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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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    Changes in black carbon emissions over Europe due to COVID-19 lockdowns
    (Katlenburg-Lindau : European Geosciences Union, 2021) Evangeliou, Nikolaos; Platt, Stephen M.; Eckhardt, Sabine; Lund Myhre, Cathrine; Laj, Paolo; Alados-Arboledas, Lucas; Backman, John; Brem, Benjamin T.; Fiebig, Markus; Flentje, Harald; Marinoni, Angela; Pandolfi, Marco; Yus-Dìez, Jesus; Prats, Natalia; Putaud, Jean P.; Sellegri, Karine; Sorribas, Mar; Eleftheriadis, Konstantinos; Vratolis, Stergios; Wiedensohler, Alfred; Stohl, Andreas
    Following the emergence of the severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) responsible for COVID-19 in December 2019 in Wuhan (China) and its spread to the rest of the world, the World Health Organization declared a global pandemic in March 2020. Without effective treatment in the initial pandemic phase, social distancing and mandatory quarantines were introduced as the only available preventative measure. In contrast to the detrimental societal impacts, air quality improved in all countries in which strict lockdowns were applied, due to lower pollutant emissions. Here we investigate the effects of the COVID-19 lockdowns in Europe on ambient black carbon (BC), which affects climate and damages health, using in situ observations from 17 European stations in a Bayesian inversion framework. BC emissions declined by 23 kt in Europe (20 % in Italy, 40 % in Germany, 34 % in Spain, 22 % in France) during lockdowns compared to the same period in the previous 5 years, which is partially attributed to COVID-19 measures. BC temporal variation in the countries enduring the most drastic restrictions showed the most distinct lockdown impacts. Increased particle light absorption in the beginning of the lockdown, confirmed by assimilated satellite and remote sensing data, suggests residential combustion was the dominant BC source. Accordingly, in central and Eastern Europe, which experienced lower than average temperatures, BC was elevated compared to the previous 5 years. Nevertheless, an average decrease of 11 % was seen for the whole of Europe compared to the start of the lockdown period, with the highest peaks in France (42 %), Germany (21 %), UK (13 %), Spain (11 %) and Italy (8 %). Such a decrease was not seen in the previous years, which also confirms the impact of COVID-19 on the European emissions of BC.
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    Long-range and local air pollution: What can we learn from chemical speciation of particulate matter at paired sites?
    (Katlenburg-Lindau : EGU, 2020) Pandolfi, Marco; Mooibroek, Dennis; Hopke, Philip; van Pinxteren, Dominik; Querol, Xavier; Herrmann, Hartmut; Alastuey, Andrés; Favez, Olivier; Hüglin, Christoph; Perdrix, Esperanza; Riffault, Véronique; Sauvage, Stéphane; van der Swaluw, Eric; Tarasova, Oksana; Colette, Augustin
    Here we report results of a detailed analysis of the urban and non-urban contributions to particulate matter (PM) concentrations and source contributions in five European cities, namely Schiedam (the Netherlands, NL), Lens (France, FR), Leipzig (Germany, DE), Zurich (Switzerland, CH) and Barcelona (Spain, ES). PM chemically speciated data from 12 European paired monitoring sites (one traffic, five urban, five regional and one continental background) were analysed by positive matrix factorisation (PMF) and Lenschow's approach to assign measured PM and source contributions to the different spatial levels. Five common sources were obtained at the 12 sites: sulfate-rich (SSA) and nitrate-rich (NSA) aerosols, road traffic (RT), mineral matter (MM), and aged sea salt (SS). These sources explained from 55 % to 88 % of PM mass at urban low-traffic-impact sites (UB) depending on the country. Three additional common sources were identified at a subset of sites/countries, namely biomass burning (BB) (FR, CH and DE), explaining an additional 9 %-13 % of PM mass, and residual oil combustion (V-Ni) and primary industrial (IND) (NL and ES), together explaining an additional 11 %-15 % of PM mass. In all countries, the majority of PM measured at UB sites was of a regional+continental (R+C) nature (64 %-74 %). The R+C PM increments due to anthropogenic emissions in DE, NL, CH, ES and FR represented around 66 %, 62 %, 52 %, 32 % and 23 %, respectively, of UB PM mass. Overall, the R+C PM increments due to natural and anthropogenic sources showed opposite seasonal profiles with the former increasing in summer and the latter increasing in winter, even if exceptions were observed. In ES, the anthropogenic R+C PM increment was higher in summer due to high contributions from regional SSA and V-Ni sources, both being mostly related to maritime shipping emissions at the Spanish sites. Conversely, in the other countries, higher anthropogenic R+C PM increments in winter were mostly due to high contributions from NSA and BB regional sources during the cold season. On annual average, the sources showing higher R+C increments were SSA (77 %-91 % of SSA source contribution at the urban level), NSA (51 %-94 %), MM (58 %-80 %), BB (42 %-78 %) and IND (91 % in NL). Other sources showing high R+C increments were photochemistry and coal combustion (97 %-99 %; identified only in DE). The highest regional SSA increment was observed in ES, especially in summer, and was related to ship emissions, enhanced photochemistry and peculiar meteorological patterns of the Western Mediterranean. The highest R+C and urban NSA increments were observed in NL and associated with high availability of precursors such as NOx and NH3. Conversely, on average, the sources showing higher local increments were RT (62 %-90 % at all sites) and V-Ni (65 %-80 % in ES and NL). The relationship between SSA and V-Ni indicated that the contribution of ship emissions to the local sulfate concentrations in NL has strongly decreased since 2007 thanks to the shift from high-sulfur-to low-sulfur-content fuel used by ships. An improvement of air quality in the five cities included here could be achieved by further reducing local (urban) emissions of PM, NOx and NH3 (from both traffic and non-traffic sources) but also SO2 and PM (from maritime ships and ports) and giving high relevance to non-urban contributions by further reducing emissions of SO2 (maritime shipping) and NH3 (agriculture) and those from industry, regional BB sources and coal combustion. © 2020 Copernicus GmbH. All rights reserved.
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    Biomass burning and urban emission impacts in the Andes Cordillera region based on in situ measurements from the Chacaltaya observatory, Bolivia (5240a.s.l.)
    (Katlenburg-Lindau : EGU, 2019) Chauvigné, Aurélien; Aliaga, Diego; Sellegri, Karine; Montoux, Nadège; Krejci, Radovan; Močnik, Griša; Moreno, Isabel; Müller, Thomas; Pandolfi, Marco; Velarde, Fernando; Weinhold, Kay; Ginot, Patrick; Wiedensohler, Alfred; Andrade, Marcos; Laj, Paolo
    This study documents and analyses a 4-year continuous record of aerosol optical properties measured at the Global Atmosphere Watch (GAW) station of Chacaltaya (CHC; 5240a.s.l.), in Bolivia. Records of particle light scattering and particle light absorption coefficients are used to investigate how the high Andean Cordillera is affected by both long-range transport and by the fast-growing agglomeration of La Paz-El Alto, located approximately 20km away and 1.5km below the sampling site. The extended multi-year record allows us to study the properties of aerosol particles for different air mass types, during wet and dry seasons, also covering periods when the site was affected by biomass burning in the Bolivian lowlands and the Amazon Basin. The absorption, scattering, and extinction coefficients (median annual values of 0.74, 12.14, and 12.96Mm-1 respectively) show a clear seasonal variation with low values during the wet season (0.57, 7.94, and 8.68Mm-1 respectively) and higher values during the dry season (0.80, 11.23, and 14.51Mm-1 respectively). The record is driven by variability at both seasonal and diurnal scales. At a diurnal scale, all records of intensive and extensive aerosol properties show a pronounced variation (daytime maximum, night-time minimum), as a result of the dynamic and convective effects. The particle light absorption, scattering, and extinction coefficients are on average 1.94, 1.49, and 1.55 times higher respectively in the turbulent thermally driven conditions than the more stable conditions, due to more efficient transport from the boundary layer. Retrieved intensive optical properties are significantly different from one season to the other, reflecting the changing aerosol emission sources of aerosol at a larger scale. Using the wavelength dependence of aerosol particle optical properties, we discriminated between contributions from natural (mainly mineral dust) and anthropogenic (mainly biomass burning and urban transport or industries) emissions according to seasons and local circulation. The main sources influencing measurements at CHC are from the urban area of La Paz-El Alto in the Altiplano and from regional biomass burning in the Amazon Basin. Results show a 28% to 80% increase in the extinction coefficients during the biomass burning season with respect to the dry season, which is observed in both tropospheric dynamic conditions. From this analysis, long-term observations at CHC provide the first direct evidence of the impact of biomass burning emissions of the Amazon Basin and urban emissions from the La Paz area on atmospheric optical properties at a remote site all the way to the free troposphere. © Author(s) 2019.
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    Multidecadal trend analysis of in situ aerosol radiative properties around the world
    (Katlenburg-Lindau : EGU, 2020) Collaud Coen, Martine; Andrews, Elisabeth; Alastuey, Andrés; Petkov Arsov, Todor; Backman, John; Brem, Benjamin T.; Bukowiecki, Nicolas; Couret, Cédric; Eleftheriadis, Konstantinos; Flentje, Harald; Fiebig, Markus; Gysel-Beer, Martin; Hand, Jenny L.; Hoffer, András; Hooda, Rakesh; Hueglin, Christoph; Joubert, Warren; Keywood, Melita; Eun Kim, Jeong; Kim, Sang-Woo; Labuschagne, Casper; Lin, Neng-Huei; Lin, Yong; Lund Myhre, Cathrine; Luoma, Krista; Lyamani, Hassan; Marinoni, Angela; Mayol-Bracero, Olga L.; Mihalopoulos, Nikos; Pandolfi, Marco; Prats, Natalia; Prenni, Anthony J.; Putaud, Jean-Philippe; Ries, Ludwig; Reisen, Fabienne; Sellegri, Karine; Sharma, Sangeeta; Sheridan, Patrick; Sherman, James Patrick; Sun, Junying; Titos, Gloria; Torres, Elvis; Tuch, Thomas; Weller, Rolf; Wiedensohler, Alfred; Zieger, Paul; Laj, Paolo
    In order to assess the evolution of aerosol parameters affecting climate change, a long-term trend analysis of aerosol optical properties was performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Ångström exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann-Kendall (MK) statistical test associated with several pre-whitening methods and with Sen's slope was used as the main trend analysis method. Comparisons with general least mean square associated with autoregressive bootstrap (GLS/ARB) and with standard least mean square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficient trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficient time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, eastern/northern Europe and the Arctic, 22 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 26 % of sites have trends which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10-year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10-year trends are primarily found for earlier periods (10-year trends ending in 2010-2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10-year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10-year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10-year trends of the scattering coefficient - there is a shift to statistically significant negative trends in 2009-2012 for all stations in the eastern and central USA. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage provides insight into potential aerosol effects on climate changes. © 2020 Royal Society of Chemistry. All rights reserved.
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    A European aerosol phenomenology - 6: Scattering properties of atmospheric aerosol particles from 28 ACTRIS sites
    (Katlenburg-Lindau : EGU, 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, Nikos; Moerman, Marcel; Nicolas, José; O'Dowd, Colin; 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, Paolo
    This 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 intraannual 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.
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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.