lnstitut für Sensorik und Elektronik

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    Publikation
    Hygroscopic properties of submicrometer atmospheric aerosol particles measured with H-TDMA instruments in various environments - a review
    (Stockholm University Press, 01.01.2008) Swietlicki, Erik; Hansson, Hans-Christen; Hämeri, Kaarle; Svenningsson, Birgitta; Massling, Andreas; McFiggans, Gordon; McMurry, Peter H.; Petäjä, Tuukka; Tunved, Peter; Gysel, Martin; Topping, David; Weingartner, Ernest; Baltensperger, Urs; Rissler, Jenny; Wiedensohler, Alfred; Kulmala, Markku
    The hygroscopic properties play a vital role for the direct and indirect effects of aerosols on climate, as well as the health effects of particulate matter (PM) by modifying the deposition pattern of inhaled particles in the humid human respiratory tract. Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA) instruments have been used in field campaigns in various environments globally over the last 25 yr to determine the water uptake on submicrometre particles at subsaturated conditions. These investigations have yielded valuable and comprehensive information regarding the particle hygroscopic properties of the atmospheric aerosol, including state of mixing. These properties determine the equilibrium particle size at ambient relative humidities and have successfully been used to calculate the activation of particles at water vapour supersaturation. This paper summarizes the existing published H-TDMA results on the sizeresolved submicrometre aerosol particle hygroscopic properties obtained from ground-based measurements at multiple marine, rural, urban and free tropospheric measurement sites. The data is classified into groups of hygroscopic growth indicating the external mixture, and providing clues to the sources and processes controlling the aerosol. An evaluation is given on how different chemical and physical properties affect the hygroscopic growth.
    01A - Beitrag in wissenschaftlicher Zeitschrift
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    Publikation
    Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation
    (Copernicus, 26.05.2010) Spracklen, Dominick V.; Carslaw, Kenneth S.; Merikanto, Joonas; Mann, Graham W.; Reddington, Carly L.; Pickering, S.; Ogren, John A.; Andrews, Elisabeth; Baltensperger, Urs; Weingartner, Ernest; Boy, Michael; Kulmala, Markku; Laakso, Lauri; Lihavainen, Heikki; Kivekäs, Niku; Komppula, Mika; Mihalopoulos, Ninolaos; Kouvarakis, Giorgos; Jennings, Stephen G.; O'Dowd, Collin D.; Birmili, Wolfram; Wiedensohler, Alfred; Weller, Rolf; Gras, John; Laj, Paolo; Sellegri, Karine; Bonn, Boris; Krejci, Radovan; Laaksonen, Ari; Hamed, Amar; Minikin, Andreas; Harrison, Roy Michael; Talbot, Robert; Sun, Junying
    We synthesised observations of total particle number (CN) concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300–2000 cm−3 in the marine boundary layer and free troposphere (FT) and 1000–10 000 cm−3 in the continental boundary layer (BL). Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2–10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R2=0.46) but fail to explain the observed seasonal cycle (R2=0.1). The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=−88%) unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=−25%). Simulated CN concentrations in the continental BL were also biased low (NMB=−74%) unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J, proportional to gas-phase sulfuric acid concentration to the power one) or kinetic-type mechanism (J proportional to sulfuric acid to the power two) with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). The nucleation constants that resulted in best overall match between model and observed CN concentrations were consistent with values derived in previous studies from detailed case studies at individual sites. In our model, kinetic and activation-type nucleation parameterizations gave similar agreement with observed monthly mean CN concentrations.
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Vorschaubild
    Publikation
    EUCAARI ion spectrometer measurements at 12 European sites – analysis of new particle formation events
    (Copernicus, 25.08.2010) Manninen, Hanna E.; Nieminen, Tuomo; Asmi, Eija; Gagné, Stéphanie; Häkkinen, Silja; Lehtipalo, Katrianne; Aalto, Pasi Pekka; Vana, Marko; Mirme, Aadu; Mirme, Sander; Hõrrak, Urmas; Plass-Dülmer, Christian; Stange, Gert; Kiss, Gyula; Hoffer, András; Törő, N.; Moerman, Marcel; Henzing, Bas; de Leeuw, Gerrit; Brinkenberg, Marcel; Kouvarakis, Giorgos N.; Bougiatioti, Aikaterini; Mihalopoulos, Nikolaos; O'Dowd, Colin D.; Ceburnis, Darius; Arneth, Almut; Svenningsson, Brigitta; Swietlicki, Erik; Tarozzi, Leone; Decesari, Stefano; Facchini, Maria Cristina; Birmili, Wolfram; Sonntag, André; Wiedensohler, Alfred; Boulon, Julien; Sellegri, Karine; Laj, Paolo; Gysel, Martin; Bukowiecki, Nicolas; Weingartner, Ernest; Wehrle, Günther; Laaksonen, Ari; Hamed, Amar; Joutsensaari, Jorma; Petäjä, Tuukka; Kerminen, Veli-Matti; Kulmala, Markku
    We present comprehensive results on continuous atmospheric cluster and particle measurements in the size range ~1–42 nm within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) project. We focused on characterizing the spatial and temporal variation of new particle formation events and relevant particle formation parameters across Europe. Different types of air ion and cluster mobility spectrometers were deployed at 12 field sites across Europe from March 2008 to May 2009. The measurements were conducted in a wide variety of environments, including coastal and continental locations as well as sites at different altitudes (both in the boundary layer and the free troposphere). New particle formation events were detected at all of the 12 field sites during the year-long measurement period. From the data, nucleation and growth rates of newly formed particles were determined for each environment. In a case of parallel ion and neutral cluster measurements, we could also estimate the relative contribution of ion-induced and neutral nucleation to the total particle formation. The formation rates of charged particles at 2 nm accounted for 1–30% of the corresponding total particle formation rates. As a significant new result, we found out that the total particle formation rate varied much more between the different sites than the formation rate of charged particles. This work presents, so far, the most comprehensive effort to experimentally characterize nucleation and growth of atmospheric molecular clusters and nanoparticles at ground-based observation sites on a continental scale.
    01A - Beitrag in wissenschaftlicher Zeitschrift
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    Publikation
    Characterization and intercomparison of aerosol absorption photometers. result of two intercomparison workshops
    (Copernicus, 2011) Müller, Thomas; Henzing, Bas; de Leeuw, Gerrit; Wiedensohler, Alfred; Alastuey, Andrés; Angelov, H.; Bizjak, Milan; Collaud Coen, Martine; Engström, J. E.; Gruening, Carsten; Hillamo, Risto; Hoffer, András; Imre, Kornélia; Ivanow, Petko; Jennings, Stephen G.; Sun, Junying; Kalivitis, Nikos; Karlsson, Hanna; Komppula, Mikka; Laj, Paolo; Li, S.-M.; Lunder, Chris; Marinoni, Angela; Martins dos Santos, Sebastiao; Moerman, Marcel; Nowak, Andreas; Ogren, John A.; Petzold, Andreas; Pichon, Jean Marc; Rodriquez, Sergio; Sharma, Sangeeta; Sheridan, Patrick J.; Teinilä, Kimmo; Tuch, Thomas; Viana, Mar; Virkkula, Aki; Weingartner, Ernest; Wilhelm, R.; Wang, Yaqiang
    Absorption photometers for real time application have been available since the 1980s, but the use of filter-based instruments to derive information on aerosol properties (absorption coefficient and black carbon, BC) is still a matter of debate. Several workshops have been conducted to investigate the performance of individual instruments over the intervening years. Two workshops with large sets of aerosol absorption photometers were conducted in 2005 and 2007. The data from these instruments were corrected using existing methods before further analysis. The inter-comparison shows a large variation between the responses to absorbing aerosol particles for different types of instruments. The unit to unit variability between instruments can be up to 30% for Particle Soot Absorption Photometers (PSAPs) and Aethalometers. Multi Angle Absorption Photometers (MAAPs) showed a variability of less than 5%. Reasons for the high variability were identified to be variations in sample flow and spot size. It was observed that different flow rates influence system performance with respect to response to absorption and instrumental noise. Measurements with non absorbing particles showed that the current corrections of a cross sensitivity to particle scattering are not sufficient. Remaining cross sensitivities were found to be a function of the total particle load on the filter. The large variation between the response to absorbing aerosol particles for different types of instruments indicates that current correction functions for absorption photometers are not adequate.
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Vorschaubild
    Publikation
    Number size distributions and seasonality of submicron particles in Europe 2008–2009
    (Copernicus, 15.06.2011) Asmi, Ari; Wiedensohler, Alfred; Laj, Paolo; Fjaeraa, Ann Mari; Sellegri, Karine; Birmili, Wolfram; Weingartner, Ernest; Baltensperger, Urs; Zdimal, Vladimir; Zikova, Nadezda; Putaud, Jean-Philippe; Marinoni, Angela; Tunved, Peter; Hansson, Hans-Christen; Fiebig, Markus; Kivekäs, Niku; Lihavainen, Heikki; Asmi, Eija; Ulevicius, Vidmantas; Aalto, Pasi Pekka; Swietlicki, Erik; Kristensson, Adam; Mihalopoulos, Nikolaos; Kalivitis, Nikos; Kalapov, Ivo; Kiss, Gyula; de Leeuw, Gerrit; Henzing, Bas; Harrison, Roy; Beddows, David; O'Dowd, Colin; Jennings, Stephen G.; Flentje, Harald; Weinhold, Kay; Meinhardt, Frank; Ries, Ludwig; Kulmala, Markku
    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-Ålesund 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.
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Vorschaubild
    Publikation
    Primary versus secondary contributions to particle number concentrations in the European boundary layer
    (Copernicus, 05.12.2011) Reddington, Carly L.; Carslaw, Ken S.; Spracklen, Dominick V.; Frontoso, Maria Grazia; Collins, Lisa M.; Merikanto, Joonas; Minikin, Andreas; Hamburger, Thomas; Coe, Hugh; Kulmala, Markku; Aalto, Pasi Pekka; Flentje, Harald; Plass-Dülmer, Christian; Birmili, Wolfram; Wiedensohler, Alfred; Wehner, Birgit; Tuch, Thomas; Sonntag, Alfred; O'Dowd, Collin D.; Jennings, Stephen G.; Dupuy, Regis; Baltensperger, Urs; Weingartner, Ernest; Hansson, Hans-Christen; Tunved, Peter; Laj, Paolo; Sellegri, Karine; Boulon, Julien; Putaud, Jean-Philippe; Gruening, Carsten; Swietlicki, Erik; Roldin, Pontus; Henzing, J.S.; Moerman, Marcel; Mihalopoulos, Nikolaos; Kouvarakis, Giorgos; Ždímal, Vladimir; Zíková, Nadezda; Marinoni, Angela; Bonasoni, Paolo; Duchi, Rocco
    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.
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Vorschaubild
    Publikation
    Mobility particle size spectrometers. harmonization of technical standards and data structure to facilitate high quality long-term observations of atmospheric particle number size distributions
    (Copernicus, 29.03.2012) Wiedensohler, Alfred; Birmili, Wolfram; Nowak, Marta; Sonntag, André; Weinhold, Kay; Merkel, Maik; Wehner, Birgit; Tuch, Thomas; Pfeifer, Sascha; Fiebig, Markus; Fjäraa, Ann Mari; Asmi, Eija; Sellegri, Karine; Depuy, R.; Venzac, Hervé; Villani, Paolo; Laj, Paolo; Aalto, Pasi Pekka; Ogren, John A.; Swietlicki, Erik; Williams, Paul I.; Roldin, Pontus; Quincey, Paul; Hüglin, Christoph; Fierz-Schmidhauser, Rahel; Gysel, Martin; Weingartner, Ernest; Riccobono, Francesco; Santos, S.; Gruening, Carsten; Faloon, K.; Beddows, D.; Harrison, Roy; Monahan, C.; Jennings, Stephen G.; O'Dowd, Colin D.; Marinoni, Angela; Horn, H.-G.; Keck, L.; Jiang, Jingkun; Scheckman, Jakob; McMurry, Peter H.; Deng, Zhaoze; Zhao, Chunsheng; Moerman, Marcel; Henzing, Bas; de Leeuw, Gerrit; Löschau, G.; Bastian, S.
    Abstract. 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.
    01A - Beitrag in wissenschaftlicher Zeitschrift
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    Publikation
    Influence of water uptake on the aerosol particle light scattering coefficients of the Central European aerosol
    (Stockholm University Press, 2014) Zieger, Paul; Fierz-Schmidhauser, Rahel; Poulain, Laurent; Müller, Thomas; Birmili, Wolfram; Spindler, Gerald; Wiedensohler, Alfred; Baltensperger, Urs; Weingartner, Ernest
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Vorschaubild
    Publikation
    A European aerosol phenomenology-5. Climatology of black carbon optical properties at 9 regional background sites across Europe
    (Elsevier, 2016) Zanatta, Marco; Gysel, Martin; Bukowiecki, Nicolas; Müller, Thomas; Weingartner, Ernest; Areskoug, Hans; Fiebig, Markus; Yttri, Karl Espen; Mihalopoulos, Nikolaos; Kouvarakis, Giorgos; Beddows, David; Harrison, Roy; Cavalli, Fabrizia; Putaud, Jean; Spindler, Gerald; Wiedensohler, Alfred; Alastuey, Andrés; Pandolfi, Marco; Sellegri, Karine; Swietlicki, Erik; Jaffrezo, Jean-Luc; Baltensperger, Urs; Laj, Paolo
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Vorschaubild
    Publikation
    Variations in tropospheric submicron particle size distributions across the European continent 2008–2009
    (Copernicus, 2014) Beddows, David; Dall'Osto, Manuel; Harrison, Roy; Kulmala, Markku; Asmi, Ari; Wiedensohler, Alfred; Laj, Paolo; Fjaeraa, Ann Mari; Sellegri, Karine; Birmili, Wolfram; Bukowiecki, Nicolas; Weingartner, Ernest; Baltensperger, Urs; Zdimal, Vladimir; Zikova, Nadezda; Putaud, Jean-Philippe; Marinoni, Angela; Tunved, Peter; Hansson, Hans-Christen; Fiebig, Markus; Kivekäs, Niku; Swietlicki, Erik; Lihavainen, Heikki; Asmi, Eija; Ulevicius, Vidmantas; Aalto, Pasi Pekka; Mihalopoulos, Nikolaos; Kalivitis, Nikos; Kalapov, Ivo; Kiss, Gyula; de Leeuw, Gerrit; Henzing, Bas; O'Dowd, Colin; Jennings, Stephen G.; Flentje, Harald; Meinhardt, Frank; Ries, Ludwig; Denier van der Gon, Hugo; Visschedijk, Antoon
    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.
    01A - Beitrag in wissenschaftlicher Zeitschrift