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- ItemA case of extreme particulate matter concentrations over Central Europe caused by dust emitted over the southern Ukraine(München : European Geopyhsical Union, 2008) Birmili, W.; Schepanski, K.; Ansmann, A.; Spindler, G.; Tegen, I.; Wehner, B.; Nowak, A.; Reimer, E.; Mattis, I.; Müller, K.; Brüggemann, E.; Gnauk, T.; Herrmann, H.; Wiedensohler, A.; Althausen, D.; Schladitz, A.; Tuch, T.; Löschau, G.On 24 March 2007, an extraordinary dust plume was observed in the Central European troposphere. Satellite observations revealed its origins in a dust storm in Southern Ukraine, where large amounts of soil were resuspended from dried-out farmlands at wind gusts up to 30 m s−1. Along the pathway of the plume, maximum particulate matter (PM10) mass concentrations between 200 and 1400 μg m−3 occurred in Slovakia, the Czech Republic, Poland, and Germany. Over Germany, the dust plume was characterised by a volume extinction coefficient up to 400 Mm−1 and a particle optical depth of 0.71 at wavelength 0.532 μm. In-situ size distribution measurements as well as the wavelength dependence of light extinction from lidar and Sun photometer measurements confirmed the presence of a coarse particle mode with diameters around 2–3 μm. Chemical particle analyses suggested a fraction of 75% crustal material in daily average PM10 and up to 85% in the coarser fraction PM10–2.5. Based on the particle characteristics as well as a lack of increased CO and CO2 levels, a significant impact of biomass burning was ruled out. The reasons for the high particle concentrations in the dust plume were twofold: First, dust was transported very rapidly into Central Europe in a boundary layer jet under dry conditions. Second, the dust plume was confined to a relatively stable boundary layer of 1.4–1.8 km height, and could therefore neither expand nor dilute efficiently. Our findings illustrate the capacity of combined in situ and remote sensing measurements to characterise large-scale dust plumes with a variety of aerosol parameters. Although such plumes from Southern Eurasia seem to occur rather infrequently in Central Europe, its unexpected features highlights the need to improve the description of dust emission, transport and transformation processes needs, particularly when facing the possible effects of further anthropogenic desertification and climate change.
- ItemFirst long-term study of particle number size distributions and new particle formation events of regional aerosol in the North China Plain(München : European Geopyhsical Union, 2011) Shen, X.J.; Sun, J.Y.; Zhang, Y.M.; Wehner, B.; Nowak, A.; Tuch, T.; Zhang, X.C.; Wang, T.T.; Zhou, H.G.; Zhang, X.L.; Dong, F.; Birmili, W.; Wiedensohler, A.Atmospheric particle number size distributions (size range 0.003–10 μm) were measured between March 2008 and August 2009 at Shangdianzi (SDZ), a rural research station in the North China Plain. These measurements were made in an attempt to better characterize the tropospheric background aerosol in Northern China. The mean particle number concentrations of the total particle, as well as the nucleation, Aitken, accumulation and coarse mode were determined to be 1.2 ± 0.9 × 104, 3.6 ± 7.9 × 103, 4.4 ± 3.4 × 103, 3.5 ± 2.8 × 103 and 2 ± 3 cm−3, respectively. A general finding was that the particle number concentration was higher during spring compared to the other seasons. The air mass origin had an important effect on the particle number concentration and new particle formation events. Air masses from northwest (i.e. inner Asia) favored the new particle formation events, while air masses from southeast showed the highest particle mass concentration. Significant diurnal variations in particle number were observed, which could be linked to new particle formation events, i.e. gas-to-particle conversion. During particle formation events, the number concentration of the nucleation mode rose up to maximum value of 104 cm−3. New particle formation events were observed on 36% of the effective measurement days. The formation rate ranged from 0.7 to 72.7 cm−3 s−1, with a mean value of 8.0 cm−3 s−1. The value of the nucleation mode growth rate was in the range of 0.3–14.5 nm h−1, with a mean value of 4.3 nm h−1. It was an essential observation that on many occasions the nucleation mode was able to grow into the size of cloud condensation nuclei (CCN) within a matter of several hours. Furthermore, the new particle formation was regularly followed by a measurable increase in particle mass concentration and extinction coefficient, indicative of a high abundance of condensable vapors in the atmosphere under study.
- ItemPrimary versus secondary contributions to particle number concentrations in the European boundary layer(München : European Geopyhsical Union, 2011) Reddington, C.L.; Carslaw, K.S.; Spracklen, D.V.; Frontoso, M.G.; Collins, L.; Merikanto, J.; Minikin, A.; Hamburger, T.; Coe, H.; Kulmala, M.; Aalto, P.; Flentje, H.; Plass-Dülmer, C.; Birmili, W.; Wiedensohler, A.; Wehner, B.; Tuch, T.; Sonntag, A.; O'Dowd, C.D.; Jennings, S.G.; Dupuy, R.; Baltensperger, U.; Weingartner, E.; Hansson, H.-C.; Tunved, P.; Laj, P.; Sellegri, K.; Boulon, J.; Putaud, J.-P.; Gruening, C.; Swietlicki, E.; Roldin, P.; Henzing, J.S.; Moerman, M.; Mihalopoulos, N.; Kouvarakis, G.; Ždímal, V.; Zíková, N.; Marinoni, A.; Bonasoni, P.; Duchi, R.It is important to understand the relative contribution of primary and secondary particles to regional and global aerosol so that models can attribute aerosol radiative forcing to different sources. In large-scale models, there is considerable uncertainty associated with treatments of particle formation (nucleation) in the boundary layer (BL) and in the size distribution of emitted primary particles, leading to uncertainties in predicted cloud condensation nuclei (CCN) concentrations. Here we quantify how primary particle emissions and secondary particle formation influence size-resolved particle number concentrations in the BL using a global aerosol microphysics model and aircraft and ground site observations made during the May 2008 campaign of the European Integrated Project on Aerosol Cloud Climate Air Quality Interactions (EUCAARI). We tested four different parameterisations for BL nucleation and two assumptions for the emission size distribution of anthropogenic and wildfire carbonaceous particles. When we emit carbonaceous particles at small sizes (as recommended by the Aerosol Intercomparison project, AEROCOM), the spatial distributions of campaign-mean number concentrations of particles with diameter >50 nm (N50) and >100 nm (N100) were well captured by the model (R2≥0.8) and the normalised mean bias (NMB) was also small (−18% for N50 and −1% for N100). Emission of carbonaceous particles at larger sizes, which we consider to be more realistic for low spatial resolution global models, results in equally good correlation but larger bias (R2≥0.8, NMB = −52% and −29%), which could be partly but not entirely compensated by BL nucleation. Within the uncertainty of the observations and accounting for the uncertainty in the size of emitted primary particles, BL nucleation makes a statistically significant contribution to CCN-sized particles at less than a quarter of the ground sites. Our results show that a major source of uncertainty in CCN-sized particles in polluted European air is the emitted size of primary carbonaceous particles. New information is required not just from direct observations, but also to determine the "effective emission size" and composition of primary particles appropriate for different resolution models.
- ItemTropospheric aerosol scattering and absorption over central Europe: A closure study for the dry particle state(München : European Geopyhsical Union, 2014) Ma, N.; Birmili, W.; Müller, T.; Tuch, T.; Cheng, Y.F.; Xu, W.Y.; Zhao, C.S.; Wiedensohler, A.This work analyses optical properties of the dry tropospheric aerosol measured at the regional Global Atmosphere Watch (GAW) observation site Melpitz in East Germany. For a continuous observation period between 2007 and 2010, we provide representative values of the dry-state scattering coefficient, hemispheric backscattering coefficient, absorption coefficient, single scattering albedo, and scattering Ångström exponent. Besides the direct measurement, the aerosol scattering coefficient was alternatively computed from experimental particle number size distributions using a Mie model. Within pre-defined limits, a closure could be achieved with the direct measurement. The achievement of closure implies that such calculations can be used as a high-level quality control measure for data sets involving multiple instrumentation. All dry-state optical properties show pronounced annual and diurnal variations, which are attributed to the corresponding variations in the regional emission fluxes, the intensity of secondary particle formation, and the mixing layer height. Air mass classification shows that atmospheric stability is a major factor influencing the dry aerosol properties at the GAW station. In the cold season, temperature inversions limit the volume available for atmospheric mixing, so that the dry-state aerosol optical properties near the ground proved quite sensitive to the geographical origin of the air mass. In the warm season, when the atmosphere is usually well-mixed during daytime, considerably less variability was observed for the optical properties between different air masses. This work provides, on the basis of quality-checked in situ measurements, a first step towards a climatological assessment of direct aerosol radiative forcing in the region under study.
- ItemMobility particle size spectrometers: Harmonization of technical standards and data structure to facilitate high quality long-term observations of atmospheric particle number size distributions(München : European Geopyhsical Union, 2012) Wiedensohler, A.; Birmili, W.; Nowak, A.; Sonntag, A.; Weinhold, K.; Merkel, M.; Wehner, B.; Tuch, T.; Pfeifer, S.; Fiebig, M.; Fjäraa, A.M.; Asmi, E.; Sellegri, K.; Depuy, R.; Venzac, H.; Villani, P.; Laj, P.; Aalto, P.; Ogren, J.A.; Swietlick, E.; Williams, P.; Roldin, P.; Quincey, P.; Hüglin, C.; Fierz-Schmidhauser, R.; Gysel, M.; Weingartner, E.; Riccobono, F.; Santos, S.; Grüning, C.; Faloon, K.; Beddows, D.; Harrison, R.; Monahan, C.; Jennings, S.G.; O'Dowd, C.D.; Marinoni, A.; Horn, H.-G.; Keck, L.; Jiang, J.; Scheckman, J.; McMurry, P.H.; Deng, Z.; Zhao, C.S.; Moerman, M.; Henzing, B.; de Leeuw, G.; Löschau, G.; Bastian, S.Mobility particle size spectrometers often referred to as DMPS (Differential Mobility Particle Sizers) or SMPS (Scanning Mobility Particle Sizers) have found a wide range of applications in atmospheric aerosol research. However, comparability of measurements conducted world-wide is hampered by lack of generally accepted technical standards and guidelines with respect to the instrumental set-up, measurement mode, data evaluation as well as quality control. Technical standards were developed for a minimum requirement of mobility size spectrometry to perform long-term atmospheric aerosol measurements. Technical recommendations include continuous monitoring of flow rates, temperature, pressure, and relative humidity for the sheath and sample air in the differential mobility analyzer. We compared commercial and custom-made inversion routines to calculate the particle number size distributions from the measured electrical mobility distribution. All inversion routines are comparable within few per cent uncertainty for a given set of raw data. Furthermore, this work summarizes the results from several instrument intercomparison workshops conducted within the European infrastructure project EUSAAR (European Supersites for Atmospheric Aerosol Research) and ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) to determine present uncertainties especially of custom-built mobility particle size spectrometers. Under controlled laboratory conditions, the particle number size distributions from 20 to 200 nm determined by mobility particle size spectrometers of different design are within an uncertainty range of around ±10% after correcting internal particle losses, while below and above this size range the discrepancies increased. For particles larger than 200 nm, the uncertainty range increased to 30%, which could not be explained. The network reference mobility spectrometers with identical design agreed within ±4% in the peak particle number concentration when all settings were done carefully. The consistency of these reference instruments to the total particle number concentration was demonstrated to be less than 5%. Additionally, a new data structure for particle number size distributions was introduced to store and disseminate the data at EMEP (European Monitoring and Evaluation Program). This structure contains three levels: raw data, processed data, and final particle size distributions. Importantly, we recommend reporting raw measurements including all relevant instrument parameters as well as a complete documentation on all data transformation and correction steps. These technical and data structure standards aim to enhance the quality of long-term size distribution measurements, their comparability between different networks and sites, and their transparency and traceability back to raw data.
- ItemSouth African EUCAARI measurements: Seasonal variation of trace gases and aerosol optical properties(München : European Geopyhsical Union, 2012) Laakso, L.; Vakkari, V.; Virkkula, A.; Laakso, H.; Backman, J.; Kulmala, M.; Beukes, J.P.; van Zyl, P.G.; Tiitta, P.; Josipovic, M.; Pienaar, J.J.; Chiloane, K.; Gilardoni, S.; Vignati, E.; Wiedensohler, A.; Tuch, T.; Birmili, W.; Piketh, S.; Collett, K.; Fourie, G.D.; Komppula, M.; Lihavainen, H.; de Leeuw, G.; Kerminen, V.-M.In this paper we introduce new in situ observations of atmospheric aerosols, especially chemical composition, physical and optical properties, on the eastern brink of the heavily polluted Highveld area in South Africa. During the observation period between 11 February 2009 and 31 January 2011, the mean particle number concentration (size range 10–840 nm) was 6310 cm3 and the estimated volume of sub-10 μm particles 9.3 μm3 m−3. The aerosol absorption and scattering coefficients at 637 nm were 8.3 Mm−1 and 49.5 Mm−1, respectively. The mean single-scattering albedo at 637 nm was 0.84 and the Ångström exponent of scattering was 1.5 over the wavelength range 450–635 nm. The mean O3, SO2, NOx and H2S-concentrations were 37.1, 11.5, 15.1 and 3.2 ppb, respectively. The observed range of concentrations was large and attributed to the seasonal variation of sources and regional meteorological effects, especially the anticyclonic re-circulation and strong winter-time inversions. In a global context, the levels of gases and particulates were typical for continental sites with strong anthropogenic influence, but clearly lower than the most polluted areas of south-eastern Asia. Of all pollutants observed at the site, ozone is the most likely to have adverse environmental effects, as the concentrations were high also during the growing season. The measurements presented here will help to close existing gaps in the ground-based global atmosphere observation system, since very little long-term data of this nature is available for southern Africa.
- ItemVariability of black carbon mass concentrations, sub-micrometer particle number concentrations and size distributions: results of the German Ultrafine Aerosol Network ranging from city street to High Alpine locations(Amsterdam [u.a.] : Elsevier Science, 2018) Sun, J.; Birmili, W.; Hermann, M.; Tuch, T.; Weinhold, K.; Spindler, G.; Schladitz, A.; Bastian, S.; Löschau, G.; Cyrys, J.; Gu, J.; Flentje, H.; Briel, B.; Asbac, C.; Kaminski, H.; Ries, L.; Sohme, R.; Gerwig, H.; Wirtz, K.; Meinhardt, F.; Schwerin, A.; Bath, O.; Ma, N.; Wiedensohler, A.This work reports the first statistical analysis of multi-annual data on tropospheric aerosols from the German Ultrafine Aerosol Network (GUAN). Compared to other networks worldwide, GUAN with 17 measurement locations has the most sites equipped with particle number size distribution (PNSD) and equivalent black carbon (eBC) instruments and the most site categories in Germany ranging from city street/roadside to High Alpine. As we know, the variations of eBC and particle number concentration (PNC) are influenced by several factors such as source, transformation, transport and deposition. The dominant controlling factor for different pollutant parameters might be varied, leading to the different spatio-temporal variations among the measured parameters. Currently, a study of spatio-temporal variations of PNSD and eBC considering the influences of both site categories and spatial scale is still missing. Based on the multi-site dataset of GUAN, the goal of this study is to investigate how pollutant parameters may interfere with spatial characteristics and site categories. © 2019 The Authors
- ItemCorrelation between traffic density and particle size distribution in a street canyon and the dependence on wind direction(München : European Geopyhsical Union, 2006) Voigtländer, J.; Tuch, T.; Birmili, W.; Wiedensohler, A.Combustion of fossil fuel in gasoline and diesel powered vehicles is a major source of aerosol particles in a city. In a street canyon, the number concentration of particles smaller than 300 nm in diameter, which can be inhaled and cause serious health effects, is dominated by particles originating from this source. In this study we measured both, particle number size distribution and traffic density continuously in a characteristic street canyon in Germany for a time period of 6 months. The street canyon with multistory buildings and 4 traffic lanes is very typical for larger cities. Thus, the measurements also are representative for many other street canyons in Europe. In contrast to previous studies, we measured and analyzed the particle number size distribution with high size resolution using a Twin Differential Mobility Analyzer (TDMPS). The measured size range was from 3 to 800 nm, separated into 40 size channels. Correlation coefficients between particle number concentration for integrated size ranges and traffic counts of 0.5 were determined. Correlations were also calculated for each of the 40 size channels of the DMPS system, respectively. We found a maximum of the correlation coefficients for nucleation mode particles in the size range between 10 and 20 nm in diameter. Furthermore, correlations between traffic and particles in dependence of meteorological data were calculated. Relevant parameters were identified by a multiple regression method. In our experiment only wind parameters have influenced the particle number concentration significantly. High correlation coefficients (up to 0.8) could be observed in the lee side of the street canyon for particles in the range between 10 and 100 nm in diameter. These values are significantly higher than correlation coefficients for other wind directions and other particle sizes. A minimum was found in the luff side of the street. These findings are in good agreement with theory of fluid dynamics in street canyons.
- ItemDispersion of traffic-related exhaust particles near the Berlin urban motorway – estimation of fleet emission factors(München : European Geopyhsical Union, 2009) Birmili, W.; Alaviippola, B.; Hinneburg, D.; Knoth, O.; Tuch, T.; Borken-Kleefeld, J.; Schacht, A.Atmospheric particle number size distributions of airborne particles (diameter range 10–500 nm) were collected over ten weeks at three sites in the vicinity of the A100 urban motorway in Berlin, Germany. The A100 carries about 180 000 vehicles on a weekday. The roadside particle distributions showed a number maximum between 20 and 60 nm clearly related to the motorway emissions. The average total number concentration at roadside was 28 000 cm−3 with a total range of 1200–168 000 cm−3. At distances of 80 and 400 m from the motorway the concentrations decreased to mean levels of 11 000 and 9000 cm−3, respectively. An obstacle-resolving dispersion model was applied to simulate the 3-D flow field and traffic tracer transport in the urban environment around the motorway. By inverse modelling, vehicle emission factors were derived that are representative of a fleet with a relative share of 6% lorry-like vehicles, and driving at a speed of 80 km h−1. Three different calculation approaches were compared, which differ in the choice of the experimental winds driving the flow simulation. The average emission factor per vehicle was 2.1 (±0.2) · 1014 km−1 for particle number and 0.077 (±0.01) · 1014 cm3 km−1 for particle volume. Regression analysis suggested that lorry-like vehicles emit 123 (±28) times more particle number than passenger car-like vehicles, and lorry-like vehicles account for about 91% of particulate number emissions on weekdays. Our work highlights the increasing applicability of 3-D flow models in urban microscale environments and their usefulness for determining traffic emission factors.
- ItemSize distributions of non-volatile particle residuals (Dp<800 nm) at a rural site in Germany and relation to air mass origin(München : European Geopyhsical Union, 2007) Engler, C.; Rose, D.; Wehner, B.; Wiedensohler, A.; Brüggemann, E.; Gnauk, T.; Spindler, G.; Tuch, T.; Birmili, W.Atmospheric aerosol particle size distributions at a continental background site in Eastern Germany were examined for a one-year period. Particles were classified using a twin differential mobility particle sizer in a size range between 3 and 800 nm. As a novelty, every second measurement of this experiment involved the removal of volatile chemical compounds in a thermodenuder at 300°C. This concept allowed to quantify the number size distribution of non-volatile particle cores – primarily associated with elemental carbon, and to compare this to the original non-conditioned size distribution. As a byproduct of the volatility analysis, new particles originating from nucleation inside the thermodenuder can be observed, however, overwhelmingly at diameters below 6 nm. Within the measurement uncertainty, every particle down to particle sizes of 15 nm is concluded to contain a non-volatile core. The volume fraction of non-volatile particulate matter (non-conditioned diameter < 800 nm) varied between 10 and 30% and was largely consistent with the experimentally determined mass fraction of elemental carbon. The average size of the non-volatile particle cores was estimated as a function of original non-conditioned size using a summation method, which showed that larger particles (>200 nm) contained more non-volatile compounds than smaller particles (<50 nm), thus indicating a significantly different chemical composition. Two alternative air mass classification schemes based on either, synoptic chart analysis (Berliner Wetterkarte) or back trajectories showed that the volume and number fraction of non-volatile cores depended less on air mass than the total particle number concentration. In all air masses, the non-volatile size distributions showed a more and a less volatile ("soot") mode, the latter being located at about 50 nm. During unstable conditions and in maritime air masses, smaller values were observed compared to stable or continental conditions. This reflects the significant emission of non-volatile material over the continent and, depending on atmospheric stratification, increased concentrations at ground level.