G. Titos

Study of the relative humidity dependence of aerosol light-scattering in southern Spain

This investigation focuses on the characterisation of the aerosol particle hygroscopicity. Aerosol particle optical properties were measured at Granada, Spain, during winter and spring seasons in 2013. Measured optical properties included particle light-absorption coefficient (σap) and particle light-scattering coefficient (σsp) at dry conditions and at relative humidity (RH) of 85±10%. The scattering enhancement factor, f(RH=85%), had a mean value of 1.5±0.2 and 1.6±0.3 for winter and spring campaigns, respectively. Cases of high scattering enhancement were more frequent during the spring campaign with 27% of the f(RH=85%) values above 1.8, while during the winter campaign only 8% of the data were above 1.8. A Saharan dust event (SDE), which occurred during the spring campaign, was characterised by a predominance of large particles with low hygroscopicity. For the day when the SDE was more intense, a mean daily value of f(RH=85%)=1.3±0.2 was calculated. f(RH=85%) diurnal cycle showed two minima during the morning and afternoon traffic rush hours due to the increase in non-hygroscopic particles such as black carbon and road dust. This was confirmed by small values of the single-scattering albedo and the scattering Ångstrom exponent. A significant correlation between f(RH=85%) and the fraction of particulate organic matter and sulphate was obtained. Finally, the impact of ambient RH in the aerosol radiative forcing was found to be very small due to the low ambient RH. For high RH values, the hygroscopic effect should be taken into account since the aerosol forcing efficiency changed from −13 W/m2 at dry conditions to −17 W/m2 at RH=85%.

Study of mineral dust entrainment in the planetary boundary layer by lidar depolarization technique

Measurements on 27 June 2011 were performed over the Southern Iberian Peninsula at Granada EARLINET station, using active and passive remote sensing and airborne and surface in-situ data in order to study the entrainment processes between aerosols in the free troposphere and those in the planetary boundary layer (PBL). To this aim the temporal evolution of the lidar depolarisation, backscatter-related Angström exponent and potential temperature profiles were used in combination with the PBL contribution to the aerosol optical depth (AOD). Our results show that the mineral dust entrainment in the PBL was caused by the convective processes which ‘trapped’ the lofted mineral dust layer, distributing the mineral dust particles within the PBL. The temporal evolution of ground-based in-situ data evidenced the impact of this process at surface level. Finally, the amount of mineral dust in the atmospheric column available to be dispersed into the PBL was estimated by means of POLIPHON (Polarizing Lidar Photometer Networking). The dust mass concentration derived from POLIPHON was compared with the coarse-mode mass concentration retrieved with airborne in-situ measurements. Comparison shows differences below 50 µg/m3 (30% relative difference) indicating a relative good agreement between both techniques.

Spatial and temporal variability of carbonaceous aerosols: Assessing the impact of biomass burning in the urban environment.

Biomass burning (BB) is a significant source of atmospheric particles in many parts of the world. Whereas many studies have demonstrated the importance of BB emissions in central and northern Europe, especially in rural areas, its impact in urban air quality of southern European countries has been sparsely investigated. In this study, highly time resolved multi-wavelength absorption coefficients together with levoglucosan (BB tracer) mass concentrations were combined to apportion carbonaceous aerosol sources. The Aethalometer model takes advantage of the different spectral behavior of BB and fossil fuel (FF) combustion aerosols. The model was found to be more sensitive to the assumed value of the aerosol Ångström exponent (AAE) for FF (AAEff) than to the AAE for BB (AAEbb). As result of various sensitivity tests the model was optimized with AAEff=1.1 and AAEbb=2. The Aethalometer model and levoglucosan tracer estimates were in good agreement. The Aethalometer model was further applied to data from three sites in Granada urban area to evaluate the spatial variation of CMff and CMbb (carbonaceous matter from FF or BB origin, respectively) concentrations within the city. The results showed that CMbb was lower in the city centre while it has an unexpected profound impact on the CM levels measured in the suburbs (about 40%). Analysis of BB tracers with respect to wind speed suggested that BB was dominated by sources outside the city, to the west in a rural area. Distinguishing whether it corresponds to agricultural waste burning or with biomass burning for domestic heating was not possible. This study also shows that although traffic restrictions measures contribute to reduce carbonaceous concentrations, the extent of the reduction is very local. Other sources such as BB, which can contribute to CM as much as traffic emissions, should be targeted to reduce air pollution.

Intercomparisons of Mobility Size Spectrometers and Condensation Particle Counters in the Frame of the Spanish Atmospheric Observational Aerosol Network

Red Española de DMAs Ambientales (REDMAAS), the Spanish network of environmental differential mobility analyzers (DMAs), currently comprises six research groups involved in the measurement of atmospheric aerosol size distributions by means of DMAs. The aim of this network is to guarantee the good quality and comparability of the routine measurements carried out at each location and in diverse environments across Spain. In order to achieve this objective, one of its main activities is the annual intercomparison of mobility size spectrometers used within the network (five units of scanning mobility particle sizers [SMPS] and one ultrafine particle monitor [UFPM]). Here we report the 2main results obtained during the 2010–2012 campaigns, including a study on particle deposition in dryers used in ambient air sampling systems. In general, all instruments showed good performance with deviations in accepted tolerance. The intercomparisons have been proved to be a useful exercise to detect instrument problems, such as incorrect calibrations. DMA calibration checks were performed with polystyrene latex reference particles. Deviations of less than 1% were observed during the first year, which increased 4.7% during the last campaign. Some differences among the responses of different condensation particle counter (CPC) models were encountered, being mainly connected to the intrinsic characteristics of each counter. The comparison of UFPM with CPCs has given good results. The SMPS intercomparisons, especially for particles above 20 nm, have been within +/−15% tolerance. Regarding particle deposition in dryers used in sampling systems, particle penetration was lower than predicted by the recommended model. This result was probably due to the fact that not all the possible mechanisms were considered in the model. Copyright 2015 American Association for Aerosol Research

Spatiotemporal evolution of a severe winter dust event in the western Mediterranean: Aerosol optical and physical properties

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.

Vertical and horizontal distribution of regional new particle formation events in Madrid

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) Published by Copernicus Publications on behalf of the European Geosciences Union. 16602 C. Carnerero et al.: Vertical and horizontal distribution of regional new particle formation events 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.

Contribution of EARLINET/ACTRIS to the summer 2013 Special Observing Period of the ChArMEx project: monitoring of a Saharan dust event over the western and central Mediterranean

ABSTRACT In the framework of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx; http://charmex.lsce.ipsl.fr/) initiative, a field campaign took place in the western Mediterranean Basin between 10 June and 5 July 2013 within the ADRIMED (Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) project. The scientific objectives of ADRIMED are the characterization of the most common ‘Mediterranean aerosols’ and their direct radiative forcing (column closure and regional scale). During 15–24 June a multi-intrusion dust event took place over the western and central Mediterranean Basin. Extra measurements were carried out by some EARLINET/ACTRIS (European Aerosol Research Lidar Network /Aerosols, Clouds, and Trace gases Research InfraStructure Network, http://www.actris.net/) lidar stations in Spain and Italy, in particular on 22 June in support to the flight over southern Italy of the Falcon 20 aircraft involved in the campaign. This article describes the physical and optical properties of dust observed at the different lidar stations in terms of dust plume centre of mass, optical depth, lidar ratio, and particle depolarization ratio. To link the differences found in the origin of dust plumes, the results are discussed on the basis of back-trajectories and air- and space-borne lidars. This work puts forward the collaboration between a European research infrastructure (ACTRIS) and an international project (ChArMEx) on topics of interest for both parties, and more generally for the atmospheric community.

Impact of primary NO2 emissions at different urban sites exceeding the European NO2 standard limit

A large part of the European population is still exposed to ambient nitrogen dioxide (NO2) levels exceeding the European Union (EU) air quality standards, being a key challenge to reduce NO2 concentrations across many European urban areas, particularly close to roads. In this work, a trend analysis of pollutants involved in NO2 processes was done for the period 2003-2014 in traffic sites from three Spanish cities (Barcelona, Madrid and Granada) that still exceed the European NO2 air quality standard limits. We also estimated the contributions of primary NO2 emissions and photo-chemically formed NO2 to the observed ambient NO2 concentrations in order to explore their possible role in the observed NO2 concentration trends. The NOx and NO concentrations at these traffic sites showed significant decreasing trends during the period 2003-2014, especially at Barcelona (BARTR) and Madrid (MADTR) traffic stations. The NO2 concentrations showed statistically significant downward trends at BARTR and MADTR and remained unchanged at Granada traffic station (GRATR) during the study period. Despite the significant decrease in NO2 concentrations in BCNTR and MADTR during the analysed period, the NO2 concentrations observed over these sites still above the annual NO2 standard limit of 40 μg m-3 and, therefore, more efficient measures are still needed. Primary NO2 emissions significantly influence NO2 concentrations at the three analysed sites. However, as no drastic changes are expected in the after-exhaust treatment technology that can reduce primary NO2 emissions to zero in the near future, only a substantial reduction in NOx emissions will help to comply with the NO2 European air quality standards. Reduction of 78%, 56% and 16% on NOx emissions in Barcelona, Madrid and Granada were estimated to be necessary to comply with the NO2 annual limit of 40 μg m-3.

Atmospheric Particle Size Distributions in the Spanish Network of Environmental DMAs (REDMAAS)

The present work is a first approach to the study of the spatio-temporal variability of the submicrometer atmospheric aerosol in Spain. The aerosol measurements have been obtained simultaneously at seven monitoring stations that compose the REDMAAS network during two measurement campaigns corresponding to summer and winter seasons.In both summer and winter periods those measurement stations with a direct influence of anthropogenic emissions recorded the highest concentrations of particle number. In the summer campaign, the average daily pattern of the aerosol size distribution in the traffic and background urban stations was conditioned by the traffic emissions and secondary aerosol formation through photochemical reactions (new particle formation events, NPF). However, the secondary aerosol had a higher contribution to the aerosol total number concentration in the rural background and high-altitude stations. In the winter campaign, in all sampling sites with the exception of Izana station, the traffic and domestic activity emissions had a greater contribution than secondary aerosol formation on particle number total concentration.New particle formation events were identified at all sites during the summer period, and at sites without direct influence of anthropogenic emissions during the winter campaign. Some aerosol shrinkage processes were also observed at the Madrid and El Arenosillo stations.