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Veröffentlichung Ultrafine Particles Pollution and Measurements(2016) Kumar, P.; Birmili, Wolfram; Wiedensohler, A.; Quincey, P.; Hallquist, M.Veröffentlichung Long-term observations of tropospheric particle number size distributions and equivalent black carbon mass concentrations in the German Ultrafine Aerosol Network (GUAN)(2016) Weinhold, Kay; Bath, Olaf; Rasch, Fabian; Birmili, Wolfram; Sonntag, Andre; Sun, Jia; Merkel, Maik; Wiedensohler, Alfred; Gerwig, Holger; Bastian, Susanne; Schladitz, Alexander; Löschau, Gunter; Cyrys, Josef; Pitz, Mike; Gu, Jianwei; Kusch, Thomas; Flentje, Harald; Quass, Ulrich; Kaminski, Heinz; Kuhlbusch, Thomas A.J.; Ries, Ludwig; Meinhardt, Frank; Schwerin, Andreas; Fiebig, Markus; Wirtz, KlausThe 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. Quelle: http://www.earth-syst-sci-data.netVeröffentlichung Evaluation of the size segregation of elemental carbon (EC) emission in Europe: influence on the simulation of EC long-range transportation(2016) Chen, Ying-Yuan; Birmili, Wolfram; Cheng, Ya-Fang; Denier van der Gon, Hugo A.C.; Ma, Nan; Wolke, Ralf; Nordmann, Stephan; 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.Quelle: http://www.atmos-chem-phys.netVeröffentlichung Sea salt emission, transport and influence on size-segregated nitrate simulation: a case study in northwestern Europe by WRF-Chem(2016) Chen, Ying-Yuan; Barthel, Stefan; Cheng, Yafang; Birmili, Wolfram; Ma, Nan; Wolke, Ralf; Schüttauf, Stephanie; Ran, Liang; Wehner, Birgit; Nordmann, Stephan; Denier van der Gon, Hugo A.C.; Mu, Quing; 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 bridgeŁ (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.Quelle: http://www.atmos-chem-phys.netVeröffentlichung Contributions of volatile and nonvolatile compounds (at 300˚C) to condensational growth of atmospheric nanoparticles: An assessment based on 8.5 years of observations at the Central Europe background site Melpitz(2017) Wang, Zhibin; Birmili, Wolfram; Hamed, ArmarLong-term measurements of particle number size distributions in combination with thermodenuder analysis have been performed since July 2003 at the Central European station of Melpitz, Germany. Up to the end of 2011, 20% of all investigated days during the 8.5?years of measurements showed new particle formation and subsequent growth. To investigate the role of various chemical compound candidates for condensational nanoparticle growth, we focused on nucleation events in which the measured size distributions with and without thermodesorption both showed growth patterns (accounting for up to ~85% of all nucleation events). In this study, particulate compounds that volatilize at 300˚C were specifically defined as ̮volatile,Ł in contrast to ̮nonvolatileŁ compounds, which remain in the particulate phase after being heated to 300˚C. A strong correlation between ambient temperature and growth rate associated with volatile substances (except gaseous sulfuric acid) was found, which implies the importance of organics (possibly oxidized biogenic organic compounds) in particle growth at Melpitz. The contributions of the volatile compounds to the growth rate due to condensation of gaseous sulfuric acid and organics were found to be about 19% and 47%, respectively. The remaining ~25% was attributed to nonvolatile residuals, which appear to form gradually during the particle growth process and are characterized as extremely low-volatility compounds. The growth rate associated with volatile components exhibited significant seasonal variation, with the highest value during summertime, whereas the growth rate associated with the nonvolatile fraction showed less fluctuation. Quelle: http://onlinelibrary.wiley.comVeröffentlichung Mobility particle size spectrometers(2018) Wiedensohler, A.; Birmili, Wolfram; Wiesner, A.; Weinhold, K.Mobility particle size spectrometers (MPSS) belong to the essential instruments in aerosol science that determine the particle number size distribution (PNSD) in the submicrometer size range. Following calibration procedures and target uncertainties against standards and reference instruments are suggested for a complete MPSS quality assurance program: (a) calibration of the CPC counting efficiency curve (within 5% for the plateau counting efficiency; within 1 nm for the 50% detection efficiency diameter), (b) sizing calibration of the MPSS, using a certified polystyrene latex (PSL) particle size standard at 203 nm (within 3%), (c) intercomparison of the PNSD of the MPSS (within 10% and 20% of the dN/dlogDP concentration for the particle size range 20Ń200 and 200Ń800 nm, respectively), and (d) intercomparison of the integral PNC of the MPSS (within 10%). Furthermore, following measurement uncertainties have been investigated: (a) PSL particle size standards in the range from 100 to 500 nm match within 1% after sizing calibration at 203 nm. (b) Bipolar diffusion chargers based on the radioactive nuclides Kr85, Am241, and Ni63 and a new ionizer based on corona discharge follow the recommended bipolar charge distribution, while soft X-ray-based charges may alter faster than expected. (c) The use of a positive high voltage supply show a 10% better performance than a negative one. (d) The intercomparison of the integral PNC of an MPSS against the total number concentration is still within the target uncertainty at an ambient pressure of approximately 500 hPa. Quelle: VerlagsinformationVeröffentlichung Aerosol particle mixing state, refractory particle number size distributions and emission factors in a polluted urban environment(2017) Kecorius, Simonas; Birmili, Wolfram; Madueno, Leizel; Vallar, EdgarVeröffentlichung Effect of Prudhoe Bay emissions on atmospheric aerosol growth events observed in Utqiagvik (Barrow), Alaska(2017) Kolesar, Katheryn R.; Birmili, Wolfram; Cellini, Jillian; Peterson, Peter K.Veröffentlichung A parameterization of the heterogeneous hydrolysis of N2O5 for mass-based aerosol models(2018) Chen, Ying-Yuan; Birmili, Wolfram; Wolke, Ralf; Ran, LiangThe 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?=??0.91) between these two parameterizations. NewN2O5 was incorporated into a 3-D fully online coupled model, COSMOŃMUSCAT, with the mass-based aerosol treatment. As a case study, we used the data from the HOPE Melpitz campaign (10Ń25 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 5Ń19, 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, 17Ń18 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. Quelle: https://www.atmos-chem-phys.net/Veröffentlichung Atmospheric new particle formation at the research station Melpitz, Germany(2018) Größ, Johannes; Birmili, Wolfram; Hamed, Amar; Sonntag, AndreThis paper revisits the atmospheric new particle formation (NPF) process in the polluted Central European troposphere, focusing on the connection with gas-phase precursors and meteorological parameters. Observations were made at the research station Melpitz (former East Germany) between 2008 and 2011 involving a neutral cluster and air ion spectrometer (NAIS). Particle formation events were classified by a new automated method based on the convolution integral of particle number concentration in the diameter interval 2Ń20?nm. To study the relevance of gaseous sulfuric acid as a precursor for nucleation, a proxy was derived on the basis of direct measurements during a 1-month campaign in May 2008. As a major result, the number concentration of freshly produced particles correlated significantly with the concentration of sulfur dioxide as the main precursor of sulfuric acid. The condensation sink, a factor potentially inhibiting NPF events, played a subordinate role only. The same held for experimentally determined ammonia concentrations. The analysis of meteorological parameters confirmed the absolute need for solar radiation to induce NPF events and demonstrated the presence of significant turbulence during those events. Due to its tight correlation with solar radiation, however, an independent effect of turbulence for NPF could not be established. Based on the diurnal evolution of aerosol, gas-phase, and meteorological parameters near the ground, we further conclude that the particle formation process is likely to start in elevated parts of the boundary layer rather than near ground level. Quelle: Verlagsinformation