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Now showing 1 - 10 of 13
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    CCN production by new particle formation in the free troposphere
    (München : European Geopyhsical Union, 2017) Rose, Clémence; Sellegri, Karine; Moreno, Isabel; Velarde, Fernando; Ramonet, Michel; Weinhold, Kay; Krejc, Radovan; Andrade, Marcos; Wiedensohler, Alfred; Ginot, Patrick; Laj, Paolo
    Global models predict that new particle formation (NPF) is, in some environments, responsible for a substantial fraction of the total atmospheric particle number concentration and subsequently contributes significantly to cloud condensation nuclei (CCN) concentrations. NPF events were frequently observed at the highest atmospheric observatory in the world, on Chacaltaya (5240 m a.s.l.), Bolivia. The present study focuses on the impact of NPF on CCN population. Neutral cluster and Air Ion Spectrometer and mobility particle size spectrometer measurements were simultaneously used to follow the growth of particles from cluster sizes down to ∼ 2 nm up to CCN threshold sizes set to 50, 80 and 100 nm. Using measurements performed between 1 January and 31 December 2012, we found that 61 % of the 94 analysed events showed a clear particle growth and significant enhancement of the CCN-relevant particle number concentration. We evaluated the contribution of NPF, relative to the transport and growth of pre-existing particles, to CCN size. The averaged production of 50 nm particles during those events was 5072, and 1481 cm−3 for 100 nm particles, with a larger contribution of NPF compared to transport, especially during the wet season. The data set was further segregated into boundary layer (BL) and free troposphere (FT) conditions at the site. The NPF frequency of occurrence was higher in the BL (48 %) compared to the FT (39 %). Particle condensational growth was more frequently observed for events initiated in the FT, but on average faster for those initiated in the BL, when the amount of condensable species was most probably larger. As a result, the potential to form new CCN was higher for events initiated in the BL (67 % against 53 % in the FT). In contrast, higher CCN number concentration increases were found when the NPF process initially occurred in the FT, under less polluted conditions. This work highlights the competition between particle growth and the removal of freshly nucleated particles by coagulation processes. The results support model predictions which suggest that NPF is an effective source of CCN in some environments, and thus may influence regional climate through cloud-related radiative processes.
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    Long-term observations of tropospheric particle number size distributions and equivalent black carbon mass concentrations in the German Ultrafine Aerosol Network (GUAN)
    (München : European Geopyhsical Union, 2016) Birmili, Wolfram; Weinhold, Kay; Rasch, Fabian; Sonntag, André; Sun, Jia; Merkel, Maik; Wiedensohler, Alfred; Bastian, Susanne; Schladitz, Alexander; Löschau, Gunter; Cyrys, Josef; Pitz, Mike; Gu, Jianwei; Kusch, Thomas; Flentje, Harald; Quass, Ulrich; Kaminski, Heinz; Kuhlbusch, Thomas A.J.; Meinhardt, Frank; Schwerin, Andreas; Bath, Olaf; Ries, Ludwig; Gerwig, Holger; Wirtz, Klaus; Fiebig, Markus
    The German Ultrafine Aerosol Network (GUAN) is a cooperative atmospheric observation network, which aims at improving the scientific understanding of aerosol-related effects in the troposphere. The network addresses research questions dedicated to both climate- and health-related effects. GUAN's core activity has been the continuous collection of tropospheric particle number size distributions and black carbon mass concentrations at 17 observation sites in Germany. These sites cover various environmental settings including urban traffic, urban background, rural background, and Alpine mountains. In association with partner projects, GUAN has implemented a high degree of harmonisation of instrumentation, operating procedures, and data evaluation procedures. The quality of the measurement data is assured by laboratory intercomparisons as well as on-site comparisons with reference instruments. This paper describes the measurement sites, instrumentation, quality assurance, and data evaluation procedures in the network as well as the EBAS repository, where the data sets can be obtained (doi:10.5072/guan).
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    Intercomparison of 15 aerodynamic particle size spectrometers (APS 3321): Uncertainties in particle sizing and number size distribution
    (München : European Geopyhsical Union, 2016) Pfeifer, Sascha; Müller, Thomas; Weinhold, Kay; Zikova, Nadezda; dos Santos, Sebastiao Martins; Marinoni, Angela; Bischof, Oliver F.; Kykal, Carsten; Ries, Ludwig; Meinhardt, Frank; Aalto, Pasi; Mihalopoulos, Nikolaos; Wiedensohler, Alfred
    Aerodynamic particle size spectrometers are a well-established method to measure number size distributions of coarse mode particles in the atmosphere. Quality assurance is essential for atmospheric observational aerosol networks to obtain comparable results with known uncertainties. In a laboratory study within the framework of ACTRIS (Aerosols, Clouds, and Trace gases Research Infrastructure Network), 15 aerodynamic particle size spectrometers (APS model 3321, TSI Inc., St. Paul, MN, USA) were compared with a focus on flow rates, particle sizing, and the unit-to-unit variability of the particle number size distribution. Flow rate deviations were relatively small (within a few percent), while the sizing accuracy was found to be within 10 % compared to polystyrene latex (PSL) reference particles. The unit-to-unit variability in terms of the particle number size distribution during this study was within 10 % to 20 % for particles in the range of 0.9 up to 3 µm, which is acceptable for atmospheric measurements. For particles smaller than that, the variability increased up to 60 %, probably caused by differences in the counting efficiencies of individual units. Number size distribution data for particles smaller than 0.9 µm in aerodynamic diameter should only be used with caution. For particles larger than 3 µm, the unit-to-unit variability increased as well. A possible reason is an insufficient sizing accuracy in combination with a steeply sloping particle number size distribution and the increasing uncertainty due to decreasing counting. Particularly this uncertainty of the particle number size distribution must be considered if higher moments of the size distribution such as the particle volume or mass are calculated, which require the conversion of the aerodynamic diameter measured to a volume equivalent diameter. In order to perform a quantitative quality assurance, a traceable reference method for the particle number concentration in the size range 0.5–3 µm is needed.
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    Phenomenology of ultrafine particle concentrations and size distribution across urban Europe
    (Amsterdam [u.a.] : Elsevier Science, 2023) Trechera, Pedro; Garcia-Marlès, Meritxell; Liu, Xiansheng; Reche, Cristina; Pérez, Noemí; Savadkoohi, Marjan; Beddows, David; Salma, Imre; Vörösmarty, Máté; Casans, Andrea; Casquero-Vera, Juan Andrés; Hueglin, Christoph; Marchand, Nicolas; Chazeau, Benjamin; Gille, Grégory; Kalkavouras, Panayiotis; Mihalopoulos, Nikos; Ondracek, Jakub; Zikova, Nadia; Niemi, Jarkko V.; Manninen, Hanna E.; Green, David C.; Tremper, Anja H.; Norman, Michael; Vratolis, Stergios; Eleftheriadis, Konstantinos; Gómez-Moreno, Francisco J.; Alonso-Blanco, Elisabeth; Gerwig, Holger; Wiedensohler, Alfred; Weinhold, Kay; Merkel, Maik; Bastian, Susanne; Petit, Jean-Eudes; Favez, Olivier; Crumeyrolle, Suzanne; Ferlay, Nicolas; Martins Dos Santos, Sebastiao; Putaud, Jean-Philippe; Timonen, Hilkka; Lampilahti, Janne; Asbach, Christof; Wolf, Carmen; Kaminski, Heinz; Altug, Hicran; Hoffmann, Barbara; Rich, David Q.; Pandolfi, Marco; Harrison, Roy M.; Hopke, Philip K.; Petäjä, Tuukka; Alastuey, Andrés; Querol, Xavier
    The 2017–2019 hourly particle number size distributions (PNSD) from 26 sites in Europe and 1 in the US were evaluated focusing on 16 urban background (UB) and 6 traffic (TR) sites in the framework of Research Infrastructures services reinforcing air quality monitoring capacities in European URBAN & industrial areaS (RI-URBANS) project. The main objective was to describe the phenomenology of urban ultrafine particles (UFP) in Europe with a significant air quality focus. The varying lower size detection limits made it difficult to compare PN concentrations (PNC), particularly PN10-25, from different cities. PNCs follow a TR > UB > Suburban (SUB) order. PNC and Black Carbon (BC) progressively increase from Northern Europe to Southern Europe and from Western to Eastern Europe. At the UB sites, typical traffic rush hour PNC peaks are evident, many also showing midday-morning PNC peaks anti-correlated with BC. These peaks result from increased PN10-25, suggesting significant PNC contributions from nucleation, fumigation and shipping. Site types to be identified by daily and seasonal PNC and BC patterns are: (i) PNC mainly driven by traffic emissions, with marked correlations with BC on different time scales; (ii) marked midday/morning PNC peaks and a seasonal anti-correlation with PNC/BC; (iii) both traffic peaks and midday peaks without marked seasonal patterns. Groups (ii) and (iii) included cities with high insolation. PNC, especially PN25-800, was positively correlated with BC, NO2, CO and PM for several sites. The variable correlation of PNSD with different urban pollutants demonstrates that these do not reflect the variability of UFP in urban environments. Specific monitoring of PNSD is needed if nanoparticles and their associated health impacts are to be assessed. Implementation of the CEN-ACTRIS recommendations for PNSD measurements would provide comparable measurements, and measurements of <10 nm PNC are needed for full evaluation of the health effects of this size fraction.
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    A phenomenology of new particle formation (NPF) at 13 European sites
    (Katlenburg-Lindau : European Geosciences Union, 2021) Bousiotis, Dimitrios; Pope, Francis D.; Beddows, David C. S.; Dall'Osto, Manuel; Massling, Andreas; Nøjgaard, Jakob Klenø; Nordstrøm, Claus; Niemi, Jarkko V.; Portin, Harri; Petäjä, Tuukka; Perez, Noemi; Alastuey, Andrés; Querol, Xavier; Kouvarakis, Giorgos; Mihalopoulos, Nikos; Vratolis, Stergios; Eleftheriadis, Konstantinos; Wiedensohler, Alfred; Weinhold, Kay; Merkel, Maik; Tuch, Thomas; Harrison, Roy M.
    New particle formation (NPF) events occur almost everywhere in the world and can play an important role as a particle source. The frequency and characteristics of NPF events vary spatially, and this variability is yet to be fully understood. In the present study, long-term particle size distribution datasets (minimum of 3 years) from 13 sites of various land uses and climates from across Europe were studied, and NPF events, deriving from secondary formation and not traffic-related nucleation, were extracted and analysed. The frequency of NPF events was consistently found to be higher at rural background sites, while the growth and formation rates of newly formed particles were higher at roadsides (though in many cases differences between the sites were small), underlining the importance of the abundance of condensable compounds of anthropogenic origin found there. The growth rate was higher in summer at all rural background sites studied. The urban background sites presented the highest uncertainty due to greater variability compared to the other two types of site. The origin of incoming air masses and the specific conditions associated with them greatly affect the characteristics of NPF events. In general, cleaner air masses present higher probability for NPF events, while the more polluted ones show higher growth rates. However, different patterns of NPF events were found, even at sites in close proximity (<ĝ€¯200ĝ€¯km), due to the different local conditions at each site. Region-wide events were also studied and were found to be associated with the same conditions as local events, although some variability was found which was associated with the different seasonality of the events at two neighbouring sites. NPF events were responsible for an increase in the number concentration of ultrafine particles of more than 400ĝ€¯% at rural background sites on the day of their occurrence. The degree of enhancement was less at urban sites due to the increased contribution of other sources within the urban environment. It is evident that, while some variables (such as solar radiation intensity, relative humidity, or the concentrations of specific pollutants) appear to have a similar influence on NPF events across all sites, it is impossible to predict the characteristics of NPF events at a site using just these variables, due to the crucial role of local conditions. © Author(s) 2021.
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    First results of the "Carbonaceous Aerosol in Rome and Environs (CARE)" Experiment: Beyond current standards for PM10
    (Basel, Switzerland : MDPI AG, 2017) Costabile, Francesca; Alas, Honey; Aufderheide, Michaela; Avino, Pasquale; Amato, Fulvio; Argentini, Stefania; Barnaba, Francesca; Berico, Massimo; Bernardoni, Vera; Biondi, Riccardo; Casasanta, Giampietro; Ciampichetti, Spartaco; Calzolai, Giulia; Canepari, Silvia; Conidi, Alessandro; Cordelli, Eugenia; Di Ianni, Antonio; Di Liberto, Luca; Facchini, Maria Cristina; Facci, Andrea; Frasca, Daniele; Gilardoni, Stefania; Grollino, Maria Giuseppa; Gualtieri, Maurizio; Lucarelli, Franco; Malaguti, Antonella; Manigrasso, Maurizio; Montagnoli, Mauro; Nava, Silvia; Perrino, Cinzia; Padoan, Elio; Petenko, Igor; Querol, Xavier; Simonetti, Giulia; Tranfo, Giovanna; Ubertini, Stefano; Valli, Gianluigi; Valentini, Sara; Vecchi, Roberta; Volpi, Francesca; Weinhold, Kay; Wiedensohler, Alfred; Zanini, Gabriele; Gobbi, Gian Paolo; Petralia, Ettore
    In February 2017 the “Carbonaceous Aerosol in Rome and Environs (CARE)” experiment was carried out in downtown Rome to address the following specific questions: what is the color, size, composition, and toxicity of the carbonaceous aerosol in the Mediterranean urban background area of Rome? The motivation of this experiment is the lack of understanding of what aerosol types are responsible for the severe risks to human health posed by particulate matter (PM) pollution, and how carbonaceous aerosols influence radiative balance. Physicochemical properties of the carbonaceous aerosol were characterised, and relevant toxicological variables assessed. The aerosol characterisation includes: (i) measurements with high time resolution (min to 1–2 h) at a fixed location of black carbon (eBC), elemental carbon (EC), organic carbon (OC), particle number size distribution (0.008–10 μm), major non refractory PM1 components, elemental composition, wavelength-dependent optical properties, and atmospheric turbulence; (ii) 24-h measurements of PM10 and PM2.5 mass concentration, water soluble OC and brown carbon (BrC), and levoglucosan; (iii) mobile measurements of eBC and size distribution around the study area, with computational fluid dynamics modeling; (iv) characterisation of road dust emissions and their EC and OC content. The toxicological assessment includes: (i) preliminary evaluation of the potential impact of ultrafine particles on lung epithelia cells (cultured at the air liquid interface and directly exposed to particles); (ii) assessment of the oxidative stress induced by carbonaceous aerosols; (iii) assessment of particle size dependent number doses deposited in different regions of the human body; (iv) PAHs biomonitoring (from the participants into the mobile measurements). The first experimental results of the CARE experiment are presented in this paper. The objective here is to provide baseline levels of carbonaceous aerosols for Rome, and to address future research directions. First, we found that BC and EC mass concentration in Rome are larger than those measured in similar urban areas across Europe (the urban background mass concentration of eBC in Rome in winter being on average 2.6 ± 2.5 μg · m−3, mean eBC at the peak level hour being 5.2 (95% CI = 5.0–5.5) μg · m−3 ). Then, we discussed significant variations of carbonaceous aerosol properties occurring with time scales of minutes, and questioned on the data averaging period used in current air quality standard for PM10 (24-h). Third, we showed that the oxidative potential induced by aerosol depends on particle size and composition, the effects of toxicity being higher with lower mass concentrations and smaller particle size. Albeit this is a preliminary analysis, findings reinforce the need for an urgent update of existing air quality standards for PM10 and PM2.5 with regard to particle composition and size distribution, and data averaging period. Our results reinforce existing concerns about the toxicity of carbonaceous aerosols, support the existing evidence indicating that particle size distribution and composition may play a role in the generation of this toxicity, and remark the need to consider a shorter averaging period (<1 h) in these new standards.
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    Decreasing trends of particle number and black carbon mass concentrations at 16 observational sites in Germany from 2009 to 2018
    (Katlenburg-Lindau : EGU, 2020) Sun, Jia; Birmili, Wolfram; Hermann, Markus; Tuch, Thomas; Weinhold, Kay; Merkel, Maik; Rasch, Fabian; Müller, Thomas; Schladitz, Alexander; Bastian, Susanne; Löschau, Gunter; Cyrys, Josef; Gu, Jianwei; Flentje, Harald; Briel, Björn; Asbach, Christoph; Kaminski, Heinz; Ries, Ludwig; Sohmer, Ralf; Gerwig, Holger; Wirtz, Klaus; Meinhardt, Frank; Schwerin, Andreas; Bath, Olaf; Ma, Nan; Wiedensohler, Alfred
    Anthropogenic emissions are dominant contributors to air pollution. Consequently, mitigation policies have been attempted since the 1990s in Europe to reduce pollution by anthropogenic emissions. To evaluate the effectiveness of these mitigation policies, the German Ultrafine Aerosol Network (GUAN) was established in 2008, focusing on black carbon (BC) and sub-micrometre aerosol particles. In this study, long-term trends of atmospheric particle number concentrations (PNCs) and equivalent BC (eBC) mass concentration over a 10-year period (2009-2018) were determined for 16 GUAN sites ranging from roadside to high Alpine environments. Overall, statistically significant decreasing trends are found for most of these parameters and environments in Germany. The annual relative slope of eBC mass concentration varies between-13.1% and-1.7% per year. The slopes of the PNCs vary from-17.2% to-1.7 %,-7.8% to-1.1 %, and-11.1% to-1.2% per year for 10-30, 30-200, and 200-800 nm size ranges, respectively. The reductions in various anthropogenic emissions are found to be the dominant factors responsible for the decreasing trends of eBC mass concentration and PNCs. The diurnal and seasonal variations in the trends clearly show the effects of the mitigation policies for road transport and residential emissions. The influences of other factors such as air masses, precipitation, and temperature were also examined and found to be less important or negligible. This study proves that a combination of emission mitigation policies can effectively improve the air quality on large spatial scales. It also suggests that a long-term aerosol measurement network at multi-type sites is an efficient and necessary tool for evaluating emission mitigation policies. © 2020 Author(s).
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    A global analysis of climate-relevant aerosol properties retrieved from the network of Global Atmosphere Watch (GAW) near-surface observatories
    (Katlenburg-Lindau : Copernicus, 2020) Laj, Paolo; Bigi, Alessandro; Rose, Clémence; Andrews, Elisabeth; Lund Myhre, Cathrine; Collaud Coen, Martine; Lin, Yong; Wiedensohler, Alfred; Schulz, Michael; Ogren, John A.; Fiebig, Markus; Prenni, Anthony; Reisen, Fabienne; Romano, Salvatore; Sellegri, Karine; Sharma, Sangeeta; Schauer, Gerhard; Sheridan, Patrick; Sherman, James Patrick; Schütze, Maik; Schwerin, Andreas; Tuch, Thomas; Sohmer, Ralf; Sorribas, Mar; Steinbacher, Martin; Sun, Junying; Titos, Gloria; Toczko, Barbara; Tulet, Pierre; Tunved, Peter; Vakkari, Ville; Velarde, Fernando; Velasquez, Patricio; Villani, Paolo; Vratolis, Sterios; Wang, Sheng-Hsiang; Weinhold, Kay; Gliß, Jonas; Weller, Rolf; Yela, Margarita; Yus-Diez, Jesus; Zdimal, Vladimir; Zieger, Paul; Zikova, Nadezda; Mortier, Augustin; Pandolfi, Marco; Petäja, Tuukka; Kim, Sang-Woo; Aas, Wenche; Putaud, Jean-Philippe; Mayol-Bracero, Olga; Keywood, Melita; Labrador, Lorenzo; Aalto, Pasi; Ahlberg, Erik; Alados Arboledas, Lucas; Alastuey, Andrés; Andrade, Marcos; Artíñano, Begoña; Ausmeel, Stina; Arsov, Todor; Asmi, Eija; Backman, John; Baltensperger, Urs; Bastian, Susanne; Bath, Olaf; Beukes, Johan Paul; Brem, Benjamin T.; Bukowiecki, Nicolas; Conil, Sébastien; Couret, Cedric; Day, Derek; Dayantolis, Wan; Degorska, Anna; Eleftheriadis, Konstantinos; Fetfatzis, Prodromos; Favez, Olivier; Flentje, Harald; Gini, Maria I.; Gregorič, Asta; Gysel-Beer, Martin; Hallar, A. Gannet; Hand, Jenny; Hoffer, Andras; Hueglin, Christoph; Hooda, Rakesh K.; Hyvärinen, Antti; Kalapov, Ivo; Kalivitis, Nikos; Kasper-Giebl, Anne; Kim, Jeong Eun; Kouvarakis, Giorgos; Kranjc, Irena; Krejci, Radovan; Kulmala, Markku; Labuschagne, Casper; Lee, Hae-Jung; Lihavainen, Heikki; Lin, Neng-Huei; Löschau, Gunter; Luoma, Krista; Marinoni, Angela; Martins Dos Santos, Sebastiao; Meinhardt, Frank; Merkel, Maik; Metzger, Jean-Marc; Mihalopoulos, Nikolaos; Nguyen, Nhat Anh; Ondracek, Jakub; Pérez, Noemi; Perrone, Maria Rita; Petit, Jean-Eudes; Picard, David; Pichon, Jean-Marc; Pont, Veronique; Prats, Natalia
    Aerosol particles are essential constituents of the Earth's atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.
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    Real World Vehicle Emission Factors for Black Carbon Derived from Longterm In-Situ Measurements and Inverse Modelling
    (Basel : MDPI, 2021) Wiesner, Anne; Pfeifer, Sascha; Merkel, Maik; Tuch, Thomas; Weinhold, Kay; Wiedensohler, Alfred
    Black carbon (BC) is one of the most harmful substances within traffic emissions, contributing considerably to urban pollution. Nevertheless, it is not explicitly regulated and the official laboratory derived emission factors are barely consistent with real world emissions. However, realistic emission factors (EFs) are crucial for emission, exposure, and climate modelling. A unique dataset of 10 years (2009–2018) of roadside and background measurements of equivalent black carbon (eBC) concentration made it possible to estimate real world traffic EFs and observe their change over time. The pollutant dispersion was modelled using the Operational Street Pollution Model (OSPM). The EFs for eBC are derived for this specific measurement site in a narrow but densely trafficked street canyon in Leipzig, Germany. The local conditions and fleet composition can be considered as typical for an inner-city traffic scenario in a Western European city. The fleet is composed of 22% diesel and 77% petrol cars in the passenger car segment, with an unknown proportion of direct injection engines. For the mixed fleet the eBC EF was found to be 48 mg km−1 in the long-term average. Accelerated by the introduction of a low emission zone, the EFs decreased over the available time period from around 70 mg km−1 to 30 – 40 mg km−1 . Segregation into light (<3.5 t) and heavy (>3.5 t) vehicles resulted in slightly lower estimates for the light vehicles than for the mixed fleet, and one order of magnitude higher values for the heavy vehicles. The found values are considerably higher than comparable emission standards for particulate matter and even the calculations of the Handbook Emission Factors for Road Transport (HBEFA), which is often used as emission model input. © 2020 by the authors. Licensee MDPI, Basel, Switzerland.
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    A full year of aerosol size distribution data from the central Arctic under an extreme positive Arctic Oscillation: insights from the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition
    (Katlenburg-Lindau : EGU, 2023) Boyer, Matthew; Aliaga, Diego; Pernov, Jakob Boyd; Angot, Hélène; Quéléver, Lauriane L. J.; Dada, Lubna; Heutte, Benjamin; Dall'Osto, Manuel; Beddows, David C. S.; Brasseur, Zoé; Beck, Ivo; Bucci, Silvia; Duetsch, Marina; Stohl, Andreas; Laurila, Tiia; Asmi, Eija; Massling, Andreas; Thomas, Daniel Charles; Nøjgaard, Jakob Klenø; Chan, Tak; Sharma, Sangeeta; Tunved, Peter; Krejci, Radovan; Hansson, Hans Christen; Bianchi, Federico; Lehtipalo, Katrianne; Wiedensohler, Alfred; Weinhold, Kay; Kulmala, Markku; Petäjä, Tuukka; Sipilä, Mikko; Schmale, Julia; Jokinen, Tuija
    The Arctic environment is rapidly changing due to accelerated warming in the region. The warming trend is driving a decline in sea ice extent, which thereby enhances feedback loops in the surface energy budget in the Arctic. Arctic aerosols play an important role in the radiative balance and hence the climate response in the region, yet direct observations of aerosols over the Arctic Ocean are limited. In this study, we investigate the annual cycle in the aerosol particle number size distribution (PNSD), particle number concentration (PNC), and black carbon (BC) mass concentration in the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition. This is the first continuous, year-long data set of aerosol PNSD ever collected over the sea ice in the central Arctic Ocean. We use a k-means cluster analysis, FLEXPART simulations, and inverse modeling to evaluate seasonal patterns and the influence of different source regions on the Arctic aerosol population. Furthermore, we compare the aerosol observations to land-based sites across the Arctic, using both long-term measurements and observations during the year of the MOSAiC expedition (2019-2020), to investigate interannual variability and to give context to the aerosol characteristics from within the central Arctic. Our analysis identifies that, overall, the central Arctic exhibits typical seasonal patterns of aerosols, including anthropogenic influence from Arctic haze in winter and secondary aerosol processes in summer. The seasonal pattern corresponds to the global radiation, surface air temperature, and timing of sea ice melting/freezing, which drive changes in transport patterns and secondary aerosol processes. In winter, the Norilsk region in Russia/Siberia was the dominant source of Arctic haze signals in the PNSD and BC observations, which contributed to higher accumulation-mode PNC and BC mass concentrations in the central Arctic than at land-based observatories. We also show that the wintertime Arctic Oscillation (AO) phenomenon, which was reported to achieve a record-breaking positive phase during January-March 2020, explains the unusual timing and magnitude of Arctic haze across the Arctic region compared to longer-term observations. In summer, the aerosol PNCs of the nucleation and Aitken modes are enhanced; however, concentrations were notably lower in the central Arctic over the ice pack than at land-based sites further south. The analysis presented herein provides a current snapshot of Arctic aerosol processes in an environment that is characterized by rapid changes, which will be crucial for improving climate model predictions, understanding linkages between different environmental processes, and investigating the impacts of climate change in future Arctic aerosol studies.