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The present work is a first approach to the study of the spatio-temporal variability of the submicrometer atmospheric aerosol in Spain. The aerosol measurements have been obtained simultaneously at seven monitoring stations that compose the REDMAAS network during two measurement campaigns corresponding to summer and winter seasons. In both summer and winter periods those measurement stations with a direct influence of anthropogenic emissions recorded the highest concentrations of particle number. In the summer campaign, the average daily pattern of the aerosol size distribution in the traffic and background urban stations was conditioned by the traffic emissions and secondary aerosol formation through photochemical reactions (new particle formation events, NPF). However, the secondary aerosol had a higher contribution to the aerosol total number concentration in the rural background and high-altitude stations. In the winter campaign, in all sampling sites with the exception of Izaña station, the traffic and domestic activity emissions had a greater contribution than secondary aerosol formation on particle number total concentration. New particle formation events were identified at all sites during the summer period, and at sites without direct influence of anthropogenic emissions during the winter campaign. Some aerosol shrinkage processes were also observed at the Madrid and El Arenosillo stations. ; This work has been financed by the Ministry of Science and Innovation (CGL2011-15008-E, CGL2010-1777, CGL2011-27020, CGL2014-52877-R & CGL2014-55230-R), Xunta de Galicia (GRC2013-047 potentially cofounded by ERDF) and the European Union Seventh Framework Programme (FP7/2007–2013) ACTRIS under grant agreement no. 262254.

The vertical profile of new particle formation (NPF) events was studied by comparing the aerosol size number distributions measured aloft and at surface level in a suburban environment in Madrid, Spain, using airborne instruments. The horizontal distribution and regional impact of the NPF events was investigated with data from three urban, urban background, and suburban stations in the Madrid metropolitan area. Intensive regional NPF episodes followed by particle growth were simultaneously recorded at three stations in and around Madrid during a field campaign in July 2016. The urban stations presented larger formation rates compared to the suburban station. Condensation and coagulation sinks followed a similar evolution at all stations, with higher values at urban stations. However, the total number concentration of particles larger than 2.5 nm was lower at the urban station and peaked around noon, when black carbon (BC) levels are at a minimum. The vertical soundings demonstrated that ultrafine particles (UFPs) are formed exclusively inside the mixed layer. As convection becomes more effective and the mixed layer grows, UFPs are detected at higher levels. The morning soundings revealed the presence of a residual layer in the upper levels in which aged particles (nucleated and grown on previous days) prevail. The particles in this layer also grow in size, with growth rates significantly smaller than those inside the mixed layer. Under conditions with strong enough convection, the soundings revealed homogeneous number size distributions and growth rates at all altitudes, which follow the same evolution at the other stations considered in this study. This indicates that UFPs are detected quasi-homogenously in an area spanning at least 17 km horizontally. The NPF events extend over the full vertical extension of the mixed layer, which can reach as high as 3000 m in the area, according to previous studies. On some days a marked decline in particle size (shrinkage) was observed in the afternoon, associated with a change in air masses. Additionally, a few nocturnal nucleation-mode bursts were observed at the urban stations, for which further research is needed to elucidate their origin. © Author(s) 2018. ; This work was supported by the Spanish Ministry of Agriculture, Fishing, Food and Environment; the Ministry of Economy, Industry and Competitiveness; the Madrid City Council and Regional Government; FEDER funds under the project HOUSE (CGL2016-78594-R); the CUD of Zaragoza (project CUD 2016-05); the Government of Catalonia (AGAUR 2017 SGR44); and the Korean Ministry of Environment through "The Eco-Innovation project". The funding received by ERA-PLANET (http://www.era-planet.eu, last access: 16 November 2018), the trans-national project SMURBS (http://www.smurbs.eu, last access: 16 November 2018) (Grant agreement No. 689443), and the support of the Academy of Finland via the Center of Excellence in Atmospheric Sciences are acknowledged. These results are part of a project (ATM-GTP/ERC) that has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (Grant agreement No. 742206). The authors also acknowledge the Doctoral program of Atmospheric Sciences at the University of Helsinki (ATM-DP). Markku Kulmala acknowledges the support of the Academy of Finland via his Academy Professorship (no. 302958). We also thank the City Council of Majadahonda for logistic assistance, and the Instituto de Ciencias Agrarias, Instituto de Salud Carlos III, Alava Ingenieros, TSI, Solma Environmental Solutions, and Airmodus for their support. ; Peer reviewed

Aerosol particles are a complex component of the atmospheric system which influence climate directly by interacting with solar radiation, and indirectly by contributing to cloud formation. The variety of their sources, as well as the multiple transformations they may undergo during their transport (including wet and dry deposition), result in significant spatial and temporal variability of their properties. Documenting this variability is essential to provide a proper representation of aerosols and cloud condensation nuclei (CCN) in climate models. Using measurements conducted in 2016 or 2017 at 62 ground-based stations around the world, this study provides the most up-to-date picture of the spatial distribution of particle number concentration (Ntot) and number size distribution (PNSD, from 39 sites). A sensitivity study was first performed to assess the impact of data availability on Ntot's annual and seasonal statistics, as well as on the analysis of its diel cycle. Thresholds of 50g% and 60g% were set at the seasonal and annual scale, respectively, for the study of the corresponding statistics, and a slightly higher coverage (75g%) was required to document the diel cycle. Although some observations are common to a majority of sites, the variety of environments characterizing these stations made it possible to highlight contrasting findings, which, among other factors, seem to be significantly related to the level of anthropogenic influence. The concentrations measured at polar sites are the lowest (g1/4g102gcm-3) and show a clear seasonality, which is also visible in the shape of the PNSD, while diel cycles are in general less evident, due notably to the absence of a regular day-night cycle in some seasons. In contrast, the concentrations characteristic of urban environments are the highest (g1/4g103-104gcm-3) and do not show pronounced seasonal variations, whereas diel cycles tend to be very regular over the year at these stations. The remaining sites, including mountain and non-urban continental and coastal stations, do not exhibit as obvious common behaviour as polar and urban sites and display, on average, intermediate Ntot (g1/4g102-103gcm-3). Particle concentrations measured at mountain sites, however, are generally lower compared to nearby lowland sites, and tend to exhibit somewhat more pronounced seasonal variations as a likely result of the strong impact of the atmospheric boundary layer (ABL) influence in connection with the topography of the sites. ABL dynamics also likely contribute to the diel cycle of Ntot observed at these stations. Based on available PNSD measurements, CCN-sized particles (considered here as either >50gnm or >100gnm) can represent from a few percent to almost all of Ntot, corresponding to seasonal medians on the order of g1/4g10 to 1000gcm-3, with seasonal patterns and a hierarchy of the site types broadly similar to those observed for Ntot. Overall, this work illustrates the importance of in situ measurements, in particular for the study of aerosol physical properties, and thus strongly supports the development of a broad global network of near surface observatories to increase and homogenize the spatial coverage of the measurements, and guarantee as well data availability and quality. The results of this study also provide a valuable, freely available and easy to use support for model comparison and validation, with the ultimate goal of contributing to improvement of the representation of aerosol-cloud interactions in models, and, therefore, of the evaluation of the impact of aerosol particles on climate. ; NOAA base funding supports the observatories BRW, BND, MLO, SMO, SPO and THD, where efforts of the dedicated observatory staff and of programmer Derek Hageman are appreciated. BRW observations are also supported in part by the Atmospheric Radiation Measurement (ARM) user facility, a US Department of Energy (DOE) Office of Science user facility managed by the Biological and Environmental Research programme. Measurements at Welgegund are supported by North-West University, the University of Helsinki and the Finnish Meteorological Institute. This publication also forms part of the output of the Biogeochemistry Research Infrastructure Platform (BIOGRIP) of the Department of Science and Innovation of South Africa. Pallas and SMEAR II are grateful for the support of the Academy of Finland Centre of Excellence programme (project no. 272041), the Academy of Finland project Greenhouse gas, aerosol and albedo variations in the changing Arctic (project no. 269095), and the Novel Assessment of Black Carbon in the Eurasian Arctic: From Historical Concentrations and Sources to Future Climate Impacts (NABCEA, project no. 296302). Aerosol measurements at Anmyeon-do were supported by the Korea Meteorological Administration Research and Development Program "Development of Monitoring and Analysis Techniques for Atmospheric Composition in Korea" under grant KMA2018-00522. Measurements at Gosan were supported by the National Research Foundation of Korea (2017R1D1A1B06032548) and the Korea Meteorological Administration Research and Development Program under grant KMI2018-01111. The Lulin station is operated under the grants funded by the Taiwan Environmental Protection Administration. WLG is supported by the China Meteorological Administration, where efforts of the dedicated observatory staff are appreciated. Sites PDM, PUY, GIF, CHC and RUN are partially operated with the support of CNRS-INSU under the long-term observation programme and the French Ministry for Research under the ACTRIS-FR national research infrastructure. PDM and GIF received specific support from the French Ministry of the Environment. ATMO Occitanie is mentioned for sampling operations at PDM. Measurements at SIRTA are hosted by CNRS and by the alternative energies and atomic energy commission (CEA) with additional contributions from the French Ministry of the Environment through its funding to the reference laboratory for air quality monitoring (LCSQA). PUY is grateful for support from ATMO Auvergne Rhône Alpes for sampling operations and the support from the personnel of the Observatoire de Physique du Globe de Clermont-Ferrand (OPGC). The specific support of the Institut de Recherche et Développement (IRD) in France and the Universidad Mayor de San Andrés in Bolivia support operations at CHC operations. The Steamboat Ski Resort provided logistical support and in-kind donations for SPL. The Desert Research Institute is a permittee of the Medicine Bow–Routt National Forests and an equal opportunity service provider and employer. SPL appreciates the extensive assistance of the NOAA/ESRL Federated Aerosol Network, of Ian McCubbin, site manager of SPL, and of Ty Atkins, Joe Messina, Dan Gilchrist and Maria Garcia, who provided technical assistance with the maintenance and data quality control for the aerosol instruments. SGP measurements/mentorship were supported by DOE-7F-30118 and staff on site. The Cape Grim Baseline Air Pollution Monitoring Station is grateful to the Australian Bureau of Meteorology for their long-term and continued support and all the staff from the Bureau of Meteorology and CSIRO, who have contributed to the generation of records reported here. The aerosol measurements at the Jungfraujoch were conducted with financial support from MeteoSwiss (GAW-CH aerosol monitoring programme) and from the European Union as well as the Swiss State Secretariat for Education, Research and Innovation (SERI) for the European Research Infrastructure for the observation of Aerosol, Clouds and Trace Gases (ACTRIS). The International Foundation High Altitude Research Station Jungfraujoch and Gornergrat (HFSJG) is mentioned for providing the research platform at the Jungfraujoch. The aerosol measurements at Kosetice received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement no. 654109 and from the project for support of the national research infrastructure ACTRIS – participation of the Czech Republic (ACTRIS-CZ – LM2015037) supported by the Ministry of Education, Youth and Sports of CR within National Sustainability Program I (NPU I), grant agreement no. LO1415. The measurements were also supported by ERDF "ACTRIS-CZ RI" (no. CZ.02.1.01/0.0/0.0/16_013/0001315). Measurements at the Madrid site were funded by the following projects: CRISOL (CGL2017–85344-R MINECO/AEI/FEDER, UE), TIGAS-CM (Madrid Regional Government Y2018/EMT5177), AIRTEC-CM (Madrid Regional Government P2018/EMT4329), REDMAAS2020 (RED2018-102594-T CIENCIA) and Red de Excelencia ACTRIS-ESPAÑA (CGL2017-90884-REDT). Measurements at Montsec and Montseny were supported by the Spanish Ministry of Economy, Industry and Competitiveness and FEDER funds under project HOUSE (CGL2016-78594-R) and by the Generalitat de Catalunya (AGAUR 2017 SGR41 and the DGQA). Aerosol measurements at El Arenosillo Observatory are supported by the National Institute for Aerospace Technology and by different R&D projects of the Ministerio Español de Economía, Industria y Competitividad (MINECO). Aerosol measurements at UGR are supported by the Spanish Ministry of Economy and Competitiveness through projects no. CGL2016-81092-R, CGL2017-90884-REDT, RTI2018-097864-B-I00 and PGC2018-098770-B-I00 and by the Andalusia Regional Government through project no. P18-RT-3820. FKL, HAC and DEM are grateful for funding by project PANhellenic infrastructure for Atmospheric Composition and climate change (MIS 5021516), which is implemented under action Reinforcement of the Research and Innovation Infrastructure, funded by operational programme Competitiveness, Entrepreneurship and Innovation (NSRF 2014-2020) and co-financed by Greece and the European Union (European Regional Development Fund). CPC measurements at Sonnblick are supported by the Climate and Air Quality Commission of the Austrian Academy of Sciences and the office of the provincial government Salzburg, Unit 5/02. At CMN, aerosol measurements were partially supported by the Italian Ministry of Research and Education. Measurements at Birkenes II are financed by the Norwegian Environment Agency. VAV is grateful for various Swedish FORMAS, Swedish Research Council (VR) grants and the Magnus Bergvall and Märta och Erik Holmberg foundations and the Swedish EPA for making the research possible at the VAV site. NMY wishes to thank the many technicians and scientists of the Neumayer overwintering crews, whose outstanding commitment enabled continuous, high-quality aerosol records over many years. Gunter Löschau is acknowledged for his contribution to the data acquisition at ANB, DTC and DRN. Financial support This research was supported by the European Commission's Horizon 2020 Framework Programme (ACTRIS2 (grant agreement no. 654109)), the University of Helsinki, the Finnish Meteorological Institute, the Department of Science and Innovation of South Africa, the Academy of Finland Centre of Excellence programme (project no. 272041), the Academy of Finland project Greenhouse gas, aerosol and albedo variations in the changing Arctic (project no. 269095), the Novel Assessment of Black Carbon in the Eurasian Arctic: From Historical Concentrations and Sources to Future Climate Impacts (NABCEA, project no. 296302), the Korea Meteorological Administration Research and Development Program "Development of Monitoring and Analysis Techniques for Atmospheric Composition in Korea" (grant no. KMA2018-00522), the National Research Foundation of Korea (grant no. 2017R1D1A1B06032548), the Korea Meteorological Administration Research and Development Program (grant no. KMI2018-01111), the Taiwan Environmental Protection Administration, the China Meteorological Administration, the National Scientific Foundation of China (41675129, 41875147), the National Key R&D Program of the Ministry of Science and Technology of the People's Republic of China (grant no. 2016YFC0203305 and 2018YFC0213204), the Chinese Academy of Meteorological Sciences (2020KJ001), the Innovation Team for Haze-fog Observation and Forecasts of MOST and CMA, CNRS-INSU, the French Ministry for Research under the ACTRIS-FR national research infrastructure, the French Ministry of the Environment, MeteoSwiss (GAW-CH aerosol monitoring programme), the Swiss State Secretariat for Education, Research and Innovation (SERI), the Ministry of Education, Youth and Sports of CR within National Sustainability Program I (NPU I, grant no. LO1415), ERDF "ACTRISCZ RI" (grant no. CZ.02.1.01/0.0/0.0/16_013/0001315), CRISOL (CGL2017-85344-R MINECO/AEI/FEDER, UE), TIGAS-CM (Madrid Regional Government Y2018/EMT-5177), AIRTEC-CM (Madrid Regional Government P2018/EMT4329), REDMAAS2020 (RED2018-102594-T CIENCIA), Red de Excelencia ACTRIS-ESPAÑA (CGL2017-90884-REDT), the Spanish Ministry of Economy, Industry and Competitiveness, FEDER funds (project HOUSE, grant no. CGL2016-78594-R), the Generalitat de Catalunya (AGAUR 2017 SGR41 and the DGQA), the National Institute for Aerospace Technology, the Ministerio Español de Economía, Industria y Competitividad (MINECO), the Spanish Ministry of Economy and Competitiveness (projects no. CGL2016-81092-R, CGL2017-90884-REDT, RTI2018-097864-B-I00 and PGC2018-098770-B-I00), the Andalusia Regional Government (project no. P18-RT-3820), the PANhellenic infrastructure for Atmospheric Composition and climate change (MIS 5021516), Research and Innovation Infrastructure, Competitiveness, Entrepreneurship and Innovation (grant no. NSRF 2014-2020), the Italian Ministry of Research and Education, the Norwegian Environment Agency, Swedish FORMAS, the Swedish Research Council (VR), the Magnus Bergvall foundation, the Märta och Erik Holmberg foundation, and the Swedish EPA. ; Peer reviewed