A long term experiment was conducted in a primary forest area in Amazonia, with continuous in-situ measurements of aerosol optical properties between February 2008 and April 2011, comprising, to our knowledge, the longest database ever in the Amazon Basin. Two major classes of aerosol particles, with significantly different optical properties were identified: coarse mode predominant biogenic aerosols in the wet season (January–June), naturally released by the forest metabolism, and fine mode dominated biomass burning aerosols in the dry season (July–December), transported from regional fires. Dry particle median scattering coefficients at the wavelength of 550 nm increased from 6.3 Mm⁻¹ to 22 Mm⁻¹, whereas absorption at 637 nm increased from 0.5 Mm⁻¹ to 2.8 Mm⁻¹ from wet to dry season. Most of the scattering in the dry season was attributed to the predominance of fine mode (PM₂) particles (40–80% of PM₁₀ mass), while the enhanced absorption coefficients are attributed to the presence of light absorbing aerosols from biomass burning. As both scattering and absorption increased in the dry season, the single scattering albedo (SSA) did not show a significant seasonal variability, in average 0.86 ± 0.08 at 637 nm for dry aerosols. Measured particle optical properties were used to estimate the aerosol forcing efficiency at the top of the atmosphere. Results indicate that in this primary forest site the radiative balance was dominated by the cloud cover, particularly in the wet season. Due to the high cloud fractions, the aerosol forcing efficiency absolute values were below −3.5 W m⁻² in 70% of the wet season days and in 46% of the dry season days. Besides the seasonal variation, the influence of out-of-Basin aerosol sources was observed occasionally. Periods of influence of the Manaus urban plume were detected, characterized by a consistent increase on particle scattering (factor 2.5) and absorption coefficients (factor 5). Episodes of biomass burning and mineral dust particles advected from Africa were observed between January and April, characterized by enhanced concentrations of crustal elements (Al, Si, Ti, Fe) and potassium in the fine mode. During these episodes, median particle absorption coefficients increased by a factor of 2, whereas median SSA values decreased by 7%, in comparison to wet season conditions

Abstract.A one-year study was performed at the Vavihill background station in southern Sweden to estimate the anthropogenic contribution to the carbonaceous aerosol. Weekly samples of the particulate matter PM 10 were collected on quartz filters, and the amounts of organic carbon, elemental carbon, radiocarbon ( 14 C) and levoglucosan were measured. This approach enabled source apportionment of the total carbon in the PM 10 fraction using the concentration ratios of the sources. The sources considered in this study were emissions from the combustion of fossil fuels and biomass, as well as biogenic sources. During the summer, the carbonaceous aerosol mass was dominated by compounds of biogenic origin (80 %), which are associated with biogenic primary and secondary organic aerosols. During the winter months, biomass combustion (32 %) and fossil fuel combustion (28 %) were the main contributors to the carbonaceous aerosol. Elemental carbon concentrations in winter were about twice as large as during summer, and can be attributed to biomass combustion, probably from domestic wood burning. The contribution of fossil fuels to elemental carbon was stable throughout the year, although the fossil contribution to organic carbon increased during the winter. Thus, the organic aerosol originated mainly from natural sources during the summer and from anthropogenic sources during the winter. The result of this source apportionment was compared with results from the EMEP MSC-W chemical transport model. The model and measurements were generally consistent for total atmospheric organic carbon, however, the contribution of the sources varied substantially. E.g. the biomass burning contributions of OC were underestimated by the model by a factor of 2.2 compared to the measurements.

Abstract. The hygroscopic growth of the atmospheric aerosol is a critical parameter for quantifying the anthropogenic radiative forcing. Until now, there has been a lack of long term measurements due to limitations in instrumental techniques. In this work, for the first time the seasonal variation of the hygroscopic properties of a continental background aerosol has been described, based on more than two years of continuous measurements. In addition to this, the diurnal variation of the hygroscopic growth has been investigated, as well as the seasonal variation in CCN concentration. These physical properties of the aerosol have been measured with a Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA), a Differential Mobility Particle Sizer (DMPS), and a Cloud Condensation Nuclei Counter (CCNC). The results show that smaller particles are generally less hygroscopic than larger ones, and that there is a clear difference in the hygroscopic properties between the Aitken and the accumulation mode. A seasonal cycle was found for all particle sizes. In general, the average hygroscopic growth is lower during wintertime, due to an increase in the relative abundance of less hygroscopic or barely hygroscopic particles. Monthly averages showed that the hygroscopic growth factors of the two dominating hygroscopic modes (one barely hygroscopic and one more hygroscopic) were relatively stable. The hygroscopic growth additionally showed a diurnal cycle, with higher growth factors during day time. CCN predictions based on H-TDMA data underpredicted the activated CCN number concentration with 7 % for a 1 % water supersaturation ratio. The underprediction increases with decreasing s, most likely due to a combination of measurement and modeling uncertainties. It was found that although the aerosol is often externally mixed, recalcuCorrespondence to: E. O. Fors (erik.fors@nuclear.lu.se) lating to an internal mixture with respect to hygroscopicity did not change the CCN concentration as a function of supersaturation significantly.

Abstract. The performance of six custom-built Hygrocopicity-Tandem Differential Mobility Analyser (H-TDMA) systems was investigated in the frame of an international calibration and intercomparison workshop held in Leipzig, February 2006. The goal of the workshop was to harmonise H-TDMA measurements and develop recommendations for atmospheric measurements and their data evaluation. The H-TDMA systems were compared in terms of the sizing of dry particles, relative humidity (RH) uncertainty, and consistency in determination of number fractions of different hygroscopic particle groups. The experiments were performed in an air-conditioned laboratory using ammonium sulphate particles or an external mixture of ammonium sulphate and soot particles.The sizing of dry particles of the six H-TDMA systems was within 0.2 to 4.2% of the selected particle diameter depending on investigated size and individual system. Measurements of ammonium sulphate aerosol found deviations equivalent to 4.5% RH from the set point of 90% RH compared to results from previous experiments in the literature. Evaluation of the number fraction of particles within the clearly separated growth factor modes of a laboratory generated externally mixed aerosol was done. The data from the H-TDMAs was analysed with a single fitting routine to investigate differences caused by the different data evaluationCorrespondence to: A. Massling (anma@dmu.dk) procedures used for each H-TDMA. The differences between the H-TDMAs were reduced from +12/−13% to +8/−6% when the same analysis routine was applied. We conclude that a common data evaluation procedure to determine number fractions of externally mixed aerosols will improve the comparability of H-TDMA measurements.It is recommended to ensure proper calibration of all flow, temperature and RH sensors in the systems. It is most important to thermally insulate the aerosol humidification unit and the second DMA and to monitor these temperatures to an accuracy of 0.2 • C. For the correct determination of external mixtures, it is necessary to take into account size-dependent losses due to diffusion in the plumbing between the DMAs and in the aerosol humidification unit.

[1] The ability of particles to activate and form cloud droplets influences the functioning of the Earth's hydrological cycle. This work links the particle water uptake at subsaturation to the critical supersaturation ratio needed for particles to become cloud condensation nuclei (CCN). Five models using the particle hygroscopic growth at subsaturation for predicting the critical supersaturation needed for droplet activation were applied to a laboratory data set of inorganic and organic compounds and mixtures of them. The data set consisted of hygroscopicity tandem differential mobility analyzer measurements and CCN counter measurements. No chemical composition information was used when applying the models. All models tested were based on modifications of Köhler theory and gave similar results. The agreement between predicted and measured critical supersaturations was good, considering the relatively simple models used. A trend of overestimating the critical supersaturations was observed, typically by ∼15%. The best performing model gave on average only a 4% offset from experimental values; the model with the largest deviation was offset by 20%. A comparison was made between the number of soluble entities (ions or nondissociating molecules) estimated from the particle hygroscopic growth at 90% relative humidity (RH) and the number estimated from the particle critical supersaturation; a ∼35% increase was observed in the effective number of entities in solution when going from 90% RH to activation. For many types of aerosols, differences in the model approaches tested do not induce large differences in the predicted critical supersaturation. However, it is most important to follow the recommendations published with the respective models and not use them indiscriminately.Citation: Rissler, J., B. Svenningsson, E. O. Fors, M. Bilde, and E. Swietlicki (2010), An evaluation and comparison of cloud condensation nucleus activity models: Predicting particle critical saturation from growth at subsaturation,