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- ItemSea salt emission, transport and influence on size-segregated nitrate simulation: A case study in northwestern Europe by WRF-Chem(München : European Geopyhsical Union, 2016) Chen, Ying; Cheng, Yafang; Ma, Nan; Wolke, Ralf; Nordmann, Stephan; Schüttauf, Stephanie; Ran, Liang; Wehner, Birgit; Birmili, Wolfram; van der Gon, Hugo A.C. Denier; Mu, Qing; Barthel, Stefan; Spindler, Gerald; Stieger, Bastian; Müller, Konrad; Zheng, Guang-Jie; Pöschl, Ulrich; Su, Hang; Wiedensohler, AlfredSea salt aerosol (SSA) is one of the major components of primary aerosols and has significant impact on the formation of secondary inorganic particles mass on a global scale. In this study, the fully online coupled WRF-Chem model was utilized to evaluate the SSA emission scheme and its influence on the nitrate simulation in a case study in Europe during 10–20 September 2013. Meteorological conditions near the surface, wind pattern and thermal stratification structure were well reproduced by the model. Nonetheless, the coarse-mode (PM1 − 10) particle mass concentration was substantially overestimated due to the overestimation of SSA and nitrate. Compared to filter measurements at four EMEP stations (coastal stations: Bilthoven, Kollumerwaard and Vredepeel; inland station: Melpitz), the model overestimated SSA concentrations by a factor of 8–20. We found that this overestimation was mainly caused by overestimated SSA emissions over the North Sea during 16–20 September. Over the coastal regions, SSA was injected into the continental free troposphere through an “aloft bridge” (about 500 to 1000 m above the ground), a result of the different thermodynamic properties and planetary boundary layer (PBL) structure between continental and marine regions. The injected SSA was further transported inland and mixed downward to the surface through downdraft and PBL turbulence. This process extended the influence of SSA to a larger downwind region, leading, for example, to an overestimation of SSA at Melpitz, Germany, by a factor of ∼ 20. As a result, the nitrate partitioning fraction (ratio between particulate nitrate and the summation of particulate nitrate and gas-phase nitric acid) increased by about 20 % for the coarse-mode nitrate due to the overestimation of SSA at Melpitz. However, no significant difference in the partitioning fraction for the fine-mode nitrate was found. About 140 % overestimation of the coarse-mode nitrate resulted from the influence of SSA at Melpitz. In contrast, the overestimation of SSA inhibited the nitrate particle formation in the fine mode by about 20 % because of the increased consumption of precursor by coarse-mode nitrate formation.
- ItemAerosol pollution maps and trends over Germany with hourly data at four rural background stations from 2009 to 2018(Katlenburg-Lindau : EGU, 2020) Heintzenberg, Jost; Birmili, Wolfram; Hellack, Bryan; Spindler, Gerald; Tuch, Thomas; Wiedensohler, AlfredA total of 10 years of hourly aerosol and gas data at four rural German stations have been combined with hourly back trajectories to the stations and inventories of the European Emissions Database for Global Atmospheric Research (EDGAR), yielding pollution maps over Germany of PM10, particle number concentrations, and equivalent black carbon (eBC). The maps reflect aerosol emissions modified with atmospheric processes during transport between sources and receptor sites. Compared to emission maps, strong western European emission centers do not dominate the downwind concentrations because their emissions are reduced by atmospheric processes on the way to the receptor area. PM10, eBC, and to some extent also particle number concentrations are rather controlled by emissions from southeastern Europe from which pollution transport often occurs under drier conditions. Newly formed particles are found in air masses from a broad sector reaching from southern Germany to western Europe, which we explain with gaseous particle precursors coming with little wet scavenging from this region. Annual emissions for 2009 of PM10, BC, SO2, and NOx were accumulated along each trajectory and compared with the corresponding measured time series. The agreement of each pair of time series was optimized by varying monthly factors and annual factors on the 2009 emissions. This approach yielded broader summer emission minima than published values that were partly displaced from the midsummer positions. The validity of connecting the ambient concentration and emission of particulate pollution was tested by calculating temporal changes in eBC for subsets of back trajectories passing over two separate prominent emission regions, region A to the northwest and B to the southeast of the measuring stations. Consistent with reported emission data the calculated emission decreases over region A are significantly stronger than over region B.
- ItemRespiratory tract deposition of inhaled roadside ultrafine refractory particles in a polluted megacity of South-East Asia(Amsterdam [u.a.] : Elsevier Science, 2019) Kecorius, Simonas; Madueño, Leizel; Löndahl, Jakob; Vallar, Edgar; Galvez, Maria Cecilia; Idolor, Luisito F.; Gonzaga-Cayetano, Mylene; Müller, Thomas; Birmili, Wolfram; Wiedensohler, AlfredRecent studies demonstrate that Black Carbon (BC) pollution in economically developing megacities remain higher than the values, which the World Health Organization considers to be safe. Despite the scientific evidence of the degrees of BC exposure, there is still a lack of understanding on how the severe levels of BC pollution affect human health in these regions. We consider information on the respiratory tract deposition dose (DD) of BC to be essential in understanding the link between personal exposure to air pollutants and corresponding health effects. In this work, we combine data on fine and ultrafine refractory particle number concentrations (BC proxy), and activity patterns to derive the respiratory tract deposited amounts of BC particles for the population of the highly polluted metropolitan area of Manila, Philippines. We calculated the total DD of refractory particles based on three metrics: refractory particle number, surface area, and mass concentrations. The calculated DD of total refractory particle number in Metro Manila was found to be 1.6 to 17 times higher than average values reported from Europe and the U.S. In the case of Manila, ultrafine particles smaller than 100 nm accounted for more than 90% of the total deposited refractory particle dose in terms of particle number. This work is a first attempt to quantitatively evaluate the DD of refractory particles and raise awareness in assessing pollution-related health effects in developing megacities. We demonstrate that the majority of the population may be highly affected by BC pollution, which is known to have negative health outcomes if no actions are taken to mitigate its emission. For the governments of such metropolitan areas, we suggest to revise currently existing environmental legislation, raise public awareness, and to establish supplementary monitoring of black carbon in parallel to already existing PM 10 and PM 2.5 measures. © 2019
- ItemA parameterization of the heterogeneous hydrolysis of N2O5 for mass-based aerosol models: Improvement of particulate nitrate prediction(Katlenburg-Lindau : EGU, 2018) Chen, Ying; Wolke, Ralf; Ran, Liang; Birmili, Wolfram; Spindler, Gerald; Schröder, Wolfram; Su, Hang; Cheng, Yafang; Tegen, Ina; Wiedensohler, AlfredThe heterogeneous hydrolysis of N2O5 on the surface of deliquescent aerosol leads to HNO3 formation and acts as a major sink of NOx in the atmosphere during night-time. The reaction constant of this heterogeneous hydrolysis is determined by temperature (T), relative humidity (RH), aerosol particle composition, and the surface area concentration (S). However, these parameters were not comprehensively considered in the parameterization of the heterogeneous hydrolysis of N2O5 in previous mass-based 3-D aerosol modelling studies. In this investigation, we propose a sophisticated parameterization (NewN2O5) of N2O5 heterogeneous hydrolysis with respect to T, RH, aerosol particle compositions, and S based on laboratory experiments. We evaluated closure between NewN2O5 and a state-of-the-art parameterization based on a sectional aerosol treatment. The comparison showed a good linear relationship (R Combining double low line 0.91) between these two parameterizations. NewN2O5 was incorporated into a 3-D fully online coupled model, COSMO-Muscat, with the mass-based aerosol treatment. As a case study, we used the data from the HOPE Melpitz campaign (10-25 September 2013) to validate model performance. Here, we investigated the improvement of nitrate prediction over western and central Europe. The modelled particulate nitrate mass concentrations ([NO3-]) were validated by filter measurements over Germany (Neuglobsow, Schmücke, Zingst, and Melpitz). The modelled [NO3-] was significantly overestimated for this period by a factor of 5-19, with the corrected NH3 emissions (reduced by 50 %) and the original parameterization of N2O5 heterogeneous hydrolysis. The NewN2O5 significantly reduces the overestimation of [NO3-] by ∼ 35 %. Particularly, the overestimation factor was reduced to approximately 1.4 in our case study (12, 17-18 and 25 September 2013) when [NO3-] was dominated by local chemical formations. In our case, the suppression of organic coating was negligible over western and central Europe, with an influence on [NO3-] of less than 2 % on average and 20 % at the most significant moment. To obtain a significant impact of the organic coating effect, N2O5, SOA, and NH3 need to be present when RH is high and T is low. However, those conditions were rarely fulfilled simultaneously over western and central Europe. Hence, the organic coating effect on the reaction probability of N2O5 may not be as significant as expected over western and central Europe.
- ItemSource apportionment and impact of long-range transport on carbonaceous aerosol particles in central Germany during HCCT-2010(Katlenburg-Lindau : EGU, 2021) Poulain, Laurent; Fahlbusch, Benjamin; Spindler, Gerald; Mueller, Konrad; van Pinxteren, Dominik; Wu, Zhijun; Iinuma, Yoshiteru; Birmili, Wolfram; Wiedensohler, Alfred; Herrmann, HartmutThe identification of different sources of the carbonaceous aerosol (organics and black carbon) was investigated at a mountain forest site located in central Germany from September to October 2010 to characterize incoming air masses during the Hill Cap Cloud Thuringia 2010 (HCCT-2010) experiment. The near-PM1 chemical composition, as measured by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), was dominated by organic aerosol (OA; 41 %) followed by sulfate (19 %) and nitrate (18 %). Source apportionment of the OA fraction was performed using the multilinear engine (ME-2) approach, resulting in the identification of the following five factors: hydrocarbon-like OA (HOA; 3 % of OA mass), biomass burning OA (BBOA; 13 %), semi-volatile-like OA (SV-OOA; 19 %), and two oxygenated OA (OOA) factors. The more oxidized OOA (MO-OOA, 28 %) was interpreted as being influenced by aged, polluted continental air masses, whereas the less oxidized OOA (LO-OOA, 37 %) was found to be more linked to aged biogenic sources. Equivalent black carbon (eBC), measured by a multi-angle absorption photometer (MAAP) represented 10 % of the total particulate matter (PM). The eBC was clearly associated with HOA, BBOA, and MO-OOA factors (all together R2=0.83). Therefore, eBC's contribution to each factor was achieved using a multi-linear regression model. More than half of the eBC (52 %) was associated with long-range transport (i.e., MO-OOA), whereas liquid fuel eBC (35 %) and biomass burning eBC (13 %) were associated with local emissions, leading to a complete apportionment of the carbonaceous aerosol. The separation between local and transported eBC was well supported by the mass size distribution of elemental carbon (EC) from Berner impactor samples. Air masses with the strongest marine influence, based on back trajectory analysis, corresponded with a low particle mass concentration (6.4–7.5 µg m−3) and organic fraction (≈30 %). However, they also had the largest contribution of primary OA (HOA ≈ 4 % and BBOA 15 %–20 %), which was associated with local emissions. Continental air masses had the highest mass concentration (11.4–12.6 µg m−3), and a larger fraction of oxygenated OA (≈45 %) indicated highly processed OA. The present results emphasize the key role played by long-range transport processes not only in the OA fraction but also in the eBC mass concentration and the importance of improving our knowledge on the identification of eBC sources.
- ItemLong-term observations of tropospheric particle number size distributions and equivalent black carbon mass concentrations in the German Ultrafine Aerosol Network (GUAN)(München : European Geopyhsical Union, 2016) Birmili, Wolfram; Weinhold, Kay; Rasch, Fabian; Sonntag, André; Sun, Jia; Merkel, Maik; Wiedensohler, Alfred; Bastian, Susanne; Schladitz, Alexander; Löschau, Gunter; Cyrys, Josef; Pitz, Mike; Gu, Jianwei; Kusch, Thomas; Flentje, Harald; Quass, Ulrich; Kaminski, Heinz; Kuhlbusch, Thomas A.J.; Meinhardt, Frank; Schwerin, Andreas; Bath, Olaf; Ries, Ludwig; Gerwig, Holger; Wirtz, Klaus; Fiebig, MarkusThe German Ultrafine Aerosol Network (GUAN) is a cooperative atmospheric observation network, which aims at improving the scientific understanding of aerosol-related effects in the troposphere. The network addresses research questions dedicated to both climate- and health-related effects. GUAN's core activity has been the continuous collection of tropospheric particle number size distributions and black carbon mass concentrations at 17 observation sites in Germany. These sites cover various environmental settings including urban traffic, urban background, rural background, and Alpine mountains. In association with partner projects, GUAN has implemented a high degree of harmonisation of instrumentation, operating procedures, and data evaluation procedures. The quality of the measurement data is assured by laboratory intercomparisons as well as on-site comparisons with reference instruments. This paper describes the measurement sites, instrumentation, quality assurance, and data evaluation procedures in the network as well as the EBAS repository, where the data sets can be obtained (doi:10.5072/guan).
- ItemSignificant increase of aerosol number concentrations in air masses crossing a densely trafficked sea area(Amsterdam : Elsevier, 2015) Kecorius, Simonas; Kivekäs, Niku; Kristensson, Adam; Tuch, Thomas; Covert, David S.; Birmili, Wolfram; Lihavainen, Heikki; Hyvärinen, Antti-Pekka; Martinsson, Johan; Sporre, Moa K.; Swietlicki, Erik; Wiedensohler, Alfred; Ulevicius, VidmantasIn this study, we evaluated 10 months data (September 2009 to June 2010) of atmospheric aerosol particle number size distribution at three atmospheric observation stations along the Baltic Sea coast: Vavihill (upwind, Sweden), Utö (upwind, Finland), and Preila (downwind, Lithuania). Differences in aerosol particle number size distributions between the upwind and downwind stations during situations of connected atmospheric flow, when the air passed each station, were used to assess the contribution of ship emissions to the aerosol number concentration (diameter interval 50–400 nm) in the Lithuanian background coastal environment. A clear increase in particle number concentration could be noticed, by a factor of 1.9 from Utö to Preila (the average total number concentration at Utö was 791 cm−3), and by a factor of 1.6 from Vavihill to Preila (the average total number concentration at Vavihill was 998 cm−3). The simultaneous measurements of absorption Ångström exponents close to unity at Preila supported our conclusion that ship emissions in the Baltic Sea contributed to the increase in particle number concentration at Preila.
- ItemDecreasing trends of particle number and black carbon mass concentrations at 16 observational sites in Germany from 2009 to 2018(Katlenburg-Lindau : EGU, 2020) Sun, Jia; Birmili, Wolfram; Hermann, Markus; Tuch, Thomas; Weinhold, Kay; Merkel, Maik; Rasch, Fabian; Müller, Thomas; Schladitz, Alexander; Bastian, Susanne; Löschau, Gunter; Cyrys, Josef; Gu, Jianwei; Flentje, Harald; Briel, Björn; Asbach, Christoph; Kaminski, Heinz; Ries, Ludwig; Sohmer, Ralf; Gerwig, Holger; Wirtz, Klaus; Meinhardt, Frank; Schwerin, Andreas; Bath, Olaf; Ma, Nan; Wiedensohler, AlfredAnthropogenic emissions are dominant contributors to air pollution. Consequently, mitigation policies have been attempted since the 1990s in Europe to reduce pollution by anthropogenic emissions. To evaluate the effectiveness of these mitigation policies, the German Ultrafine Aerosol Network (GUAN) was established in 2008, focusing on black carbon (BC) and sub-micrometre aerosol particles. In this study, long-term trends of atmospheric particle number concentrations (PNCs) and equivalent BC (eBC) mass concentration over a 10-year period (2009-2018) were determined for 16 GUAN sites ranging from roadside to high Alpine environments. Overall, statistically significant decreasing trends are found for most of these parameters and environments in Germany. The annual relative slope of eBC mass concentration varies between-13.1% and-1.7% per year. The slopes of the PNCs vary from-17.2% to-1.7 %,-7.8% to-1.1 %, and-11.1% to-1.2% per year for 10-30, 30-200, and 200-800 nm size ranges, respectively. The reductions in various anthropogenic emissions are found to be the dominant factors responsible for the decreasing trends of eBC mass concentration and PNCs. The diurnal and seasonal variations in the trends clearly show the effects of the mitigation policies for road transport and residential emissions. The influences of other factors such as air masses, precipitation, and temperature were also examined and found to be less important or negligible. This study proves that a combination of emission mitigation policies can effectively improve the air quality on large spatial scales. It also suggests that a long-term aerosol measurement network at multi-type sites is an efficient and necessary tool for evaluating emission mitigation policies. © 2020 Author(s).
- ItemEvaluation of the size segregation of elemental carbon (EC) emission in Europe: Influence on the simulation of EC long-range transportation(München : European Geopyhsical Union, 2016) Chen, Ying; Cheng, Ya-Fang; Nordmann, Stephan; Birmili, Wolfram; van der Gon, Hugo A.C. Denier; Ma, Nan; Wolke, Ralf; Wehner, Birgit; Sun, Jia; Spindler, Gerald; Mu, Qing; Pöschl, Ulrich; Su, Hang; Wiedensohler, AlfredElemental Carbon (EC) has a significant impact on human health and climate change. In order to evaluate the size segregation of EC emission in the EUCAARI inventory and investigate its influence on the simulation of EC long-range transportation in Europe, we used the fully coupled online Weather Research and Forecasting/Chemistry model (WRF-Chem) at a resolution of 2 km focusing on a region in Germany, in conjunction with a high-resolution EC emission inventory. The ground meteorology conditions, vertical structure and wind pattern were well reproduced by the model. The simulations of particle number and/or mass size distributions were evaluated with observations at the central European background site Melpitz. The fine mode particle concentration was reasonably well simulated, but the coarse mode was substantially overestimated by the model mainly due to the plume with high EC concentration in coarse mode emitted by a nearby point source. The comparisons between simulated EC and Multi-angle Absorption Photometers (MAAP) measurements at Melpitz, Leipzig-TROPOS and Bösel indicated that the coarse mode EC (ECc) emitted from the nearby point sources might be overestimated by a factor of 2–10. The fraction of ECc was overestimated in the emission inventory by about 10–30 % for Russia and 5–10 % for Eastern Europe (e.g., Poland and Belarus). This incorrect size-dependent EC emission results in a shorter atmospheric life time of EC particles and inhibits the long-range transport of EC. A case study showed that this effect caused an underestimation of 20–40 % in the EC mass concentration in Germany under eastern wind pattern.
- ItemAerosol particle mixing state, refractory particle number size distributions and emission factors in a polluted urban environment: Case study of Metro Manila, Philippines(Oxford [u.a.] : Elsevier, 2017) Kecorius, Simonas; Madueño, Leizel; Vallar, Edgar; Alas, Honey; Betito, Grace; Birmili, Wolfram; Cambaliza, Maria Obiminda; Catipay, Grethyl; Gonzaga-Cayetano, Mylene; Galvez, Maria Cecilia; Lorenzo, Genie; Müller, Thomas; Simpas, James B.; Tamayo, Everlyn Gayle; Wiedensohler, AlfredUltrafine soot particles (black carbon, BC) in urban environments are related to adverse respiratory and cardiovascular effects, increased cases of asthma and premature deaths. These problems are especially pronounced in developing megacities in South-East Asia, Latin America, and Africa, where unsustainable urbanization ant outdated environmental protection legislation resulted in severe degradation of urban air quality in terms of black carbon emission. Since ultrafine soot particles do often not lead to enhanced PM10 and PM2.5 mass concentration, the risks related to ultrafine particle pollution may therefore be significantly underestimated compared to the contribution of secondary aerosol constituents. To increase the awareness of the potential toxicological relevant problems of ultrafine black carbon particles, we conducted a case study in Metro Manila, the capital of the Philippines. Here, we present a part of the results from a detailed field campaign, called Manila Aerosol Characterization Experiment (MACE, 2015). Measurements took place from May to June 2015 with the focus on the state of mixing of aerosol particles. The results were alarming, showing the abundance of externally mixed refractory particles (soot proxy) at street site with a maximum daily number concentration of approximately 15000 #/cm3. That is up to 10 times higher than in cities of Western countries. We also found that the soot particle mass contributed from 55 to 75% of total street site PM2.5. The retrieved refractory particle number size distribution appeared to be a superposition of 2 ultrafine modes at 20 and 80 nm with a corresponding contribution to the total refractory particle number of 45 and 55%, respectively. The particles in the 20 nm mode were most likely ash from metallic additives in lubricating oil, tiny carbonaceous particles and/or nucleated and oxidized organic polymers, while bigger ones (80 nm) were soot agglomerates. To the best of the authors’ knowledge, no other studies reported such high number concentration of ultrafine refractory particles under ambient conditions. Inverse modeling of emission factors of refractory particle number size distributions revealed that diesel-fed public utility Jeepneys, commonly used for public transportation, are responsible for 94% of total roadside emitted refractory particle mass. The observed results showed that the majority of urban pollution in Metro Manila is dominated by carbonaceous aerosol. This suggests that PM10 or PM2.5 metrics do not fully describe possible health related effects in this kind of urban environments. Extremely high concentrations of ultrafine particles have been and will continue to induce adverse health related effects, because of their potential toxicity. We imply that in megacities, where the major fraction of particulates originates from the transport sector, PM10 or PM2.5 mass concentration should be complemented by legislative measurements of equivalent black carbon mass concentration.