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- ItemChanges in the production rate of secondary aerosol particles in Central Europe in view of decreasing SO2 emissions between 1996 and 2006(München : European Geopyhsical Union, 2010) Hamed, A.; Birmili, W.; Joutsensaari, J.; Mikkonen, S.; Asmi, A.; Wehner, B.; Spindler, G.; Jaatinen, A.; Wiedensohler, A.; Korhonen, H.; Lehtinen, K.E.J.; Laaksonen, A.In anthropogenically influenced atmospheres, sulphur dioxide (SO2) is the main precursor of gaseous sulphuric acid (H2SO4), which in turn is a main precursor for atmospheric particle nucleation. As a result of socio-economic changes, East Germany has seen a dramatic decrease in anthropogenic SO2 emissions between 1989 and present, as documented by routine air quality measurements in many locations. We have attempted to evaluate the influence of changing SO2 concentrations on the frequency and intensity of new particle formation (NPF) using two different data sets (1996–1997; 2003–2006) of experimental particle number size distributions (diameter range 3–750 nm) from the atmospheric research station Melpitz near Leipzig, Germany. Between the two periods SO2 concentrations decreased by 65% on average, while the frequency of NPF events dropped by 45%. Meanwhile, the average formation rate of 3 nm particles decreased by 68% on average. The trends were statistically significant and therefore suggest a connection between the availability of anthropogenic SO2 and freshly formed new particles. In contrast to the decrease in new particle formation, we found an increase in the mean growth rate of freshly nucleated particles (+22%), suggesting that particle nucleation and subsequent growth into larger sizes are delineated with respect to their precursor species. Using three basic parameters, the condensation sink for H2SO4, the SO2 concentration, and the global radiation intensity, we were able to define the characteristic range of atmospheric conditions under which particle formation events take place at the Melpitz site. While the decrease in the concentrations and formation rates of the new particles was rather evident, no similar decrease was found with respect to the generation of cloud condensation nuclei (CCN; particle diameter >100 nm) as a result of atmospheric nucleation events. On the contrary, the production of CCN following nucleation events appears to have increased by tens of percents. Our aerosol dynamics model simulations suggest that such an increase can be caused by the increased particle growth rate.
- ItemAnalysis of exceedances in the daily PM10 mass concentration (50 μg m−3) at a roadside station in Leipzig, Germany(München : European Geopyhsical Union, 2012) Engler, C.; Birmili, W.; Spindler, G.; Wiedensohler, A.Five years of PM10 and PM2.5 ambient air measurements at a roadside, an urban, and a regional background site in Leipzig (Germany) were analyzed for violations of the legal PM10 limit value (EC, 1999). The annual mean PM10 concentrations at the three sites were well below the legal threshold of 40 μg m−3 (32.6, 22.0 and 21.7 μg m−3, respectively). At roadside, the daily maximum value of 50 μg m−3 was exceeded on 232 days (13% of all days) in 2005–2009, which led to a violation of the EC directive in three out of five years. We analysed the meteorological factors and local source contributions that eventually led to the exceedances of the daily limit value. As noted in other urban environments before, most exceedance days were observed in the cold season. Exceedance days were most probable under synoptic situations characterised by stagnant winds, low temperatures and strong temperature inversions in winter time. However, these extreme situations accounted for only less than half of the exeedance days. We also noticed a significant number of exceedance days that occurred in the cold season under south-westerly winds, and in the warm season in the presence of easterly winds. Our analysis suggests that local as well as regional sources of PM are equally responsible for exceedances days at the roadside site. The conclusion is that a combined effort of local, national and international reduction measures appears most likely to avoid systematic exceedances of the daily limit value in the future.
- ItemAerosol hygroscopicity derived from size-segregated chemical composition and its parameterization in the North China Plain(München : European Geopyhsical Union, 2014) Liu, H.J.; Zhao, C.S.; Nekat, B.; Ma, N.; Wiedensohler, A.; van Pinxteren, D.; Spindler, G.; Müller, K.; Herrmann, H.Hygroscopic growth of aerosol particles is of significant importance in quantifying the aerosol radiative effect in the atmosphere. In this study, hygroscopic properties of ambient particles are investigated based on particle chemical composition at a suburban site in the North China Plain during the HaChi campaign (Haze in China) in summer 2009. The size-segregated aerosol particulate mass concentration as well as the particle components such as inorganic ions, organic carbon and water-soluble organic carbon (WSOC) are identified from aerosol particle samples collected with a ten-stage impactor. An iterative algorithm is developed to evaluate the hygroscopicity parameter κ from the measured chemical composition of particles. During the HaChi summer campaign, almost half of the mass concentration of particles between 150 nm and 1 μm is contributed by inorganic species. Organic matter (OM) is abundant in ultrafine particles, and 77% of the particulate mass with diameter (Dp) of around 30 nm is composed of OM. A large fraction of coarse particle mass is undetermined and is assumed to be insoluble mineral dust and liquid water. The campaign's average size distribution of κ values shows three distinct modes: a less hygroscopic mode (Dp < 150 nm) with κ slightly above 0.2, a highly hygroscopic mode (150 nm < Dp < 1 μm) with κ greater than 0.3 and a nearly hydrophobic mode (Dp > 1 μm) with κ of about 0.1. The peak of the κ curve appears around 450 nm with a maximum value of 0.35. The derived κ values are consistent with results measured with a high humidity tandem differential mobility analyzer within the size range of 50–250 nm. Inorganics are the predominant species contributing to particle hygroscopicity, especially for particles between 150 nm and 1 μm. For example, NH4NO3, H2SO4, NH4HSO4 and (NH4)2SO4 account for nearly 90% of κ for particles of around 900 nm. For ultrafine particles, WSOC plays a critical role in particle hygroscopicity due to the predominant mass fraction of OM in ultrafine particles. WSOC for particles of around 30 nm contribute 52% of κ. Aerosol hygroscopicity is related to synoptic transport patterns. When southerly wind dominates, particles are more hygroscopic; when northerly wind dominates, particles are less hygroscopic. Aerosol hygroscopicity also has a diurnal variation, which can be explained by the diurnal evolution of planetary boundary layer, photochemical aging processes during daytime and enhanced black carbon emission at night. κ is highly correlated with mass fractions of SO42−, NO3− and NH4+ for all sampled particles as well as with the mass fraction of WSOC for particles of less than 100 nm. A parameterization scheme for κ is developed using mass fractions of SO42−, NO3−, NH4+ and WSOC due to their high correlations with κ, and κ calculated from the parameterization agrees well with κ derived from the particle's chemical composition. Further analysis shows that the parameterization scheme is applicable to other aerosol studies in China.
- ItemSeasonal and diurnal variations of particulate nitrate and organic matter at the IfT research station Melpitz(München : European Geopyhsical Union, 2011) Poulain, L.; Spindler, G.; Birmili, W.; Plass-Dülmer, C.; Weinhold, K.; Wiedensohler, A.; Herrmann, H.Ammonium nitrate and several organic compounds such as dicarboxylic acids (e.g. succinic acid, glutaric acid), some Polycyclic Aromatic Hydrocarbon (PAHs) or some n-alkanes are semi-volatile. The transition of these compounds between the gas and particulate phase may significantly change the aerosol particles radiative properties, the heterogeneous chemical properties, and, naturally, the total particulate mass concentration. To better assess these time-dependent effects, three intensive field experiments were conducted in 2008–2009 at the Central European EMEP research station Melpitz (Germany) using an Aerodyne Aerosol Mass Spectrometer (AMS). Data from all seasons highlight organic matter as being the most important particulate fraction of PM1 in summer (59%) while in winter, the nitrate fraction was more prevalent (34.4%). The diurnal variation of nitrate always showed the lowest concentration during the day while its concentration increased during the night. This night increase of nitrate concentration was higher in winter (ΔNO3− = 3.6 μg m−3) than in summer (ΔNO3− = 0.7 μg m−3). The variation in particulate nitrate was inherently linked to the gas-to-particle-phase equilibrium of ammonium nitrate and the dynamics of the atmosphere during day. The results of this study suggest that during summer nights, the condensation of HNO3 and NH3 on pre-existing particles represents the most prevalent source of nitrate, whereas during winter, nighttime chemistry is the predominant source of nitrate. During the summer 2008's campaign, a clear diurnal evolution in the oxidation state of the organic matter became evident (Organic Mass to Organic Carbon ratio (OM/OC) ranging from 1.65 during night to 1.80 during day and carbon oxidation state (OSc) from −0.66 to −0.4), which could be correlated to hydroxyl radical (OH) and ozone concentrations, indicating a photochemical transformation process. In summer, the organic particulate matter seemed to be heavily influenced by regional secondary formation and transformation processes, facilitated by photochemical production processes as well as a diurnal cycling of the substances between the gas and particulate phase. In winter, these processes were obviously less pronounced (OM/OC ranging from 1.60 to 1.67 and OSc from −0.8 to −0.7), so that organic matter apparently originated mainly from aged particles and long range transport.
- ItemRelating particle hygroscopicity and CCN activity to chemical composition during the HCCT-2010 field campaign(München : European Geopyhsical Union, 2013) Wu, Z.J.; Poulain, L.; Henning, S.; Dieckmann, K.; Birmili, W.; Merkel, M.; van Pinxteren, D.; Spindler, G.; Müller, K.; Stratmann, F.; Herrmann, H.; Wiedensohler, A.Particle hygroscopic growth at 90% RH (relative humidity), cloud condensation nuclei (CCN) activity, and size-resolved chemical composition were concurrently measured in the Thüringer Wald mid-level mountain range in central Germany in the fall of 2010. The median hygroscopicity parameter values, κ, of 50, 75, 100, 150, 200, and 250 nm particles derived from hygroscopicity measurements are respectively 0.14, 0.14, 0.17, 0.21, 0.24, and 0.28 during the sampling period. The closure between HTDMA (Hygroscopicity Tandem Differential Mobility Analyzers)-measured (κHTDMA) and chemical composition-derived (κchem) hygroscopicity parameters was performed based on the Zdanovskii–Stokes–Robinson (ZSR) mixing rule. Using size-averaged chemical composition, the κ values are substantially overpredicted (30 and 40% for 150 and 100 nm particles). Introducing size-resolved chemical composition substantially improved closure. We found that the evaporation of NH4NO3, which may happen in a HTDMA system, could lead to a discrepancy in predicted and measured particle hygroscopic growth. The hygroscopic parameter of the organic fraction, κorg, is positively correlated with the O : C ratio (κorg = 0.19 × (O : C) − 0.03). Such correlation is helpful to define the κorg value in the closure study. κ derived from CCN measurement was around 30% (varied with particle diameters) higher than that determined from particle hygroscopic growth measurements (here, hydrophilic mode is considered only). This difference might be explained by the surface tension effects, solution non-ideality, gas-particle partitioning of semivolatile compounds, and the partial solubility of constituents or non-dissolved particle matter. Therefore, extrapolating from HTDMA data to properties at the point of activation should be done with great care. Finally, closure study between CCNc (cloud condensation nucleus counter)-measured (κCCN) and chemical composition (κCCN, chem) was performed using CCNc-derived κ values for individual components. The results show that the κCCN can be well predicted using particle size-resolved chemical composition and the ZSR mixing rule.