Browsing by Author "Wiedensohler, Alfred"
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Publication A dual-wavelength photothermal aerosol absorption monitor. Design, calibration and performance(Copernicus, 2022) Drinovec, Luka; Jagodič, Uroš; Pirker, Luka; Škarabot, Miha; Kurtjak, Mario; Vidović, Kristijan; Ferrero, Luca; Visser, Bradley; Röhrbein, Jannis; Weingartner, Ernest; Kalbermatter, Daniel M.; Vasilatou, Konstantina; Bühlmann, Tobias; Pascale, Celine; Müller, Thomas; Wiedensohler, Alfred; Močnik, GrišaThere exists a lack of aerosol absorption measurement techniques with low uncertainties and without artefacts. We have developed the two-wavelength Photothermal Aerosol Absorption Monitor (PTAAM-2λ), which measures the aerosol absorption coefficient at 532 and 1064 nm. Here we describe its design, calibration and mode of operation and evaluate its applicability, limits and uncertainties. The 532 nm channel was calibrated with ∼ 1 µmol mol−1 NO2, whereas the 1064 nm channel was calibrated using measured size distribution spectra of nigrosin particles and a Mie calculation. Since the aerosolized nigrosin used for calibration was dry, we determined the imaginary part of the refractive index of nigrosin from the absorbance measurements on solid thin film samples. The obtained refractive index differed considerably from the one determined using aqueous nigrosin solution. PTAAM-2λ has no scattering artefact and features very low uncertainties: 4 % and 6 % for the absorption coefficient at 532 and 1064 nm, respectively, and 9 % for the absorption Ångström exponent. The artefact-free nature of the measurement method allowed us to investigate the artefacts of filter photometers. Both the Aethalometer AE33 and CLAP suffer from cross sensitivity to scattering – this scattering artefact is most pronounced for particles smaller than 70 nm. We observed a strong dependence of the filter multiple scattering parameter on the particle size in the 100–500 nm range. The results from the winter ambient campaign in Ljubljana showed similar multiple scattering parameter values for ambient aerosols and laboratory experiments. The spectral dependence of this parameter resulted in AE33 reporting the absorption Ångström exponent for different soot samples with values biased 0.23–0.35 higher than the PTAAM-2λ measurement. Photothermal interferometry is a promising method for reference aerosol absorption measurements.01A - Beitrag in wissenschaftlicher ZeitschriftPublication A European aerosol phenomenology - 1. physical characteristics of particulate matter at kerbside, urban, rural and background sites in Europe(Elsevier, 05/2004) Van Dingenen, Rita; Raes, Frank; Putaud, Jean-Philippe; Baltensperger, Urs; Charron, Aurélie; Facchini, Maria Cristina; Decesari, Stefano; Fuzzi, Sandro; Gehrig, Robert; Hansson, Hans-Christen; Harrison, Roy M.; Hüglin, Cristoph; Jones, Alan M.; Laj, Paolo; Lorbeer, Gundi; Maenhaut, Willy; Palmgren, Finn; Querol, Xavier; Rodriguez, Sergio; Schneider, Jürgen; ten Brink, Harry; Tunved, Peter; Tørseth, Kjetil; Wehner, Birgit; Weingartner, Ernest; Wiedensohler, Alfred; Wåhlin, PeterThis paper synthesizes data on aerosol (particulate matter, PM) physical characteristics, which were obtained in European aerosol research activities at free-troposphere, natural, rural, near-city, urban, and kerbside sites over the past decade. It covers only two sites in the semi-arid Mediterranean area, and lacks data from Eastern Europe. The data include PM10 and/or PM2.5 mass concentrations, and aerosol particle size distributions. Such data sets are more comprehensive than those currently provided by air quality monitoring networks (e.g. EMEP, EUROAIRNET). Data available from 31 sites in Europe (called “The Network”) were reviewed. They were processed and plotted to allow comparisons in spite of differences in the sampling and analytical techniques used in various studies. A number of conclusions are drawn as follows: Background annual average PM10 and PM2.5 mass concentrations for continental Europe are 7.0±4.1 and 4.8±2.4 μg mˉ³, respectively. The EU 2005 annual average PM10 standard of 40 μg mˉ³ is exceeded at a few sites in The Network. At all near city, urban and kerbside sites, the EU 2010 annual average PM10 standard of 20 μg mˉ³, as well as the US-EPA annual average PM2.5 standard of 15 μg mˉ³ are exceeded. In certain regions, PM10 and PM2.5 in cities are strongly affected by the regional aerosol background. There is no “universal” (i.e. valid for all sites) ratio between PM2.5 and PM10 mass concentrations, although fairly constant ratios do exist at individual sites. There is no universal correlation between PM mass concentration on the one hand, and total particle number concentration on the other hand, although a ‘baseline’ ratio between number and mass is found for sites not affected by local emissions. This paper is the first part of two companion papers of which the second part describes chemical characteristics.01A - Beitrag in wissenschaftlicher ZeitschriftPublication A European aerosol phenomenology - 6. Scattering properties of atmospheric aerosol particles from 28 ACTRIS sites(Copernicus, 2018) Pandolfi, Marco; Alados-Arboledas, Lucas; Alastuey, Andrés; Andrade, Marcos; Angelov, Christo; Artiñano, Begoña; Backman, John; Baltensperger, Urs; Bonasoni, Paolo; Bukowiecki, Nicolas; Collaud Coen, Martine; Conil, Sébastien; Coz, Esther; Crenn, Vincent; Dudoitis, Vadimas; Ealo, Marina; Eleftheriadis, Kostas; Favez, Olivier; Fetfatzis, Prodromos; Fiebig, Markus; Flentje, Harald; Ginot, Patrick; Gysel, Martin; Henzing, Bas; Hoffer, Andras; Holubova Smejkalova, Adela; Kalapov, Ivo; Kalivitis, Nikos; Kouvarakis, Giorgos; Kristensson, Adam; Kulmala, Markku; Lihavainen, Heikki; Lunder, Chris; Luoma, Krista; Lyamani, Hassan; Marinoni, Angela; Mihalopoulos, Nikolaos; Moerman, Marcel; Nicolas, José; O'Dowd, Colin D.; Petäjä, Tuukka; Petit, Jean-Eudes; Pichon, Jean Marc; Prokopciuk, Nina; Putaud, Jean-Philippe; Rodríguez, Sergio; Sciare, Jean; Sellegri, Karine; Swietlicki, Erik; Titos, Gloria; Tuch, Thomas; Tunved, Peter; Ulevicius, Vidmantas; Vaishya, Aditya; Vana, Milan; Virkkula, Aki; Vratolis, Stergios; Weingartner, Ernest; Wiedensohler, Alfred; Laj, PaoloThis paper presents the light-scattering properties of atmospheric aerosol particles measured over the past decade at 28 ACTRIS observatories, which are located mainly in Europe. The data include particle light scattering (σsp) and hemispheric backscattering (σbsp) coefficients, scattering Ångström exponent (SAE), backscatter fraction (BF) and asymmetry parameter (g). An increasing gradient of σsp is observed when moving from remote environments (arctic/mountain) to regional and to urban environments. At a regional level in Europe, σsp also increases when moving from Nordic and Baltic countries and from western Europe to central/eastern Europe, whereas no clear spatial gradient is observed for other station environments. The SAE does not show a clear gradient as a function of the placement of the station. However, a west-to-east-increasing gradient is observed for both regional and mountain placements, suggesting a lower fraction of fine-mode particle in western/south-western Europe compared to central and eastern Europe, where the fine-mode particles dominate the scattering. The g does not show any clear gradient by station placement or geographical location reflecting the complex relationship of this parameter with the physical properties of the aerosol particles. Both the station placement and the geographical location are important factors affecting the intra-annual variability. At mountain sites, higher σsp and SAE values are measured in the summer due to the enhanced boundary layer influence and/or new particle-formation episodes. Conversely, the lower horizontal and vertical dispersion during winter leads to higher σsp values at all low-altitude sites in central and eastern Europe compared to summer. These sites also show SAE maxima in the summer (with corresponding g minima). At all sites, both SAE and g show a strong variation with aerosol particle loading. The lowest values of g are always observed together with low σsp values, indicating a larger contribution from particles in the smaller accumulation mode. During periods of high σsp values, the variation of g is less pronounced, whereas the SAE increases or decreases, suggesting changes mostly in the coarse aerosol particle mode rather than in the fine mode. Statistically significant decreasing trends of σsp are observed at 5 out of the 13 stations included in the trend analyses. The total reductions of σsp are consistent with those reported for PM2.5 and PM10 mass concentrations over similar periods across Europe.01A - Beitrag in wissenschaftlicher ZeitschriftPublication 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, Paolo01A - Beitrag in wissenschaftlicher ZeitschriftPublication A global study of hygroscopicity-driven light-scattering enhancement in the context of other in situ aerosol optical properties(Copernicus, 2021) Titos, Gloria; Burgos, María A.; Zieger, Paul; Alados-Arboledas, Lucas; Baltensperger, Urs; Jefferson, Anne; Sherman, James; Weingartner, Ernest; Henzing, Bas; Luoma, Krista; O'Dowd, Colin; Wiedensohler, Alfred; Andrews, ElisabethThe scattering and backscattering enhancement factors (f(RH) and fb(RH)) describe how aerosol particle light scattering and backscattering, respectively, change with relative humidity (RH). They are important parameters in estimating direct aerosol radiative forcing (DARF). In this study we use the dataset presented in Burgos et al. (2019) that compiles f(RH) and fb(RH) measurements at three wavelengths (i.e., 450, 550 and 700 nm) performed with tandem nephelometer systems at multiple sites around the world. We present an overview of f(RH) and fb(RH) based on both long-term and campaign observations from 23 sites representing a range of aerosol types. The scattering enhancement shows a strong variability from site to site, with no clear pattern with respect to the total scattering coefficient. In general, higher f(RH) is observed at Arctic and marine sites, while lower values are found at urban and desert sites, although a consistent pattern as a function of site type is not observed. The backscattering enhancement fb(RH) is consistently lower than f(RH) at all sites, with the difference between f(RH) and fb(RH) increasing for aerosol with higher f(RH). This is consistent with Mie theory, which predicts higher enhancement of the light scattering in the forward than in the backward direction as the particle takes up water. Our results show that the scattering enhancement is higher for PM1 than PM10 at most sites, which is also supported by theory due to the change in scattering efficiency with the size parameter that relates particle size and the wavelength of incident light. At marine-influenced sites this difference is enhanced when coarse particles (likely sea salt) predominate. For most sites, f(RH) is observed to increase with increasing wavelength, except at sites with a known dust influence where the spectral dependence of f(RH) is found to be low or even exhibit the opposite pattern. The impact of RH on aerosol properties used to calculate radiative forcing (e.g., single-scattering albedo, ω0, and backscattered fraction, b) is evaluated. The single-scattering albedo generally increases with RH, while b decreases. The net effect of aerosol hygroscopicity on radiative forcing efficiency (RFE) is an increase in the absolute forcing effect (negative sign) by a factor of up to 4 at RH = 90 % compared to dry conditions (RH < 40 %). Because of the scarcity of scattering enhancement measurements, an attempt was made to use other more commonly available aerosol parameters (i.e., ω0 and scattering Ångström exponent, αsp) to parameterize f(RH). The majority of sites (75 %) showed a consistent trend with ω0 (higher f(RH = 85 %) for higher ω0), while no clear pattern was observed between f(RH = 85 %) and αsp. This suggests that aerosol ω0 is more promising than αsp as a surrogate for the scattering enhancement factor, although neither parameter is ideal. Nonetheless, the qualitative relationship observed between ω0 and f(RH) could serve as a constraint on global model simulations.01A - Beitrag in wissenschaftlicher ZeitschriftPublication A synthesis of cloud condensation nuclei counter (CCNC) measurements within the EUCAARI network(Copernicus, 2015) Paramonov, Mikhail; Kerminen, Veli-Matti; Gysel, Martin; Aalto, Pasi Pekka; Andreae, Meinrat O.; Asmi, Eija; Baltensperger, Urs; Bougiatioti, Aikaterini; Brus, David; Frank, Göran; Good, Nicholas; Gunthe, Sachin S.; Hao, Liqing; Irwin, Martin; Jaatinen, Antti; Jurányi, Zsófia; King, S. M.; Kortelainen, Aki; Kristensson, Adam; Lihavainen, Heikki; Kulmala, Markku; Lohmann, Ulrike; Martin, Scot T.; McFiggans, Gordon; Mihalopoulos, Nikolaos; Nenes, Athanasios; O'Dowd, Colin D.; Ovadnevaite, Jurgita; Petäjä, Tuukka; Pöschl, Ulrich; Roberts, Greg; Rose, Diana; Svenningsson, Birgitta; Swietlicki, Erik; Weingartner, Ernest; Whitehead, James; Wiedensohler, Alfred; Wittbom, Cerina; Sierau, BerkoCloud 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.01A - Beitrag in wissenschaftlicher ZeitschriftPublication Aerosol decadal trends – Part 2. In-situ aerosol particle number concentrations at GAW and ACTRIS stations(Copernicus, 2013) Asmi, Ari; Collaud Coen, Martine; Ogren, John A.; Andrews, Elisabeth; Sheridan, Patrick; Jefferson, Anne; Weingartner, Ernest; Baltensperger, Urs; Bukowiecki, Nicolas ; Lihavainen, Heikki; Kivekäs, Niku; Asmi, Eija; Aalto, Pasi Pekka; Kulmala, Markku; Wiedensohler, Alfred; Birmili, Wolfram; Hamed, Amar; O'Dowd, Colin; Jennings, Stephen G.; Weller, Rolf; Flentje, Harald; Fjaeraa, Ann Mari; Fiebig, Markus; Myhre, Cathrine Lund; Hallar, Anna Gannet; Swietlicki, Erik; Kristensson, Adam; Laj, PaoloWe have analysed the trends of total aerosol particle number concentrations (N) measured at long-term measurement stations involved either in the Global Atmosphere Watch (GAW) and/or EU infrastructure project ACTRIS. The sites are located in Europe, North America, Antarctica, and on Pacific Ocean islands. The majority of the sites showed clear decreasing trends both in the full-length time series, and in the intra-site comparison period of 2001–2010, especially during the winter months. Several potential driving processes for the observed trends were studied, and even though there are some similarities between N trends and air temperature changes, the most likely cause of many northern hemisphere trends was found to be decreases in the anthropogenic emissions of primary particles, SO2 or some co-emitted species. We could not find a consistent agreement between the trends of N and particle optical properties in the few stations with long time series of all of these properties. The trends of N and the proxies for cloud condensation nuclei (CCN) were generally consistent in the few European stations where the measurements were available. This work provides a useful comparison analysis for modelling studies of trends in aerosol number concentrations.01A - Beitrag in wissenschaftlicher ZeitschriftPublication 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, YaqiangAbsorption 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 ZeitschriftPublication 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, MarkkuWe 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 ZeitschriftPublication 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, JunyingWe 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 ZeitschriftPublication 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, MarkkuThe 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 ZeitschriftPublication 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, Ernest01A - Beitrag in wissenschaftlicher ZeitschriftPublication 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 ZeitschriftPublication 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, MarkkuTwo 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 ZeitschriftPublication Predicting hygroscopic growth using single particle chemical composition estimates(Wiley, 2014) Healy, Robert M.; Evans, Greg J.; Murphy, Michael; Jurányi, Zsófia; Tritscher, Torsten; Laborde, Marie; Weingartner, Ernest; Gysel, Martin; Poulain, Laurent; Kamilli, Katharina A.; Wiedensohler, Alfred; O'Connor, Ian P.; McGillicuddy, Eoin; Sodeau, John R.; Wenger, John C.Single particle mass spectral data, collected in Paris, France, have been used to predict hygroscopic growth at the single particle level. The mass fractions of black carbon, organic aerosol, ammonium, nitrate, and sulphate present in each particle were estimated using a combination of single particle mass spectrometer and bulk aerosol chemical composition measurements. The Zdanovskii‐Stokes‐Robinson (ZSR) approach was then applied to predict hygroscopic growth factors based on these mass fraction estimates. Smaller particles with high black carbon mass fractions and low inorganic ion mass fractions exhibited the lowest predicted growth factors, while larger particles with high inorganic ion mass fractions exhibited the highest growth factors. Growth factors were calculated for subsaturated relative humidity (90%) to enable comparison with hygroscopic tandem differential mobility analyzer measurements. Mean predicted and measured hygroscopic growth factors for 110, 165, and 265 nm particles were found to agree within 6%. Single particle‐based ZSR hygroscopicity estimates offer an advantage over bulk aerosol composition‐based hygroscopicity estimates by providing additional chemical mixing state information. External mixing can be determined for particles of a given diameter through examination of the predicted hygroscopic growth factor distributions. Using this approach, 110 nm and 265 nm particles were found to be predominantly internally mixed; however, external mixing of 165 nm particles was observed periodically when thinly coated and thickly coated black carbon particles were simultaneously detected. Single particle‐resolved chemical information will be useful for modeling efforts aimed at constraining cloud condensation nuclei activity and hygroscopic growth.01A - Beitrag in wissenschaftlicher ZeitschriftPublication 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, RoccoIt 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 ZeitschriftPublication Studying the vertical aerosol extinction coefficient by comparing in situ airborne data and elastic backscatter lidar(Copernicus, 2016) Rosati, Bernadette; Herrmann, Erik; Bucci, Silvia; Fierli, Federico; Cairo, Francesco; Gysel, Martin; Tillmann, Ralf; Größ, Johannes; Gobbi, Gian Paolo; Di Liberto, Luca; Di Donfrancesco, Guido; Wiedensohler, Alfred; Weingartner, Ernest; Virtanen, Annele; Mentel, Thomas F.; Baltensperger, UrsVertical profiles of aerosol particle optical properties were explored in a case study near the San Pietro Capofiume (SPC) ground station during the PEGASOS Po Valley campaign in the summer of 2012. A Zeppelin NT airship was employed to investigate the effect of the dynamics of the planetary boundary layer at altitudes between ∼ 50 and 800 m above ground. Determined properties included the aerosol particle size distribution, the hygroscopic growth factor, the effective index of refraction and the light absorption coefficient. The first three parameters were used to retrieve the light scattering coefficient. Simultaneously, direct measurements of both the scattering and absorption coefficient were carried out at the SPC ground station. Additionally, a single wavelength polarization diversity elastic lidar system provided estimates of aerosol extinction coefficients using the Klett method to accomplish the inversion of the signal, for a vertically resolved comparison between in situ and remote-sensing results. Note, however, that the comparison was for the most part done in the altitude range where the overlap function is incomplete and accordingly uncertainties are larger. First, the airborne results at low altitudes were validated with the ground measurements. Agreement within approximately ±25 and ±20 % was found for the dry scattering and absorption coefficient, respectively. The single scattering albedo, ranged between 0.83 and 0.95, indicating the importance of the absorbing particles in the Po Valley region. A clear layering of the atmosphere was observed during the beginning of the flight (until ∼ 10:00 LT – local time) before the mixing layer (ML) was fully developed. Highest extinction coefficients were found at low altitudes, in the new ML, while values in the residual layer, which could be probed at the beginning of the flight at elevated altitudes, were lower. At the end of the flight (after ∼ 12:00 LT) the ML was fully developed, resulting in constant extinction coefficients at all altitudes measured on the Zeppelin NT. Lidar estimates captured these dynamic features well and good agreement was found for the extinction coefficients compared to the in situ results, using fixed lidar ratios (LR) between 30 and 70 sr for the altitudes probed with the Zeppelin. These LR are consistent with values for continental aerosol particles that can be expected in this region.01A - Beitrag in wissenschaftlicher ZeitschriftPublication 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, AntoonCluster~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 ZeitschriftPublication Vertical profiling of aerosol hygroscopic properties in the planetary boundary layer during the PEGASOS campaigns(Copernicus, 2016) Rosati, Bernadette; Gysel, Martin; Rubach, Florian; Mentel, Thomas F.; Goger, Brigitta; Poulain, Laurent; Schlag, Patrick; Miettinen, Pasi; Pajunoja, Aki; Virtanen, Annele; Klein Baltink, Henk; Henzing, Bas; Größ, Johannes; Gobbi, Gian Paolo; Wiedensohler, Alfred; Kiendler-Scharr, Astrid; Decesari, Stefano; Facchini, Maria Cristina; Weingartner, Ernest; Baltensperger, UrsVertical profiles of the aerosol particles hygroscopic properties, their mixing state as well as chemical composition were measured above northern Italy and the Netherlands. An aerosol mass spectrometer (AMS; for chemical composition) and a white-light humidified optical particle spectrometer (WHOPS; for hygroscopic growth) were deployed on a Zeppelin NT airship within the PEGASOS project. This allowed one to investigate the development of the different layers within the planetary boundary layer (PBL), providing a unique in situ data set for airborne aerosol particles properties in the first kilometre of the atmosphere. Profiles measured during the morning hours on 20 June 2012 in the Po Valley, Italy, showed an increased nitrate fraction at ∼ 100 m above ground level (a.g.l.) coupled with enhanced hygroscopic growth compared to ∼ 700 m a. g. l. This result was derived from both measurements of the aerosol composition and direct measurements of the hygroscopicity, yielding hygroscopicity parameters (κ) of 0.34 ± 0.12 and 0.19 ± 0.07 for 500 nm particles, at ∼ 100 and ∼ 700 m a. g. l., respectively. The difference is attributed to the structure of the PBL at this time of day which featured several independent sub-layers with different types of aerosols. Later in the day the vertical structures disappeared due to the mixing of the layers and similar aerosol particle properties were found at all probed altitudes (mean κ ≈ 0.18 ± 0.07). The aerosol properties observed at the lowest flight level (100 m a. g. l.) were consistent with parallel measurements at a ground site, both in the morning and afternoon. Overall, the aerosol particles were found to be externally mixed, with a prevailing hygroscopic fraction. The flights near Cabauw in the Netherlands in the fully mixed PBL did not feature altitude-dependent characteristics. Particles were also externally mixed and had an even larger hygroscopic fraction compared to the results in Italy. The mean κ from direct measurements was 0.28 ± 0.10, thus considerably higher than κ values measured in Italy in the fully mixed PBL.01A - Beitrag in wissenschaftlicher Zeitschrift