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Cloud condensation nuclei counter (CCNC) measurements performed at 14 locations around the world within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) framework have been analysed and discussed with respect to the cloud condensation nuclei (CCN) activation and hygroscopic properties of the atmospheric aerosol. The annual mean ratio of activated cloud condensation nuclei (NCCN) to the total number concentration of particles (NCN), known as the activated fraction A, shows a similar functional dependence on supersaturation S at many locations - exceptions to this being certain marine locations, a free troposphere site and background sites in south-west Germany and northern Finland. The use of total number concentration of particles above 50 and 100 nm diameter when calculating the activated fractions (A50 and A100, respectively) renders a much more stable dependence of A on S; A50 and A100 also reveal the effect of the size distribution on CCN activation. With respect to chemical composition, it was found that the hygroscopicity of aerosol particles as a function of size differs among locations. The hygroscopicity parameter κ decreased with an increasing size at a continental site in south-west Germany and fluctuated without any particular size dependence across the observed size range in the remote tropical North Atlantic and rural central Hungary. At all other locations κ increased with size. In fact, in Hyytiälä, Vavihill, Jungfraujoch and Pallas the difference in hygroscopicity between Aitken and accumulation mode aerosol was statistically significant at the 5% significance level. In a boreal environment the assumption of a size-independent κ can lead to a potentially substantial overestimation of NCCN at S levels above 0.6 %. The same is true for other locations where κ was found to increase with size. While detailed information about aerosol hygroscopicity can significantly improve the prediction of NCCN, total aerosol number concentration and aerosol size distribution remain more important parameters. The seasonal and diurnal patterns of CCN activation and hygroscopic properties vary among three long-term locations, highlighting the spatial and temporal variability of potential aerosol-cloud interactions in various environments. [ABSTRACT FROM AUTHOR]

[Display omitted] • Source apportionment of organic aerosol in 22 year-long datasets in Europe; • Harmonised source apportionment protocol; • Oxygenated organic aerosol dominates across Europe in all seasons; • Solid-fuel combustion is a significant source in most European sites, especially in winter; • Traffic source is present in both urban and non-urban sites with constant and non-negligible contributions. Organic aerosol (OA) is a key component of total submicron particulate matter (PM 1), and comprehensive knowledge of OA sources across Europe is crucial to mitigate PM 1 levels. Europe has a well-established air quality research infrastructure from which yearlong datasets using 21 aerosol chemical speciation monitors (ACSMs) and 1 aerosol mass spectrometer (AMS) were gathered during 2013–2019. It includes 9 non-urban and 13 urban sites. This study developed a state-of-the-art source apportionment protocol to analyse long-term OA mass spectrum data by applying the most advanced source apportionment strategies (i.e., rolling PMF, ME-2, and bootstrap). This harmonised protocol was followed strictly for all 22 datasets, making the source apportionment results more comparable. In addition, it enables quantification of the most common OA components such as hydrocarbon-like OA (HOA), biomass burning OA (BBOA), cooking-like OA (COA), more oxidised-oxygenated OA (MO-OOA), and less oxidised-oxygenated OA (LO-OOA). Other components such as coal combustion OA (CCOA), solid fuel OA (SFOA: mainly mixture of coal and peat combustion), cigarette smoke OA (CSOA), sea salt (mostly inorganic but part of the OA mass spectrum), coffee OA, and ship industry OA could also be separated at a few specific sites. Oxygenated OA (OOA) components make up most of the submicron OA mass (average = 71.1%, range from 43.7 to 100%). Solid fuel combustion-related OA components (i.e., BBOA, CCOA, and SFOA) are still considerable with in total 16.0% yearly contribution to the OA, yet mainly during winter months (21.4%). Overall, this comprehensive protocol works effectively across all sites governed by different sources and generates robust and consistent source apportionment results. Our work presents a comprehensive overview of OA sources in Europe with a unique combination of high time resolution (30–240 min) and long-term data coverage (9–36 months), providing essential information to improve/validate air quality, health impact, and climate models. [ABSTRACT FROM AUTHOR]

Biomass burning is a major source of Brown Carbon (BrC), strongly contributing to radiative forcing. In urban areas of the climate-sensitive Southeastern European region, where strong emissions from residential wood burning (RWB) are reported, radiative impacts of carbonaceous aerosols remain largely unknown. This study examines the absorption properties of water- and methanol-soluble organic carbon (WSOC, MeS_OC) in a city (Ioannina, Greece) heavily impacted by RWB. Measurements were performed during winter (December 2019 - February 2020) and summer (July - August 2019) periods, characterized by RWB and photochemical processing of organic aerosol (OA), respectively. PM 2.5 filter extracts were analyzed spectrophotometrically for water- and methanol-soluble BrC (WS_BrC, MeS_BrC) absorption. WSOC concentrations were quantified using TOC analysis, while those of MeS_OC were determined using a newly developed direct quantification protocol, applied for the first time to an extended series of ambient samples. The direct method led to a mean MeS_OC/OC of 0.68 and a more accurate subsequent estimation of absorption efficiencies. The mean winter WS_BrC and MeS_BrC absorptions at 365 nm were 13.9 Mm -1 and 21.9 Mm -1 , respectively, suggesting an important fraction of water-insoluble OA. Mean winter WS_BrC and MeS_BrC absorptions were over 10 times those observed in summer. MeS_OC was more absorptive than WSOC in winter (mean mass absorption efficiencies - MAE 365 : 1.81 vs 1.15 m 2 gC -1 ) and especially in summer (MAE: 1.12 vs 0.27 m 2 gC -1 ) due to photo-dissociation and volatilization of BrC chromophores. The winter radiative forcing (RF) of WS_BrC and MeS_BrC relative to elemental carbon (EC) was estimated at 8.7 % and 16.7 %, respectively, in the 300-2500 nm band. However, those values increased to 48.5 % and 60.2 % at 300-400 nm, indicating that, under intense RWB, BrC forcing becomes comparable to that of soot. The results highlight the consideration of urban BrC emissions in radiative transfer models, as a considerable climate forcing factor., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)