles as insoluble, wettable spheres with mobility equivalent diameter. To test whether this effect is an artifact due to heating of the light-absorbing carbon black particles in the laser beam, experiments at different laser powers were conducted. No systematic dependence of the activation of pure carbon black particles on laser power was observed. The observations could be modeled using spherical particles and an effective contact angle of 4-6 degrees of water at their surface. The addition of a small amount of NaCl to the carbon black particles (by adding 5% by mass NaCl to the carbon black suspension) greatly enhanced their CCN efficiency. The measured CCN efficiencies were consistent with Kohler theory for particles consisting of insoluble and hygroscopic material. However, coating the carbon black particles with hexadecanol (a typical film-forming compound with one hydrophobic and one hydrophilic end) efficiently suppressed the CCN activation of the carbon black particles.

Abstract. We thoroughly characterized a system for thermal separation of organic carbon (OC) and elemental carbon (EC) for subsequent radiocarbon analysis. Different organic compounds as well as ambient aerosol filter samples were introduced into an oven system and combusted to CO 2 in pure O 2 . The main objective was to test which combustion times and temperatures are best suited to separate OC and EC. The final separation step for OC was combustion at 360 • C for 15 min. Combustion at this temperature proved enough to remove several organic test substances from the filter (including high molecular weight humic acid) but did not remove substantial amounts of EC. For isolation of EC, OC first needs to be completely removed from the filter. This was achieved by water extraction of the filter, followed by combustion of the water insoluble OC at 360 • C and combustion at an intermediate temperature step of 2 min at 450 • C. This last step removed the most refractory OC together with some EC. Finally, the remaining EC was combusted to CO 2 at 650 • C. The recovery of black carbon after the intermediate 450 • C step was approximately 80 %. Several tests provided strong evidence that OC was removed efficiently during the intermediate temperature step: (i) brown carbon, indicative of refractory OC, was removed; (ii) the fraction modern of EC did not decrease significantly if the temperature of the intermediate step was further increased. Based on tests with various organic compounds, we estimated that charred organic carbon could contribute 4-8 % to an elemental carbon sample that was isolated according to our method.