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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. ; This research was supported by the European Commission's Horizon 2020 Framework Programme (ACTRIS-2 (grant agreement no. 654109)); AEMET; European ERDF funds through different Spanish R&D projects of the Spanish Ministerio de Economía, Industria y Competitividad; the North-West University; the University of Helsinki; the Finnish Meteorological Institute; 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; CNRS-INSU; French Ministry for Research under the ACTRIS-FR national research infrastructure; French Ministry of the Environment; US Environmental Protection Agency; MeteoSwiss (GAW-CH aerosol monitoring programme); the Swiss State Secretariat for Education, Research and Innovation (SERI); Ministry of Education, Youth and Sports of CR within National Sustainability Program I (NPU I, grant no. LO1415); ERDF "ACTRIS-CZ 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); 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); NOAA/ESRL/GMD; 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; Swedish Research Council (VR); the Magnus Bergvall foundation; the Märta och Erik Holmberg foundation; and the Swedish EPA.

Although particulate organic and elemental carbon (OC and EC) are important constituents of the suspended atmospheric particulate matter (PM), measurements of OC and EC are much less common and more uncertain than measurements of e.g. the ionic components of PM. In the framework of atmospheric research infrastructures supported by the European Union, actions have been undertaken to determine and mitigate sampling artefacts, and assess the comparability of OC and EC data obtained in a network of 10 atmospheric observatories across Europe. Positive sampling artefacts (from 0.4 to 2.8 μg C/m3) and analytical discrepancies (between −50% and +40% for the EC/TC ratio) have been taken into account to generate a robust data set, from which we established the phenomenology of carbonaceous aerosols at regional background sites in Europe. Across the network, TC and EC annual average concentrations range from 0.4 to 9 μg C/m3, and from 0.1 to 2 μg C/m3, respectively. TC/PM10 annual mean ratios range from 0.11 at a Mediterranean site to 0.34 at the most polluted continental site, and TC/PM2.5 ratios are slightly greater at all sites (0.15–0.42). EC/TC annual mean ratios range from 0.10 to 0.22, and do not depend much on PM concentration levels, especially in winter. Seasonal variations in PM and TC concentrations, and in TC/PM and EC/TC ratios, differ across the network, which can be explained by seasonal changes in PM source contributions at some sites. © 2016 The Authors ; EUSAAR (FP6/2001-2006, grant agreement no. RII3-GT-2006-026140), ACTRIS (FP7/2007-2013, grant agreement no. 262254), ACTRIS2 (H2020-INFRAIA-2014-2015, grant agreement no. 654109), EPA Ireland is acknowledged for the research support at Mace Head, the Norwegian Environment Agency for the measurements at Birkenes. Appendix A ; Peer reviewed

Further research is needed to reduce the existing uncertainties on the effect that specific aerosol particle sources have on light extinction and consequently on climate. This study presents a new approach that aims to quantify the mass scattering and absorption efficiencies (MSEs and MAEs) of different aerosol sources at urban (Barcelona - BCN), regional (Montseny - MSY) and remote (Montsec - MSA) background sites in the north-western (NW) Mediterranean. An analysis of source apportionment to the measured multi-wavelength light scattering (σsp) and absorption (σap) coefficients was performed by means of a multilinear regression (MLR) model for the periods 2009-2014, 2010-2014 and 2011-2014 at BCN, MSY and MSA respectively. The source contributions to PM10 mass concentration, identified by means of the positive matrix factorization (PMF) model, were used as dependent variables in the MLR model. With this approach we addressed both the effect that aerosol sources have on air quality and their potential effect on light extinction through the determination of their MSEs and MAEs. An advantage of the presented approach is that the calculated MSEs and MAEs take into account the internal mixing of atmospheric particles. Seven aerosol sources were identified at MSA and MSY, and eight sources at BCN. Mineral, aged marine, secondary sulfate, secondary nitrate and V-Ni bearing sources were common at the three sites. Traffic, industrial/metallurgy and road dust resuspension sources were isolated at BCN, whereas mixed industrial/traffic and aged organics sources were identified at MSY and MSA. The highest MSEs were observed for secondary sulfate (4.5 and 10.7 m2 g-1, at MSY and MSA), secondary nitrate (8.8 and 7.8 m2 g-1) and V-Ni bearing source (8 and 3.5 m2 g-1). These sources dominated the scattering throughout the year with marked seasonal trends. The V-Ni bearing source, originating mainly from shipping in the area under study, simultaneously contributed to both σsp and σap, being the second most efficient light-absorbing source in BCN (MAE = 0.9 m2 g-1). The traffic source at BCN and the industrial/traffic at MSY exhibited the highest MAEs (1.7 and 0.9 m2 g-1). These sources were major contributors to σap at BCN and MSY; however at MSA, secondary nitrate exerted the highest influence on σap (MAE = 0.4 m2 g-1). The sources which were predominantly composed of fine and relatively dark particles, such as industrial/traffic, aged organics and V-Ni, were simultaneously characterized by low single scattering albedo (SSA) and a high scattering Ångström exponent (SAE). Conversely, mineral and aged marine showed the lowest SAE and the highest SSA, being scattering the dominant process in the light extinction. The good agreement found between modelled and measured particle optical properties allowed the reconstruction of σsp and σap long-term series over the period 2004-2014 at MSY. Significant decreasing trends were found for the modelled σsp and σap (-4.6 and -4.1 % yr-1). © Author(s) 2018. ; Acknowledgements. This work was supported by the MINECO (Spanish Ministry of Economy and Competitiveness) and FEDER funds under the PRISMA project (CGL2012-39623-C02/00) by the MAGRAMA (Spanish Ministry of Agriculture, Food and Environment) and by the Generalitat de Catalunya (AGAUR 2014 SGR33 and the DGQA). This work has received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement no. 654109. Marco Pandolfi is funded by a Ramón y Cajal Fellowship (RYC-2013-14036) awarded by the MINECO. The authors would like to express their gratitude to Karl Ropkins and David C. Carslaw for providing the OpenAir software used in this paper (Carslaw and Ropkins, 2012; Carslaw, 2012). ; Peer reviewed

The study of Saharan dust events (SDEs) and biomass burning (BB) emissions are both topics of great scientific interest since they are frequent and important polluting scenarios affecting air quality and climate. The main aim of this work is evaluating the feasibility of using near-real-time in situ aerosol optical measurements for the detection of these atmospheric events in the western Mediterranean Basin (WMB). With this aim, intensive aerosol optical properties (SAE: scattering Ångström exponent, AAE: absorption Ångström exponent, SSAAE: single scattering albedo Ångström exponent and AAE: asymmetry parameter) were derived from multi-wavelength aerosol light scattering, hemispheric backscattering and absorption measurements performed at regional (Montseny; MSY, 720 m a.s.l.) and continental (Montsec; MSA, 1570 m a.s.l.) background sites in the WMB. A sensitivity study aiming at calibrating the measured intensive optical properties for SDEs and BB detection is presented and discussed. The detection of SDEs by means of the SSAAE parameter and Ångström matrix (made up by SAE and AAE) depended on the altitude of the measurement station and on SDE intensity. At MSA (mountain-top site) SSAAE detected around 85% of SDEs compared with 50% at the MSY station, where pollution episodes dominated by fine anthropogenic particles frequently masked the effect of mineral dust on optical properties during less intense SDEs. Furthermore, an interesting feature of SSAAE was its capability to detect the presence of mineral dust after the end of SDEs. Thus, resuspension processes driven by summer regional atmospheric circulations and dry conditions after SDEs favoured the accumulation of mineral dust at regional level having important consequences for air quality. On average, SAE, AAE and g ranged between-0.7 and 1, 1.3 and 2.5 and 0.5 and 0.75 respectively during SDEs. Based on the aethalometer model, BB contribution to equivalent black carbon (BC) accounted for 36 and 40 % at MSY and MSA respectively. Linear relationships were found between AAE and bb, with AAE values reaching around 1.5 when bb was higher than 50%. BB contribution to organic matter (OM) at MSY was around 30%. Thus fossil fuel (FF) combustion sources showed important contributions to both BC and OM in the region under study. Results for OM source apportionment showed good agreement with simultaneous biomass burning organic aerosol (BBOA) and hydrocarbon-like organic aerosol (HOA) obtained by applying a positive matrix factorization model (PMF) to simultaneous Aerosol Chemical Speciation Monitor (ACSM) measurements. A wildfire episode was identified at MSY, showing AAE values up to 2 when daily BB contributions to BC and OM were 73 and 78% respectively. © 2016 The Author(s). ; This work was supported by the MINECO (Spanish Ministry of Economy and Competitiveness), the MAGRAMA (Spanish Ministry of Agriculture, Food and Environment), the Generalitat de Catalunya (AGAUR 2014 SGR33 and the DGQA) and FEDER funds under the PRISMA project (CGL2012- 39623-C02/00). This work has received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement No 654109. Marco Pandolfi is funded by a Ramón y Cajal Fellowship (RYC-2013-14036) awarded by the Spanish Ministry of Economy and Competitiveness. The authors would like to express their gratitude to D. C. Carslaw and K. Ropkins for providing the OpenAir software used in this paper (Carslaw and Ropkins, 2012; Carslaw, 2012). ; Peer reviewed

An outstanding Saharan dust event affected the Iberian Peninsula during winter 2016 (20 to 25 February). The impact of this event on ambient PM10 surface levels and its spatial and temporal evolution was investigated by means of data from 250 air quality stations across mainland Spain and the Balearic Islands. The event had a significant impact on surface PM10 levels, and on 22 February, 90% of the air quality monitoring sites registered PM10 concentrations above the EU daily limit value of 50 µg/m3. The study of the attenuated backscattering vertical profiles associated with African dust evidenced a complex structure, with a thick aerosol layer that was at higher altitudes over the pre-Pyrenees compared to the coastal area of Barcelona but closer to the surface than typically observed at both sites. Optical and physical properties of dust particles were investigated at the continental background Global Atmosphere Watch mountain observatory of Montsec (MSA) in the pre-Pyrenees. Good agreement was found between in situ and passive remote sensing methodologies once the aloft dust layer reached the MSA station. Scattering Ångström exponent values decreased to values close to zero (even below zero for surface in situ measurements) indicating the predominance of coarse particles. On the contrary, absorption Ångström exponent values increased during the Saharan dust outbreak denoting an absorption enhancement at shorter wavelengths, characteristic of mineral dust particles. Furthermore, the performance of NMMB/BSC-Dust and BSC-DREAM8b models has been qualitatively evaluated for the dust spatial distribution across Spain and the vertical structure over MSA and Barcelona showing good agreement. © 2017. The Authors. ; This work was supported by the MINECO (Spanish Ministry of Economy and Competitiveness, and FEDER funds, under the PRISMA project (CGL2012- 39623-C02/00) and project TEC2015- 63832-P), the MAGRAMA (Spanish Ministry of Agriculture, Food and Environment), the Generalitat de Catalunya (AGAUR 2014 SGR33, and the Departament de Territori I Sostenibilitat). This work has received funding from the European Union's Horizon 2020 Research and Innovation Programme under grant agreement 654109 (ACTRIS-2). M. Pandolfi is funded by a Ramón y Cajal Fellowship (RYC-2013-14036) awarded by the Spanish Ministry of Economy and Competitiveness. G. Titos is funded by the Spanish Ministry of Economy and Competitiveness under postdoctoral programme Juan de la Cierva-formación (FJCI-2014-20819). We thank Alberto Cazorla for in-depth discussion about the ceilometer data processing. Ana Calvo is thankfully acknowledged for helpful discussion on the optical spec trometer and providing the diameters correction. Th.View More ; Peer reviewed

The Sierra Nevada Lidar aerOsol Profiling Experiment I and II (SLOPE I and II) campaigns were intended to determine the vertical structure of aerosols by remote sensing instruments and test the various retrieval schemes for obtaining aerosol microphysical and optical properties with in situ measurements. The SLOPE I and II campaigns were developed during the summers of 2016 and 2017, respectively, combining active and passive remote sensing with in situ measurements at stations belonging to the AGORA observatory (Andalusian Global ObseRvatory of the Atmosphere) in the Granada area (Spain). In this work, we use the in situ measurements of these campaigns to evaluate aerosol properties retrieved by the GRASP code (Generalized Retrieval of Atmosphere and Surface Properties) combining lidar and sun–sky photometer measurements. We show an overview of aerosol properties retrieved by GRASP during the SLOPE I and II campaigns. In addition, we evaluate the GRASP retrievals of total aerosol volume concentration (discerning between fine and coarse modes), extinction and scattering coefficients, and for the first time we present an evaluation of the absorption coefficient. The statistical analysis of aerosol optical and microphysical properties, both column-integrated and vertically resolved, from May to July 2016 and 2017 shows a large variability in aerosol load and types. The results show a strong predominance of desert dust particles due to North African intrusions. The vertically resolved analysis denotes a decay of the atmospheric aerosols with an altitude up to 5 km a.s.l. Finally, desert dust and biomass burning events were chosen to show the high potential of GRASP to retrieve vertical profiles of aerosol properties (e.g. absorption coefficient and single scattering albedo) for different aerosol types. The aerosol properties retrieved by GRASP show good agreement with simultaneous in situ measurements (nephelometer, aethalometer, scanning mobility particle sizer, and aerodynamic particle sizer) performed at the Sierra Nevada Station (SNS) in Granada. In general, GRASP overestimates the in situ data at the SNS with a mean difference lower than 6 µm3 cm−3 for volume concentration, and 11 and 2 Mm−1 for the scattering and absorption coefficients. On the other hand, the comparison of GRASP with airborne measurements also shows an overestimation with mean absolute differences of 14 ± 10 and 1.2 ± 1.2 Mm−1 for the scattering and absorption coefficients, showing a better agreement for the absorption (scattering) coefficient with higher (lower) aerosol optical depth. The potential of GRASP shown in this study will contribute to enhancing the representativeness of the aerosol vertical distribution and provide information for satellite and global model evaluation. ; Jose Antonio Benavent-Oltra is funded by the University of Granada through "Plan Propio. Programa 7, Convocatoria 2019". Roberto Román is funded by MINECO under the postdoctoral programme Juan de la Cierva-Incorporación (IJCI2016-30007). Juan Andrés Casquero-Vera is funded by MINECO under the predoctoral programme FPI (BES-2017-080015). Maria J. Granados-Muñoz received funding from the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No 796539. Oleg Dubovik was supported by the Labex CaPPA project, which is funded by the French National Research Agency under contract "ANR-11-LABX0005-01". This work was also supported by the Spanish Ministry of Economy and Competitiveness (projects CMT2015-66742-R, CGL2016-81092-R, CGL2017-85344-R, RTI2018-097864-B-I00 and CGL2017-90884-REDT), by the Andalusia Regional Government through project P18-RT-3820 and the Unity of Excellence "María de Maeztu" (project MDM-2016-0600) financed by the Spanish State Research Agency (AEI). The authors thankfully acknowledge the FEDER programme for the instrumentation used in this work, the University of Granada, which supported this study through the Excellence Units Program, and the Sierra Nevada National Park. We also thank Dr. Grisa Monick who provided the Aethalometer AVIO AE-33 installed on the aircraft. Thanks to AERONET and ACTRIS/AERONET Europe for the scientific and technical support. Finally, the authors would like to acknowledge the use of the GRASP inversion algorithm software (http://www.grasp-open.com, last access: 1 April 2020), in this work. ; Peer reviewed

Ground-level and vertical measurements (performed using tethered and non-tethered balloons), coupled with modelling, of ozone (O3), other gaseous pollutants (NO, NO2, CO, SO2) and aerosols were carried out in the plains (Vic Plain) and valleys of the northern region of the (BMA) in July 2015, an area typically recording the highest O3 episodes in Spain. Our results suggest that these very high O3 episodes were originated by three main contributions: (i) the surface fumigation from high O3 reservoir layers located at 1500-3000 mg-a.g.l. (according to modelling and non-tethered balloon measurements), and originated during the previous day(s) injections of polluted air masses at high altitude; (ii) local/regional photochemical production and transport (at lower heights) from the BMA and the surrounding coastal settlements, into the inland valleys; and (iii) external (to the study area) contributions of both O3 and precursors. These processes gave rise to maximal O3 levels in the inland plains and valleys northwards from the BMA when compared to the higher mountain sites. Thus, a maximum O3 concentration was observed within the lower tropospheric layer, characterised by an upward increase of O3 and black carbon (BC) up to around 100-200 m a.g.l. (reaching up to 300 μg mg-3 of O3 as a 10 s average), followed by a decrease of both pollutants at higher altitudes, where BC and O3 concentrations alternate in layers with parallel variations, probably as a consequence of the atmospheric transport from the BMA and the return flows (to the sea) of strata injected at certain heights the previous day(s). At the highest altitudes reached in this study with the tethered balloons (900-1000 m a.g.l.) during the campaign, BC and O3 were often anti-correlated or unrelated, possibly due to a prevailing regional or even hemispheric contribution of O3 at those altitudes. In the central hours of the days a homogeneous O3 distribution was evidenced for the lowest 1 km of the atmosphere, although probably important variations could be expected at higher levels, where the high O3 return strata are injected according to the modelling results and non-tethered balloon data. Relatively low concentrations of ultrafine particles (UFPs) were found during the study, and nucleation episodes were only detected in the boundary layer. Two types of O3 episodes were identified: type A with major exceedances of the O3 information threshold (180 μg mg-3 on an hourly basis) caused by a clear daily concatenation of local/regional production with accumulation (at upper levels), fumigation and direct transport from the BMA (closed circulation); and type B with regional O3 production without major recirculation (or fumigation) of the polluted BMA/regional air masses (open circulation), and relatively lower O3 levels, but still exceeding the 8 h averaged health target. To implement potential O3 control and abatement strategies two major key tasks are proposed: (i) meteorological forecasting, from June to August, to predict recirculation episodes so that NOx and VOC abatement measures can be applied before these episodes start; (ii) sensitivity analysis with high-resolution modelling to evaluate the effectiveness of these potential abatement measures of precursors for O3 reduction. © 2017 Author(s). ; The present work was supported by the Spanish Ministry of Economy and Competitiveness and FEDER funds under the project HOUSE (CGL2016-78594-R), by the Generalitat de Catalunya (AGAUR 2015 SGR33 and the DGQA). Part of this research was supported by the Korean Ministry of the Environment through "The Eco-Innovation project". The participation of University of Marseille and University of Birmingham was partially supported by two TNA actions projects carried out under the ACTRIS2 project (grant agreement No. 654109) financed by the European Union's Horizon 2020 research and innovation program. The support of the CUD of Zaragoza (project CUD 2013-18) is also acknowledged. We are very thankful to the Generalitat de Catalunya for supplying the air quality data from the XVPCA stations, to METEOCAT (the Meteorological Office of Catalonia) for providing meteorological data and to the IES J. Callís and the Meteorological Station from Vica (especially to Manel Dot) for allowing the performance of the vertical profiles and mobile unit measurements, respectively. In memoriam of Andrei Lyasota ; Peer reviewed

Various studies have reported that the photochemical nucleation of new ultrafine particles (UFPs) in urban environments within high insolation regions occurs simultaneously with high ground ozone (O3) levels. In this work, we evaluate the atmospheric dynamics leading to summer O3 episodes in the Madrid air basin (central Iberia) by means of measuring a 3-D distribution of concentrations for both pollutants. To this end, we obtained vertical profiles (up to 1200m above ground level) using tethered balloons and miniaturised instrumentation at a suburban site located to the SW of the Madrid Metropolitan Area (MMA), the Majadahonda site (MJDH), in July 2016. Simultaneously, measurements of an extensive number of air quality and meteorological parameters were carried out at three supersites across the MMA. Furthermore, data from O3 soundings and daily radio soundings were also used to interpret atmospheric dynamics. The results demonstrate the concatenation of venting and accumulation episodes, with relative lows (venting) and peaks (accumulation) in O3 surface levels. Regardless of the episode type, the fumigation of high-altitude O3 (arising from a variety of origins) contributes the major proportion of surface O3 concentrations. Accumulation episodes are characterised by a relatively thinner planetary boundary layer ( 2400ma.s.l.). This orographic-meteorological setting causes the vertical recirculation of air masses and enrichment of O3 in the lower tropospheric layers. When the highly polluted urban plume from Madrid is affected by these dynamics, the highest Ox (O3CNO2) concentrations are recorded in the MMA. Vertical O3 profiles during venting episodes, with strong synoptic winds and a deepening of the planetary boundary layer reaching > 2000ma.s.l., were characterised by an upward gradient in O3 levels, whereas a reverse situation with O3 concentration maxima at lower levels was found during the accumulation episodes due to local and/or regional production. The two contributions to O3 surface levels (fumigation from high-altitude strata, a high O3 background, and/or regional production) require very different approaches for policy actions. In contrast to O3 vertical top-down transfer, UFPs are formed in the planetary boundary layer (PBL) and are transferred upwards progressively with the increase in PBL growth. © Author(s) 2018. ; Acknowledgements. The present work was supported by the Spanish Ministry of Agriculture, Fishing, Food and Environment, the Madrid City Council and Madrid Regional Government, and by the Ministry of Economy, Industry and Competitiveness and FEDER funds under the project HOUSE (CGL2016-78594-R) and the Gen-eralitat de Catalunya (AGAUR 2017 SGR41). Part of this research was supported by the Korea Ministry of Environment through "The Eco-Innovation project". Support is also acknowledged from the CUD of Zaragoza (project CUD 2016-05), UPV/EHU (UFI 11/47, GIU 16/03), the project PROACLIM CGL2014-52877-R, the City Council of Majadahonda for logistic support, AEMET for providing surface meteorological data, and data from radio soundings and ozone free soundings. We thank Alava Ingenieros, TSI, Solma Environmental Solutions, and Airmodus for their support and María Díez for her computer support in the treatment of radiosonde data. Dr. Escudero has been awarded a José Castillejo grant from the Spanish Ministry of Education and Science (CAS17/00108). ; Peer reviewed

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

The third intensive measurement period (IMP) organised by the European Monitoring and Evaluation Programme (EMEP) under the UNECE CLTRAP took place in summer 2012 and winter 2013, with PM10 filter samples concurrently collected at 20 (16 EMEP) regional background sites across Europe for subsequent analysis of their mineral dust content. All samples were analysed by the same or a comparable methodology. Higher PM10 mineral dust loadings were observed at most sites in summer (0.5-10 μgm-3) compared to winter (0.2-2 μgm-3), with the most elevated concentrations in the southern-and easternmost countries, accounting for 20-40% of PM10. Saharan dust outbreaks were responsible for the high summer dust loadings at western and central European sites, whereas regional or local sources explained the elevated concentrations observed at eastern sites. The eastern Mediterranean sites experienced elevated levels due to African dust outbreaks during both summer and winter. The mineral dust composition varied more in winter than in summer, with a higher relative contribution of anthropogenic dust during the former period. A relatively high contribution of K from non-mineral and non-sea-salt sources, such as biomass burning, was evident in winter at some of the central and eastern European sites. The spatial distribution of some components and metals reveals the influence of specific anthropogenic sources on a regional scale: shipping emissions (V, Ni, and SO2- 4 ) in the Mediterranean region, metallurgy (Cr, Ni, and Mn) in central and eastern Europe, high temperature processes (As, Pb, and SO2- 4 ) in eastern countries, and traffic (Cu) at sites affected by emissions from nearby cities. © 2016 Author(s). CC Attribution 3.0 License. ; The present work was supported by the Cooperative Programme for Monitoring and Evaluation of the Longrange Transmission of Air pollutants in Europe (EMEP) under UNECE. We also acknowledge support by the European Union Seventh Framework Programme (FP7/2007-2013) through ACTRIS (grant agreement no. 262254) and by the European Union's Horizon 2020 research and innovation programme under grant agreement No. 654109. The participation of IDAEA-CSIC was supported by the Spanish Ministry of Economy and Competitiveness and FEDER funds under the project PRISMA (CGL2012-39623-C02-1), by the Generalitat de Catalunya (AGAUR 2015 SGR33 and the DGQA). The authors wish to thank the Norwegian Ministry of foreign affairs for support to the measurements in Armenia and Moldova. The French participation to the campaigns was funded by the French Agency of Environment and Energy Management (ADEME, grants 1262C0022 and 1262C0039). Mines Douai acknowledges support from the CaPPA project which is financed by the French National Research Agency (ANR) through the PIA (Programme d'Investissement d'Avenir) under contract ANR-11-LABX-0005- 01, the "Nord-Pas de Calais" Regional Council and the European Regional Development Fund (ERDF). Participation of the ANDRA is also acknowledged for the measurements at OPE-ANDRA. The authors are also indebted to the fieldwork teams at Auchencorth Moss and Harwell (NERC CEH and Riccardo Energy and Environment Staff). The authors would also like to express our gratitude to the Atmospheric Modelling Laboratory from the Barcelona Supercomputing Centre, the Naval Research Laboratory and the SeaWiFS project (NASA) for the provision of the DREAM, NAAPs aerosol maps and the satellite imagery, respectively. The authors wish to thank D. C. Carslaw and K. Ropkins for providing the Openair software used in this paper (Carslaw and Ropkins, 2012; Carslaw, 2012). ; 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