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    A concept of an automated function control for ambient aerosol measurements using mobility particle size spectrometers
    (München : European Geopyhsical Union, 2014) Schladitz, A.; Merkel, M.; Bastian, S.; Birmili, W.; Weinhold, K.; Löschau, G.; Wiedensohler, A.
    An automated function control unit was developed to regularly check the ambient particle number concentration derived from a mobility particle size spectrometer as well as its zero-point behaviour. The function control allows unattended quality assurance experiments at remote air quality monitoring or research stations under field conditions. The automated function control also has the advantage of being able to get a faster system stability response than the recommended on-site comparisons with reference instruments. The method is based on a comparison of the total particle number concentration measured by a mobility particle size spectrometer and a condensation particle counter while removing diffusive particles smaller than 20 nm in diameter. In practice, the small particles are removed by a set of diffusion screens, as traditionally used in a diffusion battery. Another feature of the automated function control is to check the zero-point behaviour of the ambient aerosol passing through a high-efficiency particulate air (HEPA) filter. The performance of the function control is illustrated with the aid of a 1-year data set recorded at Annaberg-Buchholz, a station in the Saxon air quality monitoring network. During the period of concern, the total particle number concentration derived from the mobility particle size spectrometer slightly overestimated the particle number concentration recorded by the condensation particle counter by 2 % (grand average). Based on our first year of experience with the function control, we developed tolerance criteria that allow a performance evaluation of a tested mobility particle size spectrometer with respect to the total particle number concentration. We conclude that the automated function control enhances the quality and reliability of unattended long-term particle number size distribution measurements. This will have beneficial effects for intercomparison studies involving different measurement sites, and help provide a higher data accuracy for cohort health and climate research studies.
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    Variations in tropospheric submicron particle size distributions across the European continent 2008-2009
    (München : European Geopyhsical Union, 2014) Beddows, D.C.S.; Dall'Osto, M.; Harrison, R.M.; Kulmala, M.; Asmi, A.; Wiedensohler, A.; Laj, P.; Fjaeraa, A.M.; Sellegri, K.; Birmili, W.; Bukowiecki, N.; Weingartner, E.; Baltensperger, U.; Zdimal, V.; Zikova, N.; Putaud, J.-P.; Marinoni, A.; Tunved, P.; Hansson, H.-C.; Fiebig, M.; Kivekäs, N.; Swietlicki, E.; Lihavainen, H.; Asmi, E.; Ulevicius, V.; Aalto, P.P.; Mihalopoulos, N.; Kalivitis, N.; Kalapov, I.; Kiss, G.; de Leeuw, G.; Henzing, B.; O'Dowd, C.; Jennings, S.G.; Flentje, H.; Meinhardt, F.; Ries, L.; Denier van der Gon, H.A.C.; Visschedijk, A.J.H.
    Cluster~analysis of particle number size distributions from~background sites across Europe~is presented. This generated a total of nine clusters of particle size distributions which could be further combined into two main groups, namely: a south-to-north category (four clusters) and a west-to-east category (five clusters). The first group was identified as most frequently being detected inside and around northern Germany and neighbouring countries, showing clear evidence of local afternoon nucleation and growth events that could be linked to movement of air masses from south to north arriving ultimately at the Arctic contributing to Arctic haze.~The second group of particle size spectra proved to have narrower size distributions and collectively showed a dependence of modal diameter upon the longitude of the site (west to east) at which they were most frequently detected.~These clusters indicated regional nucleation (at the coastal sites) growing to larger modes further inland. The apparent growth rate of the modal diameter was around 0.6–0.9 nm h−1. Four specific air mass back-trajectories were successively taken as case studies to examine in real time the evolution of aerosol size distributions across Europe. ~While aerosol growth processes can be observed as aerosol traverses Europe, the processes are often obscured by the addition of aerosol by emissions en route. This study revealed that some of the 24 stations exhibit more complex behaviour than others, especially when impacted by local sources or a variety of different air masses. Overall, the aerosol size distribution clustering analysis greatly simplifies the complex data set and allows a description of aerosol aging processes, which reflects the longer-term average development of particle number size distributions as air masses advect across Europe.
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    Chemistry of new particle growth in mixed urban and biogenic emissions - Insights from CARES
    (München : European Geopyhsical Union, 2014) Setyan, A.; Song, C.; Merkel, M.; Knighton, W.B.; Onasch, T.B.; Canagaratna, M.R.; Worsnop, D.R.; Wiedensohler, A.; Shilling, J.E.; Zhang, Q.
    Regional new particle formation and growth events (NPEs) were observed on most days over the Sacramento and western Sierra foothills area of California in June 2010 during the Carbonaceous Aerosols and Radiative Effect Study (CARES). Simultaneous particle measurements at both the T0 (Sacramento, urban site) and the T1 (Cool, rural site located ~40 km northeast of Sacramento) sites of CARES indicate that the NPEs usually occurred in the morning with the appearance of an ultrafine mode at ~15 nm (in mobility diameter, Dm, measured by a mobility particle size spectrometer operating in the range 10-858 nm) followed by the growth of this modal diameter to ~50 nm in the afternoon. These events were generally associated with southwesterly winds bringing urban plumes from Sacramento to the T1 site. The growth rate was on average higher at T0 (7.1 ± 2.7 nm h−1) than at T1 (6.2 ± 2.5 nm h−1), likely due to stronger anthropogenic influences at T0. Using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), we investigated the evolution of the size-resolved chemical composition of new particles at T1. Our results indicate that the growth of new particles was driven primarily by the condensation of oxygenated organic species and, to a lesser extent, ammonium sulfate. New particles appear to be fully neutralized during growth, consistent with high NH3 concentration in the region. Nitrogen-containing organic ions (i.e., CHN+, CH4N+, C2H3N+, and C2H4N+) that are indicative of the presence of alkyl-amine species in submicrometer particles enhanced significantly during the NPE days, suggesting that amines might have played a role in these events. Our results also indicate that the bulk composition of the ultrafine mode organics during NPEs was very similar to that of anthropogenically influenced secondary organic aerosol (SOA) observed in transported urban plumes. In addition, the concentrations of species representative of urban emissions (e.g., black carbon, CO, NOx, and toluene) were significantly higher whereas the photo-oxidation products of biogenic VOCs (volatile organic compounds) and the biogenically influenced SOA also increased moderately during the NPE days compared to the non-event days. These results indicate that the frequently occurring NPEs over the Sacramento and Sierra Nevada regions were mainly driven by urban plumes from Sacramento and the San Francisco Bay Area, and that the interaction of regional biogenic emissions with the urban plumes has enhanced the new particle growth. This finding has important implications for quantifying the climate impacts of NPEs on global scale.
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    General overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) – integrating aerosol research from nano to global scales
    (München : European Geopyhsical Union, 2011) Kulmala, M.; Asmi, A.; Lappalainen, H.K.; Carslaw, K.S.; Pöschl, U.; Baltensperger, U.; Hov, Ø.; Brenquier, J.-L.; Pandis, S.N.; Facchini, M.C.; Hansson, H.-C.; Wiedensohler, A.; O'Dowd, C.D.; Boers, R.; Boucher, O.; de Leeuw, G.; Denier van der Gon, H.A.C.; Feichter, J.; Krejci, R.; Laj, P.; Lihavainen, H.; Lohmann, U.; McFiggans, G.; Mentel, T.; Pilinis, C.; Riipinen, I.; Schulz, M.; Stohl, A.; Swietlicki, E.; Vignati, E.; Alves, C.; Amann, M.; Ammann, M.; Arabas, S.; Artaxo, P.; Baars, H.; Beddows, D.C.S.; Bergström, R.; Beukes, J.P.; Bilde, M.; Burkhart, J.F.; Canonaco, F.; Clegg, S.L.; Coe, H.; Crumeyrolle, S.; D'Anna, B.; Decesari, S.; Gilardoni, S.; Fischer, M.; Fjaeraa, A.M.; Fountoukis, C.; George, C.; Gomes, L.; Halloran, P.; Hamburger, T.; Harrison, R.M.; Herrmann, H.; Hoffmann, T.; Hoose, C.; Hu, M.; Hyvärinen, A.; Hõrrak, U.; Iinuma, Y.; Iversen, T.; Josipovic, M.; Kanakidou, M.; Kiendler-Scharr, A.; Kirkevåg, A.; Kiss, G.; Klimont, Z.; Kolmonen, P.; Komppula, M.; Kristjánsson, J.-E.; Laakso, L.; Laaksonen, A.; Labonnote, L.; Lanz, V.A.; Lehtinen, K.E.J.; Rizzo, L.V.; Makkonen, R.; Manninen, H.E.; McMeeking, G.; Merikanto, J.; Minikin, A.; Mirme, S.; Morgan, W.T.; Nemitz, E.; O'Donnell, D.; Panwar, T.S.; Pawlowska, H.; Petzold, A.; Pienaar, J.J.; Pio, C.; Plass-Duelmer, C.; Prévôt, A.S.H.; Pryor, S.; Reddington, C.L.; Roberts, G.; Rosenfeld, D.; Schwarz, J.; Seland, Ø.; Sellegri, K.; Shen, X.J.; Shiraiwa, M.; Siebert, H.; Sierau, B.; Simpson, D.; Sun, J.Y.; Topping, D.; Tunved, P.; Vaattovaara, P.; Vakkari, V.; Veefkind, J.P.; Visschedijk, A.; Vuollekoski, H.; Vuolo, R.; Wehner, B.; Wildt, J.; Woodward, S.; Worsnop, D.R.; van Zadelhoff, G.-J.; Zardini, A.A.; Zhang, K.; van Zyl, P.G.; Kerminen, V.-M.
    In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies.
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    Number size distributions and seasonality of submicron particles in Europe 2008–2009
    (München : European Geopyhsical Union, 2011) Asmi, A.; Wiedensohler, A.; Laj, P.; Fjaeraa, A.-M.; Sellegri, K.; Birmili, W.; Weingartner, E.; Baltensperger, U.; Zdimal, V.; Zikova, N.; Putaud, J.-P.; Marinoni, A.; Tunved, P.; Hansson, H.-C.; Fiebig, M.; Kivekäs, N.; Lihavainen, H.; Asmi, E.; Ulevicius, V.; Aalto, P.P.; Swietlicki, E.; Kristensson, A.; Mihalopoulos, N.; Kalivitis, N.; Kalapov, I.; Kiss, G.; de Leeuw, G.; Henzing, B.; Harrison, R.M.; Beddows, D.; O'Dowd, C.; Jennings, S.G.; Flentje, H.; Weinhold, K.; Meinhardt, F.; Ries, L.; Kulmala, M.
    Two years of harmonized aerosol number size distribution data from 24 European field monitoring sites have been analysed. The results give a comprehensive overview of the European near surface aerosol particle number concentrations and number size distributions between 30 and 500 nm of dry particle diameter. Spatial and temporal distribution of aerosols in the particle sizes most important for climate applications are presented. We also analyse the annual, weekly and diurnal cycles of the aerosol number concentrations, provide log-normal fitting parameters for median number size distributions, and give guidance notes for data users. Emphasis is placed on the usability of results within the aerosol modelling community. We also show that the aerosol number concentrations of Aitken and accumulation mode particles (with 100 nm dry diameter as a cut-off between modes) are related, although there is significant variation in the ratios of the modal number concentrations. Different aerosol and station types are distinguished from this data and this methodology has potential for further categorization of stations aerosol number size distribution types. The European submicron aerosol was divided into characteristic types: Central European aerosol, characterized by single mode median size distributions, unimodal number concentration histograms and low variability in CCN-sized aerosol number concentrations; Nordic aerosol with low number concentrations, although showing pronounced seasonal variation of especially Aitken mode particles; Mountain sites (altitude over 1000 m a.s.l.) with a strong seasonal cycle in aerosol number concentrations, high variability, and very low median number concentrations. Southern and Western European regions had fewer stations, which decreases the regional coverage of these results. Aerosol number concentrations over the Britain and Ireland had very high variance and there are indications of mixed air masses from several source regions; the Mediterranean aerosol exhibit high seasonality, and a strong accumulation mode in the summer. The greatest concentrations were observed at the Ispra station in Northern Italy with high accumulation mode number concentrations in the winter. The aerosol number concentrations at the Arctic station Zeppelin in Ny-\AA lesund in Svalbard have also a strong seasonal cycle, with greater concentrations of accumulation mode particles in winter, and dominating summer Aitken mode indicating more recently formed particles. Observed particles did not show any statistically significant regional work-week or weekday related variation in number concentrations studied. Analysis products are made for open-access to the research community, available in a freely accessible internet site. The results give to the modelling community a reliable, easy-to-use and freely available comparison dataset of aerosol size distributions.
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    Water uptake by biomass burning aerosol at sub- and supersaturated conditions: closure studies and implications for the role of organics
    (München : European Geopyhsical Union, 2011) Dusek, U.; Frank, G.P.; Massling, A.; Zeromskiene, K.; Iinuma, Y.; Schmid, O.; Helas, G.; Hennig, T.; Wiedensohler, A.; Andreae, M.O.
    We investigate the CCN activity of freshly emitted biomass burning particles and their hygroscopic growth at a relative humidity (RH) of 85%. The particles were produced in the Mainz combustion laboratory by controlled burning of various wood types. The water uptake at sub- and supersaturations is parameterized by the hygroscopicity parameter, κ (c.f. Petters and Kreidenweis, 2007). For the wood burns, κ is low, generally around 0.06. The main emphasis of this study is a comparison of κ derived from measurements at sub- and supersaturated conditions (κG and κCCN), in order to see whether the water uptake at 85% RH can predict the CCN properties of the biomass burning particles. Differences in κGand κCCN can arise through solution non-idealities, the presence of slightly soluble or surface active compounds, or non-spherical particle shape. We find that κG and κCCN agree within experimental uncertainties (of around 30%) for particle sizes of 100 and 150 nm; only for 50 nm particles is κCCN larger than κG by a factor of 2. The magnitude of this difference and its dependence on particle size is consistent with the presence of surface active organic compounds. These compounds mainly facilitate the CCN activation of small particles, which form the most concentrated solution droplets at the point of activation. The 50 nm particles, however, are only activated at supersaturations higher than 1% and are therefore of minor importance as CCN in ambient clouds. By comparison with the actual chemical composition of the biomass burning particles, we estimate that the hygroscopicity of the water-soluble organic carbon (WSOC) fraction can be represented by a κWSOC value of approximately 0.2. The effective hygroscopicity of a typical wood burning particle can therefore be represented by a linear mixture of an inorganic component with κ ≅ 0.6, a WSOC component with κ ≅ 0.2, and an insoluble component with κ = 0.
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    The chemistry of OH and HO2 radicals in the boundary layer over the tropical Atlantic Ocean
    (München : European Geopyhsical Union, 2010) Whalley, L.K.; Furneaux, K.L.; Goddard, A.; Lee, J.D.; Mahajan, A.; Oetjen, H.; Read, K.A.; Kaaden, N.; Carpenter, L.J.; Lewis, A.C.; Plane, J.M.C.; Saltzman, E.S.; Wiedensohler, A.; Heard, D.E.
    Fluorescence Assay by Gas Expansion (FAGE) has been used to detect ambient levels of OH and HO2 radicals at the Cape Verde Atmospheric Observatory, located in the tropical Atlantic marine boundary layer, during May and June 2007. Midday radical concentrations were high, with maximum concentrations of 9 ×106 molecule cm−3 and 6×108 molecule cm−3 observed for OH and HO2, respectively. A box model incorporating the detailed Master Chemical Mechanism, extended to include halogen chemistry, heterogeneous loss processes and constrained by all available measurements including halogen and nitrogen oxides, has been used to assess the chemical and physical parameters controlling the radical chemistry. The model was able to reproduce the daytime radical concentrations to within the 1 σ measurement uncertainty of 20% during the latter half of the measurement period but significantly under-predicted [HO2] by 39% during the first half of the project. Sensitivity analyses demonstrate that elevated [HCHO] (~2 ppbv) on specific days during the early part of the project, which were much greater than the mean [HCHO] (328 pptv) used to constrain the model, could account for a large portion of the discrepancy between modelled and measured [HO2] at this time. IO and BrO, although present only at a few pptv, constituted ~19% of the instantaneous sinks for HO2, whilst aerosol uptake and surface deposition to the ocean accounted for a further 23% of the HO2 loss at noon. Photolysis of HOI and HOBr accounted for ~13% of the instantaneous OH formation. Taking into account that halogen oxides increase the oxidation of NOx (NO → NO2), and in turn reduce the rate of formation of OH from the reaction of HO2 with NO, OH concentrations were estimated to be 9% higher overall due to the presence of halogens. The increase in modelled OH from halogen chemistry gives an estimated 9% shorter lifetime for methane in this region, and the inclusion of halogen chemistry is necessary to model the observed daily cycle of O3 destruction that is observed at the surface. Due to surface losses, we hypothesise that HO2 concentrations increase with height and therefore contribute a larger fraction of the O3 destruction than at the surface.
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    A synthesis of cloud condensation nuclei counter (CCNC) measurements within the EUCAARI network
    (München : European Geopyhsical Union, 2015) Paramonov, M.; Kerminen, V.-M.; Gysel, M.; Aalto, P.P.; Andreae, M.O.; Asmi, E.; Baltensperger, U.; Bougiatioti, A.; Brus, D.; Frank, G.P.; Good, N.; Gunthe, S.S.; Hao, L.; Irwin, M.; Jaatinen, A.; Jurányi, Z.; King, S.M.; Kortelainen, A.; Kristensson, A.; Lihavainen, H.; Kulmala, M.; Lohmann, U.; Martin, S.T.; McFiggans, G.; Mihalopoulos, N.; Nenes, A.; O'Dowd, C.D.; Ovadnevaite, J.; Petäjä, T.; Pöschl, U.; Roberts, G.C.; Rose, D.; Svenningsson, B.; Swietlicki, E.; Weingartner, E.; Whitehead, J.; Wiedensohler, A.; Wittbom, C.; Sierau, B.
    Cloud condensation nuclei counter (CCNC) measurements performed at 14 locations around the world within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) framework have been analysed and discussed with respect to the cloud condensation nuclei (CCN) activation and hygroscopic properties of the atmospheric aerosol. The annual mean ratio of activated cloud condensation nuclei (NCCN) to the total number concentration of particles (NCN), known as the activated fraction A, shows a similar functional dependence on supersaturation S at many locations – exceptions to this being certain marine locations, a free troposphere site and background sites in south-west Germany and northern Finland. The use of total number concentration of particles above 50 and 100 nm diameter when calculating the activated fractions (A50 and A100, respectively) renders a much more stable dependence of A on S; A50 and A100 also reveal the effect of the size distribution on CCN activation. With respect to chemical composition, it was found that the hygroscopicity of aerosol particles as a function of size differs among locations. The hygroscopicity parameter κ decreased with an increasing size at a continental site in south-west Germany and fluctuated without any particular size dependence across the observed size range in the remote tropical North Atlantic and rural central Hungary. At all other locations κ increased with size. In fact, in Hyytiälä, Vavihill, Jungfraujoch and Pallas the difference in hygroscopicity between Aitken and accumulation mode aerosol was statistically significant at the 5 % significance level. In a boreal environment the assumption of a size-independent κ can lead to a potentially substantial overestimation of NCCN at S levels above 0.6 %. The same is true for other locations where κ was found to increase with size. While detailed information about aerosol hygroscopicity can significantly improve the prediction of NCCN, total aerosol number concentration and aerosol size distribution remain more important parameters. The seasonal and diurnal patterns of CCN activation and hygroscopic properties vary among three long-term locations, highlighting the spatial and temporal variability of potential aerosol–cloud interactions in various environments.
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    First 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.
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    Analysis of number size distributions of tropical free tropospheric aerosol particles observed at Pico Espejo (4765 m a.s.l.), Venezuela
    (München : European Geopyhsical Union, 2011) Schmeissner, T.; Krejci, R.; Ström, J.; Birmili, W.; Wiedensohler, A.; Hochschild, G.; Gross, J.; Hoffmann, P.; Calderon, S.
    The first long-term measurements of aerosol number and size distributions in South-American tropical free troposphere (FT) were performed from March 2007 until March 2009. The measurements took place at the high altitude Atmospheric Research Station Alexander von Humboldt. The station is located on top of the Sierra Nevada mountain ridge at 4765 m a.s.l. nearby the city of Mérida, Venezuela. Aerosol size distribution and number concentration data was obtained with a custom-built Differential Mobility Particle Sizer (DMPS) system and a Condensational Particle Counter (CPC). The analysis of the annual and diurnal variability of the tropical FT aerosol focused mainly on possible links to the atmospheric general circulation in the tropics. Considerable annual and diurnal cycles of the particle number concentration were observed. Highest total particle number concentrations were measured during the dry season (January–March, 519 ± 613 cm−3), lowest during the wet season (July–September, 318 ± 194 cm−3). The more humid FT (relative humidity (RH) range 50–95 %) contained generally higher aerosol particle number concentrations (573 ± 768 cm−3 during dry season, 320 ± 195 cm−3 during wet season) than the dry FT (RH < 50 %, 454 ± 332 cm−3 during dry season, 275 ± 172 cm−3 during wet season), indicating the importance of convection for aerosol distributions in the tropical FT. The diurnal cycle in the variability of the particle number concentration was mainly driven by local orography.