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High altitude stations are often emphasized as free tropospheric measuring sites but they remain influenced by atmospheric boundary layer (ABL) air masses due to convective transport processes. The local and meso-scale topographical features around the station are involved in the convective boundary layer development and in the formation of thermally induced winds leading to ABL air lifting. The station altitude alone is not a sufficient parameter to characterize the ABL influence. In this study, a topography analysis is performed allowing calculation of a newly defined index called ABL-TopoIndex. The ABL-TopoIndex is constructed in order to correlate with the ABL influence at the high altitude stations and long-term aerosol time series are used to assess its validity. Topography data from the global digital elevation model GTopo30 were used to calculate five parameters for 43 high and 3 middle altitude stations situated on five continents. The geometric mean of these five parameters determines a topography based index called ABL-TopoIndex, which can be used to rank the high altitude stations as a function of the ABL influence. To construct the ABL-TopoIndex, we rely on the criteria that the ABL influence will be low if the station is one of the highest points in the mountainous massif, if there is a large altitude difference between the station and the valleys or high plains, if the slopes around the station are steep, and finally if the inverse drainage basin potentially reflecting the source area for thermally lifted pollutants to reach the site is small. All stations on volcanic islands exhibit a low ABL-TopoIndex, whereas stations in the Himalayas and the Tibetan Plateau have high ABL-TopoIndex values. Spearman's rank correlation between aerosol optical properties and number concentration from 28 stations and the ABL-TopoIndex, the altitude and the latitude are used to validate this topographical approach. Statistically significant (SS) correlations are found between the 5th and 50th percentiles of all aerosol parameters and the ABL-TopoIndex, whereas no SS correlation is found with the station altitude. The diurnal cycles of aerosol parameters seem to be best explained by the station latitude although a SS correlation is found between the amplitude of the diurnal cycles of the absorption coefficient and the ABL-TopoIndex. © 2018 Author(s)., The authors gratefully acknowledge the following persons and organizations. – Wolfgang Schwanghart, the programmer of the TopoToolBox for putting his codes as a freeware and for all the kind and always rapid support he offers. – CHC: the Chacaltaya consortium and Laboratory for Atmospheric Physics at UMSA for taking care of the station and collecting the data. Swedish participation was supported by the Swedish Foundation for International Cooperation in Research and Higher Education (STINT) and the Swedish research council FORMAS. – CMN: the European Commission funded ACTRIS, ACTRIS2 EU project and NEXTDATA National project funded by MIUR. – IZO: Global Atmospheric Watch program funded by AEMET and by the project AEROATLAN (CGL2015-66299-P), funded by the Ministry of Economy and Competitiveness of Spain and the European Regional Development Fund (ERDF). – JFJ: International Foundation High Altitude Research Stations Jungfraujoch and Gornergrat (HFSJG) and the Federal Office of Meteorology and Climatology, MeteoSwiss, within the Swiss program of the Global Atmosphere Watch (GAW) of the World Meteorological Organization, funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement no. 654109 (ACTRIS2), and the Swiss State Secretariat for Education, Research and Innovation (SERI) under contract no. 15.0159-1. The opinions expressed and arguments employed herein do not necessarily reflect the official views of the Swiss Government. – LLN: the Taiwan Environmental Protection Administration. – MSA and MSY: 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.

Although indoor air pollution from the use of biomass fuels is a serious health problem in Senegal, little effort has been made in this country to evaluate indoor air quality impacts from biomass combustion with traditional stoves and indoor air quality improvements derived from the use of improved cookstoves. A cross-sectional study was conducted in a rural village of Senegal to determine indoor air pollution during cooking and non-cooking periods. PM2.5 and CO concentration levels were determined, along with two far less studied pollutants in cookstove studies, ultrafine particles and black carbon, using portable monitors. A total of 22 households were selected, 12 using the traditional stove and 10 using a locally produced rocket stove. Rocket stoves, the most extended type of improved stove used in sub-Saharan Africa, contributed to a significant reduction of total fine and ultrafine (UFP) particles and carbon monoxide (CO) (75,4%, 30,5% and 54,3%, respectively, p

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 Angstrom 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 Angstrom 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.

While exposure to traffic pollutants significantly decreases with distance from the curb, very dense urban architectures hamper such dispersion. Moreover, the building height reduces significantly the dispersion of pollutants. We have investigated the horizontal variability of Black Carbon (BC) and the vertical variability of NO2 and BC within the urban blocks. Increasing the distance from road BC concentrations decreased following an exponential curve reaching halving distances at 25 m (median), although with a wide variability among sites. Street canyons showed sharper fall-offs than open roads or roads next to a park. Urban background concentrations were achieved at 67 m distance on average, with higher distances found for more trafficked roads. Vertical fall-off of BC was less pronounced than the horizontal one since pollutants homogenize quickly vertically after rush traffic hours. Even shallower vertical fall-offs were found for NO2. For both pollutants, background concentrations were never reached within the building height. A street canyon effect was also found exacerbating concentrations at the lowest floors of the leeward side of the road. These inputs can be useful for assessing population exposure, air quality policies, urban planning and for models validation.

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.

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).

Access to detailed comparisons in air quality variations encountered when commuting through a city offers the urban traveller more informed choice on how to minimise personal exposure to inhalable pollutants. In this study we report on an experiment designed to compare atmospheric contaminants inhaled during bus, subway train, tram and walking journeys through the city of Barcelona. Average number concentrations of particles 10-300 nm in size, N, are lowest in the commute using subway trains (N5.0×104cm-3), with extreme transient peaks at busy traffic crossings commonly exceeding 1.0×105cm-3 and accompanied by peaks in Black Carbon and CO. Subway particles are coarser (mode 90nm) than in buses, trams or outdoors (1200ppm in crowded buses and trains. There are also striking differences in inhalable particle chemistry depending on the route chosen, ranging from aluminosiliceous at roadsides and near pavement works, ferruginous with enhanced Mn, Co, Zn, Sr and Ba in the subway environment, and higher levels of Sb and Cu inside the bus. We graphically display such chemical variations using a ternary diagram to emphasise how "air quality" in the city involves a consideration of both physical and chemical parameters, and is not simply a question of measuring particle number or mass. © 2015 The Authors., This work was supported by the ACS Foundation contributing to the dissemination of good environmental practices and environmental protection activities, the Spanish Ministry of Economy and Competitiveness and FEDER funds within the I+D Project CGL2012-33066 (METRO), and the IMPROVE LIFE project ( LIFE13 ENV/ES/000263 ). VM and ASF acknowledge funding from the European Union Seventh Framework Programme ( FP7/2007-2013 ) for a Marie Curie ITN (Grant agreement no. 315760 HEXACOMM ). Additional funding from AXA Research Fund is acknowledged. Fulvio Amato is beneficiary of the Juan de la Cierva postdoctoral Grant ( JCI-2012-13473 ) from the Spanish Ministry of Economy and Competitiveness. Appendix A

High altitude stations are often emphasized as free tropospheric measuring sites but they remain influenced by atmospheric boundary layer (ABL) air masses due to convective transport processes. The local and meso-scale topographical features around the station are involved in the convective boundary layer development and in the formation of thermally induced winds leading to ABL air lifting. The station altitude is not a sufficient parameter to characterize the ABL influence. Topography data from the global digital elevation model GTopo30 were used to calculate 5 parameters for 46 high altitude stations situated in five continents. The geometric mean of these 5 parameters determines a topography based index called ABL-TopoIndex which can be used to rank the high altitude stations as a function of the ABL influence. To construct the ABL-TopoIndex, we rely on the criteria that the ABL influence will be low if the station is one of the highest points in the mountainous massif, if there is a large altitude difference between the station and the valleys or plateaus, if the slopes around the station are steep, and finally if the drainage basin for air convection is small. All stations on volcanic islands exhibit a low ABL-TopoIndex whereas stations in the Himalaya and the Tibetan Plateau have high ABL-TopoIndex values. Spearman's rank correlation between aerosol optical properties and number concentration from 28 stations and the ABL-TopoIndex, the altitude and the latitude are used to validate this topographical approach. Statistically significant (s.s.) correlations are found between the 5 and 50 percentiles of all aerosol parameters and the ABL-TopoIndex whereas no s.s. correlation is found with the station altitude. The diurnal cycles of aerosol parameters seem to be best explained by the station latitude although a s.s. correlation is found between the amplitude of the diurnal cycles of the absorption coefficient and the ABL-TopoIndex. Finally, the main flow paths for air convection were calculated for various ABL heights.

We assessed the sensitivity of simulated mass scattering cross sections (\(\alpha ^{sca}_{\lambda }\) [m\(^{2}\)/g]) of three aerosol species to different particle microphysical properties and derived constraints on these microphysical properties for the north-western Mediterranean basin, by means of a comparison between code calculations and observations. In particular, we calculated \(\alpha ^{sca}_{\lambda }\) of mineral dust, organic carbon and sulfate at three wavelengths in the visible range with a T-matrix optical code, considering \({\pm }20\%\) perturbations on size distribution, refractive index and mass density, and oblate/prolate spheroids with two different axial ratios as shape perturbations. Then, we compared the simulation results with a set of observed \(\alpha ^{sca}_{\lambda }\) of mineral dust, aged organics and ammonium sulfate sources provided by the IDAEA-CSIC of Barcelona (Spain) and representative of the north-western Mediterranean basin.

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

Road dust suspension is an increasing concern in terms of being a source of atmospheric particulate matter (PM) in cities, due to its toxicity and the lack of knowledge on emission estimates, impact and mostly with respect to measures to control or mitigate it. Both technological and policy measures have been proposed, but their application is limited by the gap of knowledge on their effectiveness in the real world. This study analyses the real-world emission factors of road dust at ten sites in the city of Milan (Italy), with an emphasis on the impact of different fleet speeds at one particular road. PM10 emission factors were estimated by means of both the EPA method (based on silt loadings) and the vertical profile of dust deposition. Road dust silt loadings varied within 0.006-0.066 g m-2, with the highest loadings found at sites affected by construction works. Typical urban roads were found to have fleet-averaged emission factors within 13-32 mg vehicle-1 km-1, which is in the central range of the literature values in Europe. The emission factors estimated by means of the vertical profile approach were within 19-26 mg VKT-1, which agree quite well with the EPA method if corrected for speed. In fact, a power-law relation was found between fleet speed and emission factor estimates, with an exponent close to 1.5 for speeds within 36-57 km h-1. These results suggest that the limitation of the maximum traffic speed can be effective for mitigating road dust emissions in cities. © Taiwan Association for Aerosol Research., This study was funded by the Milan Council (Ambiente e Territorio s.r.l., AMAT) and the Italian Ministry of the Environment.

Further research is needed to reduce the existing uncertainties on the effect that specific aerosol sources have on radiative forcing, thus supporting the assessment of future mitigation strategies which should be focused on both air quality and climate, and not acting separately. This study presents a new approach aimed at quantifying the mass scattering and absorption efficiencies (MSE and MAE) of different aerosol sources at urban (Barcelona-BCN), regional (Montseny-MSY) and remote (Montsec-MSA) background sites in the northwestern (NW) Mediterranean. An analysis of source apportionment to the measured scattering and absorption coefficients was performed by means of a multilinear regression (MLR) model during 2010–2014 at BCN and MSY and during 2011–2014 at MSA. The source contributions to PM10 mass, identified by means of the Positive Matrix Factorization (PMF) model, were used as dependent variables in the MLR model in order to take into account the internal mixing state of atmospheric aerosols. Seven aerosol sources were obtained at MSA and MSY and 8 sources at BCN. Mineral, Aged marine, Ammonium sulfate, Ammonium nitrate and V-Ni bearing sources were common at the three sites. Traffic, Industrial/metallurgy and Road-resuspension were isolated at BCN, whereas Industrial/Traffic and Aged organics were solely identified at MSY and MSA. The highest MSE were found for Ammonium sulfate (4.5 and 10.7 m2 g−1), Ammonium nitrate (8.8 and 7.8 m2 g−1) and V-Ni (8 and 3.5 m2 g−1) at MSY and MSA respectively, dominating the scattering throughout the year with marked seasonal trends. V-Ni bearing, originated mainly from shipping emissions, simultaneously contributed to both scattering and absorption being the second most efficient absorptive source in BCN (0.9 m2 g−1). The Traffic source at BCN and the equivalent Industrial/Traffic at MSY and MSA mainly governed the light absorption and exhibited the highest MAE (1.7, 0.9 and 0.2 m2 g−1, respectively). Sources predominantly composed by fine and relatively dark particles such as Industrial/Traffic, Aged organics and V-Ni were simultaneously characterized with low single scattering albedo (SSA) and high scattering Angstrom exponent (SAE). Conversely, Mineral and Aged marine showed the highest SAE and the lowest SSA, being scattering the dominant process in the light extinction. The good agreement between modeled and measured optical properties allowed for the reconstruction of scattering, absorption and SSA time series by means of the PMF-MLR technique for the period 2004–2014 at MSY. Significant decreasing trends were found for the modeled scattering and absorption (−4.6 and −4.1 % y−1) coefficients. Interestingly, the observed reduction in the SSA (−0.11 % y−1) might suggests a less effectiveness of the air quality strategies focused on reducing pollutants containing black carbon (BC) particles, which highly contribute to light absorption and thus climate warming., 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 D. C. Carslaw and K. Ropkins for providing the OpenAir software used in this paper (Carslaw and Ropkins, 2012; Carslaw, 2012).

Ground level and vertical measurements (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 Barcelona Metropolitan Area (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 m a.g.l., 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/m3 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 (900–1000 m a.g.l.) during the campaign, BC and O3 were often anti-correlated or unrelated, possibly due to a prevailing regional/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 free sounding data. Relatively low concentrations of ultrafine particles (UFP) were recorded in the 100–200 m a.g.l. atmospheric layer where concentrations of O3 were high; and nucleation episodes were only detected into the boundary layer. Two types of O3 episodes were identified: Type A) with major exceedances of the O3 information threshold (180 µg/m3 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 (neither fumigation) of the polluted BMA/regional air masses (open circulation), and relatively lower O3 levels. The interpretation of OX (O3 + NO2) experimental data from strategically selected monitoring sites on the coast and inland, together with the photochemical modelling results have allowed to study the O3 phenomenology associated with the onset and development of severe episodes in the region of Catalonia in NE Spain. 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 VOCs 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.

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 %BCbb, with AAE values reaching around 1.5 when %BCbb 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).

Background Commuters usually have choices regarding the mode of public transport they use in the city, but in the context of particulate pollution it is not an especially well-informed choice. We demonstrate from an innovative study in Barcelona that not only the concentration and number but also the chemistry of airborne particles inhaled during the commute vary greatly depending on the chosen travel mode. Methods Portable equipment for measuring black carbon, PM2.5 (mass and chemistry), and number of ultrafine particles (UFP) were carried in a backpack on 78 8-10 km round trip suburb-to-city-centre morning commutes by either tram, subway, bus, or exclusively on foot, with the same start and finish points. All equipment were duplicated, allowing two people (carrying a GPS) to make a simultaneous synchronised journey using different transport modes. Results The study revealed notable differences between the chosen morning commutes. In terms of average number of UFP concentration, the poorest air quality was associated with walking in the city centre (5.4-5.9 × 104 particles/cm3, depending on route chosen). The highest UFP concentrations using public transport occurred during bus travel (mean concentrations of 4.7 × 104 particles/cm3), the lowest in the subway (2.3 × 104 particles/cm3), with the tram registering values in between the other two (3.0 × 104 particles/cm3). Average UFP size was highest in the subway (90nm) and lowest when walking in traffic (54nm), with black carbon levels correspondingly highest when walking (7.3 µg/m3), decreasing to half this value progressively through metro>bus>tram. PM2.5 concentrations were lower when walking and/or in the tram and higher in the subway and bus. Chemical compositions also reveal interesting differences, with peaks in metallic tracers (such as Cu, Sb, Fe, Mn, Al and Ti) depending on transport mode. High transient peaks for all contaminants were related mostly to traffic (UFP numbers, black carbon), roadworks (PM concentrations) or fellow commuters (e.g. smoking). Conclusions Individual exposure to air pollutants while travelling across the city varies greatly depending on the type of transport selected and route taken. To access Barcelona city centre, in terms of both UFP number and PM2.5 concentrations the subway and tram systems are cleaner than the bus. Although walking is to be encouraged for personal exercise and lower average concentrations of PM2.5, the penalty to be paid by pedestrians in the city centre is the exposure to a concentration of well over double the one when travelling by subway.

Highlights • Aerosol scattering simulated under variable microphysical properties (visible range). • Sensitivity of scattering to microphysical properties depends on particle mean size. • Scattering spectral dependence is slightly affected by microphysical assumptions. • Size distribution and real refractive index have strongest impact on scattering. • Comparison with source scattering observations constrained microphysical assumptions. This work has been funded by the Spanish Ministry of Economy and Competitiveness [grant: CGL2013-46736-R] and by the ACTRIS Research Infrastructure Project of the European Union's Horizon 2020 research and innovation programme [grant agreement: No. 654109]. Further support has been provided by the Severo Ochoa Program, awarded by the Spanish Government [grant: SEV-2011-00067]. This work was also supported by the MINECO (Spanish Ministry of Economy and Competitiveness), the MAGRAMA (Spanish Ministry of Agriculture, Food and Environment) and FEDER funds under the PRISMA project [grant: CGL2012-39623-C02/00]. Further fundings have been provided by the European Union's Horizon 2020 research and innovation programme [grant agreement: No. 654109]. Vincenzo Obiso is funded by the Spanish Ministry of Economy and Competitiveness [‘FPI-SO’ grant: SVP-2013-067953]. Marco Pandolfi is funded by the Spanish Ministry of Economy and Competitiveness [‘Ramón y Cajal’ grant: RYC-2013-14036]. We thank Noemi Pérez for providing the PM chemical speciated data for the Montseny station and the developers of the T-Matrix code for making it freely available.

The 2001–2016 contribution of African dust outbreaks to ambient regional background PM10 and PM2.5 levels over Spain, as well as changes induced in the PMx composition over NE Spain in 2009–2016, were investigated. A clear decrease in PMx dust contributions from the Canary Islands to N Iberia was found. A parallel increase in the PM2.5/PM10 ratio (30% in the Canary Islands to 57% in NW Iberia) was evidenced, probably due to size segregation and the larger relative contribution of the local PMx with increasing distance from Africa. PM1–10 and PM2.5–10 measured in Barcelona during African dust outbreaks (ADOs) were 43–46% higher compared to non-ADO days. The continental background contribution prevailed in terms of both PM1–10 and PM2.5–10 during ADO days (62 and 69%, respectively, and 31 and 27% for non-ADO days). The relative contributions of AlO/FeO/CaO to PMx fraction showed that AlO is a suitable tracer for African dust in our context; while CaO at the urban site is clearly affected by local resuspension, construction and road dust, and FeO by dust from vehicle brake discs. The results also provide evidence that PM increases during ADOs are caused not only by the mineral dust load, but by an increased accumulation of locally emitted or co-transported anthropogenic pollutants as compared with non-ADO days. Possible causes for this accumulation are discussed. We recommend that further epidemiological studies should explore independently the potential effects of mineral dust and the anthropogenic PM during ADOs, because, at least over SW Europe, not only mineral dust affects the air quality during African dust episodes. © 2019 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/). Contents lists available at ScienceDirectScience of the Total Environment journal homepage:www.elsevier.com/locate/scitotenv, This study was supported by the Spanish Ministry for the Ecological Transition with a number of research contracts to investigate air quality problems in Spain, the Spanish Ministry of Science, Innovation and Universities and FEDER funds under the project HOUSE (CGL2016-78594-R), the ACTRIS2 project (grant agreement No. 654109) financed by the European Union's Horizon 2020 - Research and Innovation Framework Programme, the Department of Territory and Sustainability and the Catalan Research Agency (AGAUR 2017 SGR41) of the Generalitat de Catalunya. The authors gratefully acknowledge the NOAA Air Resources Laboratory (ARL) for the provision of the HYSPLIT transport and dispersion model (http://www.ready.noaa.gov); and to BSC, Barcelona Supercomputing Centre (https://ess.bsc.es/bsc-dust-daily-forecast), SKIRON-Simulations from the University of Athens (http://forecast.uoa.gr/dustindx.php), and the NAAPs-Navy Research Laboratory outputs (https://www.nrlmry.navy.mil/aerosol_web/) for the open access to their dust forecast systems. The authors wish to thank the Catalan Meteorological Service for providing the BCN radio-sounding data. Marco Pandolfi is funded by a Ramón y Cajal Fellowship (RYC-2013-14036) awarded by the Spanish Ministry of Science, Innovation and Universities.

To estimate global aerosol radiative forcing, measurements of aerosol optical properties are made by the National Oceanic and Atmospheric Administration (NOAA) Earth System Research Laboratory (ESRL)’s Global Monitoring Division (GMD) and their collaborators at 30 monitoring locations around the world. Many of the sites are located in regions influenced by specific aerosol types (Asian and Saharan desert dust, Asian pollution, biomass burning, etc.). This network of monitoring stations is a shared endeavor of NOAA and many collaborating organizations, including the World Meteorological Organization (WMO)’s Global Atmosphere Watch (GAW) program, the U.S. Department of Energy (DOE), several U.S. and foreign universities, and foreign science organizations. The result is a long-term cooperative program making atmospheric measurements that are directly comparable with those from all the other network stations and with shared data access. The protocols and software developed to support the program facilitate participation in GAW’s atmospheric observation strategy, and the sites in the NOAA/ESRL network make up a substantial subset of the GAW aerosol observations. This paper describes the history of the NOAA/ESRL Federated Aerosol Network, details about measurements and operations, and some recent findings from the network measurements., NOAA Climate Program Office’s Atmospheric Chemistry, Carbon Cycle, and Climate (AC4) program

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 (sp) and hemispheric backscattering (bsp) coefficients, scattering Ångström exponent (SAE), backscatter fraction (BF) and asymmetry parameter (g). An increasing gradient of sp is observed when moving from remote environments (arctic/mountain) to regional and to urban environments. At a regional level in Europe, sp 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 sp 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 sp 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 sp values, indicating a larger contribution from particles in the smaller accumulation mode. During periods of high sp 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 sp are observed at 5 out of the 13 stations included in the trend analyses. The total reductions of sp are consistent with those reported for PM2:5 and PM10 mass concentrations over similar periods across Europe.

Deltas provide many worthy ecosystem services. Yet, delta basins are quite vulnerable, especially in the face of climate change, which can affect the outcome of both agriculture and biodiversity. Moreover, rice paddy cultivation is well known to contribute with strong emissions of greenhouse gases (GHGs), such as methane (CH4). Thus, knowing the atmospheric variability of CH4 in relation to the different stages of the rice culture cycle could help to improve GHGs' mitigation strategies in deltas. The Ebro River Delta, in the northwestern Mediterranean basin, forms part of the largest Spanish river basin and is mainly covered by rice fields. In this study, for the first time, ground level (40 cm a.g.l.) atmospheric CH4 concentrations have been monitored in this area, through twenty-seven car mobile transects, over the course of one year. Seasonal, diurnal and spatial variability of CH4 concentrations were studied to identify its relationship with rice cultivation, meteorological conditions and land-use distribution. With regard to seasonal variability, autumn transects showed the highest mean values for atmospheric CH4 (2.466 ppm) when dead rice straw is mixed with the sediment, and weed growth is prevented. Spring and summer measurements gave the highest mean CH4 values at dawn (1.897–3.544 ppm), whereas autumn and winter produced the mean values after sunset (2.148–2.930 ppm). Spatial differences were accounted for by proximity to urban areas, presence of shallow water storage structures, and distance to seawater.