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- ItemEvaluation on the role of sulfuric acid in the mechanisms of new particle formation for Beijing case(München : European Geopyhsical Union, 2011) Wang, Z.B.; Hu, M.; Yue, D.L.; Zheng, J.; Zhang, R.Y.; Wiedensohler, A.; Wu, Z.J.; Nieminen, T.; Boy, M.New particle formation (NPF) is considered as an important mechanism for gas-to-particle transformation, and gaseous sulfuric acid is believed as a crucial precursor. Up to now few field-based studies on nucleation mechanisms and the role of sulfuric acid were conducted in China. In this study, simultaneously measurements of particle number size distributions and gaseous sulfuric acid concentrations were performed from July to September in 2008. Totally, 22 new particle formation events were observed during the entire 85 campaign days. The results show that in the case of both higher source and sink values, the result of the competition between source and sink is more likely the key limiting factor to determine the observation of NPF events in Beijing. The concentrations of gaseous sulfuric acid show good correlations with freshly nucleated particles (N3-6 and formation rates (J3 and J1.5. The power-law relationship between H2SO4 concentration and N3-6 or J is adopted to explore the nucleation mechanism. The exponents are showed a great range (from 1 to 7). More than half of the NPF events exhibit an exponent larger than 2.5. For these cases, the thermodynamic process works better than the activation or kinetic nucleation theories to explain the nucleation events in urban atmosphere of Beijing.
- ItemHygroscopic properties of the Paris urban aerosol in relation to its chemical composition(München : European Geopyhsical Union, 2014) Kamilli, K.A.; Poulain, L.; Held, A.; Nowak, A.; Birmili, W.; Wiedensohler, A.Aerosol hygroscopic growth factors and chemical properties were measured as part of the MEGAPOLI "Megacities Plume Case Study" at the urban site Laboratoire d'Hygiène de la Ville de Paris (LHVP) in the city center of Paris from June to August 2009, and from January to February 2010. Descriptive hygroscopic growth factors (DGF) were derived in the diameter range from 25 to 350 nm at relative humidities of 30, 55, 75, and 90% by applying the summation method on humidified and dry aerosol size distributions measured simultaneously with a humidified differential mobility particle sizer (HDMPS) and a twin differential mobility particle sizer (TDMPS). For 90% relative humidity, the DGF varied from 1.06 to 1.46 in summer, and from 1.06 to 1.66 in winter. Temporal variations in the observed mean DGF could be well explained with a simple growth model based on the aerosol chemical composition measured by aerosol mass spectrometry (AMS) and black carbon photometry (MAAP). In particular, good agreement was observed when sulfate was the predominant inorganic factor. A clear overestimation of the predicted growth factor was found when the nitrate mass concentration exceeded values of 10 μg m−3, e.g., during winter.
- ItemFormation and growth of nucleated particles into cloud condensation nuclei: Model-measurement comparison(München : European Geopyhsical Union, 2013) Westervelt, D.M.; Pierce, J.R.; Riipinen, I.; Trivitayanurak, W.; Hamed, A.; Kulmala, M.; Laaksonen, A.; Decesari, S.; Adams, P.J.Aerosol nucleation occurs frequently in the atmosphere and is an important source of particle number. Observations suggest that nucleated particles are capable of growing to sufficiently large sizes that they act as cloud condensation nuclei (CCN), but some global models have reported that CCN concentrations are only modestly sensitive to large changes in nucleation rates. Here we present a novel approach for using long-term size distribution observations to evaluate a global aerosol model's ability to predict formation rates of CCN from nucleation and growth events. We derive from observations at five locations nucleation-relevant metrics such as nucleation rate of particles at diameter of 3 nm (J3), diameter growth rate (GR), particle survival probability (SP), condensation and coagulation sinks, and CCN formation rate (J100). These quantities are also derived for a global microphysical model, GEOS-Chem-TOMAS, and compared to the observations on a daily basis. Using GEOS-Chem-TOMAS, we simulate nucleation events predicted by ternary (with a 10−5 tuning factor) or activation nucleation over one year and find that the model slightly understates the observed annual-average CCN formation mostly due to bias in the nucleation rate predictions, but by no more than 50% in the ternary simulations. At the two locations expected to be most impacted by large-scale regional nucleation, Hyytiälä and San Pietro Capofiume, predicted annual-average CCN formation rates are within 34 and 2% of the observations, respectively. Model-predicted annual-average growth rates are within 25% across all sites but also show a slight tendency to underestimate the observations, at least in the ternary nucleation simulations. On days that the growing nucleation mode reaches 100 nm, median single-day survival probabilities to 100 nm for the model and measurements range from less than 1–6% across the five locations we considered; however, this does not include particles that may eventually grow to 100 nm after the first day. This detailed exploration of new particle formation and growth dynamics adds support to the use of global models as tools for assessing the contribution of microphysical processes such as nucleation to the total number and CCN budget.
- ItemAerosol size-resolved trace metal composition in remote northern tropical atlantic marine environment: Case study cape verde islands(München : European Geopyhsical Union, 2013) Fomba, K.W.; Müller, K.; van Pinxteren, D.; Herrmann, H.Size-resolved trace metal concentrations of 15 elements in aerosol particles at the Cape Verde Atmospheric Observatory (CVAO) under remote background conditions were investigated through analysis of aerosol samples collected during intensive field studies from January 2007 to November 2011 using total reflection x-ray fluorescence (TXRF). The identification of the main air mass origin that influence remote marine aerosol in the northern tropical Atlantic has been investigated. In total, 317 samples were collected. The dataset was analyzed according to the main air mass inflow at the station. We found that remote conditions make up about 45% of the meteorological conditions in a year at CVAO and thus the northern tropical Atlantic. Surprisingly, air masses from North America are often responsible for higher trace metal concentrations in this region. Elements such as Zn, Pb, Cu, Cr, Ni, and V were mostly found in the submicron size fractions, while elements with dominant crustal or oceanic origin such as Fe, Ti, Mn, Sr, and Rb were found in the coarse fractions (>1 μm). The highest metal concentrations, especially for Zn (3.23 ng m−3), Cu (0.81 ng m−3), Sr (2.63 ng m−3), and Cr (0.53 ng m−3), were observed in air masses originating from North America and the concentrations were within the same concentration range to those reported previously in the literature for remote marine aerosols. Fe (12.26 ng m−3), Ti (0.91 ng m−3), and Mn (0.35 ng m−3) showed higher concentrations when air mass came from Europe and the Canary Islands. Pb concentration was low (<0.20 ng m−3) and did not vary significantly with air mass direction. The low Pb concentration is indicative of the complete phase-out of leaded gasoline even in African countries. Crustal enrichment factor values decreased from fine to coarse-mode particles with low values (<4) observed for Fe, Mn, and Rb, and high values (>20) for Zn, Cu, Ni, Cr, Pb, and Se. The observed enrichment of the elements was attributed to crustal, marine, anthropogenic, and biogenic sources, as well as long-range transport and resuspension. Zn, Cu and Pb were indicators of anthropogenic activities, while Ti and Sr were indicators of crustal and marine origin, respectively. Oceanic and biogenic emissions might have contributed to most of the Se observed. This work provides the first long-term size-resolved trace metals study for remote tropical northern Atlantic marine aerosols and the dataset could serve as good initiation of yearly flux estimates.
- ItemA parameterization of low visibilities for hazy days in the North China Plain(München : European Geopyhsical Union, 2012) Chen, J.; Zhao, C.S.; Ma, N.; Liu, P.F.; Göbel, T.; Hallbauer, E.; Deng, Z.Z.; Ran, L.; Xu, W.Y.; Liang, Z.; Liu, H.J.; Yan, P.; Zhou, X.J.; Wiedensohler, A.Visibility degradation is a pervasive and urgent environmental problem in China. The occurrence of low visibility events is frequent in the North China Plain, where the aerosol loading is quite high and aerosols are strongly hygroscopic. A parameterization of light extinction (Kex) for low visibilities on hazy days is proposed in this paper, based on visibility, relative humidity (RH), aerosol hygroscopic growth factors and particle number size distributions measured during the Haze in China (HaChi) Project. Observational results show that a high aerosol volume concentration is responsible for low visibility at RH <90%; while for RH >90%, decrease of visibility is mainly influenced by the increase of RH. The parameterization of Kex is developed on the basis of aerosol volume concentrations and RH, taking into accounts the sensitivity of visibility to the two factors and the availability of corresponding data. The extinction coefficients calculated with the parameterization schemes agree well with the directly measured values.