Physical and optical properties of aerosols over an urban location in Spain: seasonal and diurnal variability

Measurements of aerosol optical properties and aerosol number size distribution obtained during the period from December 2005 to November 2007 at Granada, an urban site in south-eastern Spain, are analyzed. Large variations of the measured variables have been found, and related to variations in emissions sources and meteorological conditions. High values of aerosol absorption and scattering coefficients are obtained during winter and low values are measured during summer. This seasonal pattern in the surface aerosol optical properties is opposite to the seasonal cycle showed by columnar aerosol optical depth. The differences in the seasonal features of the surface and column-integrated data are related to seasonal variations in the aerosol vertical distribution, aerosol sources and boundary layer height. In winter the number density of "fine" particles (0.5<particle diameter<1 μm) is significantly larger than in summer while the number density of "coarse" particles (1<particle diameter<20 μm) is slightly larger during summer and spring than during winter and autumn. The scattering Angström exponent, αs, presents an evident seasonal cycle with values of 1.8±0.2, 1.6±0.3, 1.3±0.3 and 1.4±0.3 in winter, spring, summer and autumn, respectively. This suggests the presence of a large fraction of submicron particles at the site, especially during winter. The aerosols measured in this study contain a large fraction of absorbing material as indicated by the average single-scattering albedo that has values of 0.65±0.07, 0.66±0.06, 0.70±0.06 and 0.73±0.06 in autumn, winter, spring and summer, respectively. The aerosol scattering albedo obtained in the surface boundary layer of Granada is below the critical value of 0.86 that determines the shift from cooling to warming. These results put in evidence the need of efforts to reduce absorbing particles (black carbon) emissions to avoid the possible warming that would result from the reductions of the cooling aerosols only. The aerosol absorption and scattering coefficients present a clear diurnal pattern, in all seasons, with two local maxima, one early in the morning and the second one in the evening. This diurnal cycle is mainly attributed to the diurnal evolution of atmospheric boundary layer and local anthropogenic activities.This work was supported by the Spanish Ministry of Science and Technology through projects No: CGL2007-66477-C02-01 and CSD2007-00067 and by the Andalusian Regional Government through projects No: P06-RNM-01503 and P08-RNM-3568

Identification of fine (PM1) and coarse (PM10-1) sources of particulate matter in an urban environment

PM10 and PM1 samples were collected at an urban site in southeastern Spain during 2006-2010. The chemical composition of all samples has been determined and analyzed by Positive Matrix Factorization (PMF) technique for fine and coarse source identification. The PMF results have been analyzed for working and non-working days in order to evaluate the change in PM sources contribution and possible future abatement strategies. A decreasing trend in PM10 levels and in its constituents has been observed, being partly associated to a reduction in anthropogenic activities due to the economic crisis. The use of fine and coarse PM in the PMF analysis allowed us for the identification of additional sources that could not be identified using only one size fraction. The mineral dust source was identified in both fractions and comprised 36 and 22% of the total mass in the coarse and fine fractions, respectively. This high contribution of the mineral source to the fine fraction may be ascribed to contamination of the source profile. The regional re-circulation source was traced by secondary sulfate, V and Ni. It was the most important source concerning PM1 mass concentration (41% of the total mass in this fraction). Although V and Ni are commonly associated to fuel oil combustion the seasonality of this source with higher concentrations in summer compared with winter suggest that the most important part of this source can be ascribed to regional pollution episodes. A traffic exhaust source was identified but only in the fine fraction, comprising 29% of the fine mass. The celestite mines source associated with nearby open-pit mines was typified by strontium, sulfate and mineral matter. PM10-1 levels were higher in working days, whereas PM1 levels remained fairly constant throughout the whole week. As a conclusion, traffic seems to be the main source to target in Granada.This work was supported by the Andalusia Regional Government through projects P12-RNM-2409 and P10-RNM-6299, by the Spanish Ministry of Science and Technology through projects CGL2010-18782, CSD2007-00067, CGL2011-13580-E/CLI and CGL2011-15008-E; and by EU through ACTRIS project (EU INFRA-2010-1.1.16-262254)Titos was funded by Spanish Ministry of Economy and Competitiveness – Secretariat of Science, Innovation and Development under grant BES-2011-043721

Columnar aerosol properties from sun-and-star photometry: statistical comparisons and day-to-night dynamic

This work presents the first analysis of long-term correlative day-to-night columnar aerosol optical properties. The aim is to better understand columnar aerosol dynamic from ground-based observations, which are poorly studied until now. To this end we have used a combination of sun-and-star photometry measurements acquired in the city of Granada (37.16° N, 3.60° W, 680 m a.s.l.; South-East of Spain) from 2007 to 2010. For the whole study period, mean aerosol optical depth (AOD) around 440 nm (± standard deviation) is 0.18 ± 0.10 and 0.19 ± 0.11 for daytime and nighttime, respectively, while the mean Angström exponent (α) is 1.0 ± 0.4 and 0.9 ± 0.4 for daytime and nighttime. The ANOVA statistical tests reveal that there are no significant differences between AOD and α obtained at daytime and those at nighttime. Additionally, the mean daytime values of AOD and α obtained during this study period are coherent with the values obtained in the surrounding AERONET stations. On the other hand, AOD around 440 nm present evident seasonal patterns characterised by large values in summer (mean value of 0.20 ± 0.10 both at daytime and nighttime) and low values in winter (mean value of 0.15 ± 0.09 at daytime and 0.17 ± 0.10 at nighttime). The Angström exponents also present seasonal patterns, but with low values in summer (mean values of 0.8 ± 0.4 and 0.9 ± 0.4 at day- and night-time) and relatively large values in winter (mean values of 1.2 ± 0.4 and 1.0 ± 0.3 at daytime and nighttime). These seasonal patterns are explained by the differences in the meteorological conditions and by the differences in the strength of the aerosol sources. To take more insight about the changes in aerosol particles between day and night, the spectral differences of the Angström exponent as function of the Angström exponent are also studied. These analyses reveal increases of the fine mode radius and of the fine mode contribution to AOD during nighttime, being more remarkable in the summer seasons. These variations are explained by the changes of the local aerosol sources and by the meteorological conditions between daytime and nighttime, as well as aerosol aging processes. Case studies during summer and winter for different aerosol loads and types are also presented to clearly illustrate these findings.This work was supported by the Spanish Ministry of Science and Technology through projects CGL2008-01330-E/CLI (Spanish Lidar Network), CGL2010-18782, CSD2007-00067 and CGL2011-13580-E/CLI; by the Andalusian Regional Government through projects P10-RNM-6299 and P08-RNM-3568; by the EU ACTRIS project (EU INFRA-2010-1.1.16-262254), and by the Postdoctoral Programme of the University of Granada

Cloud Screening and Quality Control Algorithm for Star Photometer Data: Assessment with Lidar Measurements and with All-sky Images

This paper presents the development and set up of a cloud screening and data quality control algorithm for a star photometer based on CCD camera as detector. These algorithms are necessary for passive remote sensing techniques to retrieve the columnar aerosol optical depth, delta Ae(lambda), and precipitable water vapor content, W, at nighttime. This cloud screening procedure consists of calculating moving averages of delta Ae() and W under different time-windows combined with a procedure for detecting outliers. Additionally, to avoid undesirable Ae(lambda) and W fluctuations caused by the atmospheric turbulence, the data are averaged on 30 min. The algorithm is applied to the star photometer deployed in the city of Granada (37.16 N, 3.60 W, 680 ma.s.l.; South-East of Spain) for the measurements acquired between March 2007 and September 2009. The algorithm is evaluated with correlative measurements registered by a lidar system and also with all-sky images obtained at the sunset and sunrise of the previous and following days. Promising results are obtained detecting cloud-affected data. Additionally, the cloud screening algorithm has been evaluated under different aerosol conditions including Saharan dust intrusion, biomass burning and pollution events

Monumental heritage exposure to urban black carbon pollution

In this study, aerosol light-absorption measurements obtained at three sites during a winter campaign were used to analyse and identify the major sources of Black Carbon (BC) particles in and around the Alhambra monument, a UNESCO World Heritage Site that receives over 2 million visitors per year. The Conditional Bivariate Probability Function and the Aethalometer model were employed to identify the main sources of BC particles and to estimate the contributions of biomass burning and fossil fuel emissions to the total Equivalent Black Carbon (EBC) concentrations over the monumental complex. Unexpected high levels of EBC were found at the Alhambra, comparable to those measured in relatively polluted European urban areas during winter. EBC concentrations above 3.0 μg/m3, which are associated with unacceptable levels of soiling and negative public reactions, were observed at Alhambra monument on 13 days from 12 October 2015 to 29 February 2016, which can pose a risk to its long-term conservation and may cause negative social and economic impacts. It was found that road traffic emissions from the nearby urban area and access road to the Alhambra were the main sources of BC particles over the monument. However, biomass burning emissions were found to have very small impact on EBC concentrations at the Alhambra. The highest EBC concentrations were observed during an extended stagnant episode associated with persistent high-pressure systems, reflecting the large impact that can have these synoptic conditions on BC over the Alhambra.European Union's Horizon 2020 Research and Innovation Programme under grant agreement No. 654109, ACTRIS-2.Spanish Ministry of Economy and Competitiveness and FEDER through project CGL2013-45410-R, CGL2016-81092-R 598 and CGL2012-30729.Andalusia Regional Government through project P12- RNM-2409 and P12-FQM-1889

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 fromthree 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 observedNO2 concentration trends. TheNOx andNOconcentrations at these traffic sites showed significant decreasing trends during the period 2003–2014, especially at Barcelona (BARTR) andMadrid (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

Aerosol light-scattering enhancement due to water uptake during the TCAP campaign

Aerosol optical properties were measured by the DOE/ARM (US Department of Energy Atmospheric Radiation Measurements) Program Mobile Facility during the Two-Column Aerosol Project (TCAP) campaign deployed at Cape Cod, Massachusetts, for a 1-year period (from summer 2012 to summer 2013). Measured optical properties included aerosol light-absorption coefficient (σap) at low relative humidity (RH) and aerosol light-scattering coefficient (σsp) at low and at RH values varying from 30 to 85%, approximately. Calculated variables included the single scattering albedo (SSA), the scattering Ångström exponent (SAE) and the scattering enhancement factor (f(RH)). Over the period of measurement, f(RH = 80%) had a mean value of 1.9 ± 0.3 and 1.8 ± 0.4 in the PM10 and PM1 fractions, respectively. Higher f(RH = 80%) values were observed for wind directions from 0 to 180° (marine sector) together with high SSA and low SAE values. The wind sector from 225 to 315° was identified as an anthropogenically influenced sector, and it was characterized by smaller, darker and less hygroscopic aerosols. For the marine sector, f(RH = 80%) was 2.2 compared with a value of 1.8 obtained for the anthropogenically influenced sector. The air-mass backward trajectory analysis agreed well with the wind sector analysis. It shows low cluster to cluster variability except for air masses coming from the Atlantic Ocean that showed higher hygroscopicity. Knowledge of the effect of RH on aerosol optical properties is of great importance for climate forcing calculations and for comparison of in situ measurements with satellite and remote sensing retrievals. In this sense, predictive capability of f(RH) for use in climate models would be enhanced if other aerosol parameters could be used as proxies to estimate hygroscopic growth. Toward this goal, we propose an exponential equation that successfully estimates aerosol hygroscopicity as a function of SSA at Cape Cod. Further work is needed to determine if the equation obtained is valid in other environments.This research was funded by the NOAA Climate Program using measurements funded by the US Department of Energy Atmospheric System Research program. The authors would like to express their gratitude to the NOAA Air Resources Laboratory (ARL) for the provision of the HYSPLIT transport and dispersion model. We would like to thank also the Openair project. G. Titos was funded by the Spanish Ministry of Economy and Competitiveness – Secretariat of Science, Innovation and Development under grants BES-2011-043721 and EEBB-I-13-06456, and projects P10-RNM-6299, CGL2010-18782 and EU INFRA-2010-1.1.16-262254

Aerosol radiative forcing during African desert dust events (2005–2010) over Southeastern Spain

The daily (24 h) averages of the aerosol radiative forcing (ARF) at the surface and the top of the atmosphere (TOA) were calculated during desert dust events over Granada (southeastern Spain) from 2005 to 2010. A radiative transfer model (SBDART) was utilized to simulate the solar irradiance values (0.31–2.8 μm) at the surface and TOA, using as input aerosol properties retrieved from CIMEL sun photometer measurements via an inversion methodology that uses the sky radiance measurements in principal plane configuration and a spheroid particle shape approximation. This inversion methodology was checked by means of simulated data from aerosol models, and the derived aerosol properties were satisfactorily compared against well-known AERONET products. Good agreement was found over a common spectral interval (0.2–4.0 μm) between the simulated SBDART global irradiances at surface and those provided by AERONET. In addition, simulated SBDART solar global irradiances at the surface have been successfully validated against CM-11 pyranometer measurements. The comparison indicates that the radiative transfer model slightly overestimates (mean bias of 3%) the experimental solar global irradiance. These results show that the aerosol optical properties used to estimate ARF represent appropriately the aerosol properties observed during desert dust outbreak over the study area. The ARF mean monthly values computed during desert dust events ranged from −13 ± 8 W m−2 to −34 ± 15 W m−2 at surface, from −4 ± 3 W m−2 to −13 ± 7 W m−2 at TOA and from +6 ± 4 to +21 ± 12 W m−2 in the atmosphere. We have checked if the differences found in aerosol optical properties among desert dust sectors translate to differences in ARF. The mean ARF at surface (TOA) were −20 ± 12 (−5 ± 5) W m−2, −21 ± 9 (−7 ± 5) W m−2 and −18 ± 9 (−6 ± 5) W m−2 for sector A (northern Morocco; northwestern Algeria), sector B (western Sahara, northwestern Mauritania and southwestern Algeria), and sector C (eastern Algeria, Tunisia), respectively. The Kolmogorov-Smirnov statistical test revealed that daily {ARF} values at TOA for sector A were significantly different from the other two sectors, likely as a result of the lower values of single scattering albedo obtained for sector A. The mean values of aerosol radiative forcing efficiency at surface (TOA) were −74 ± 12 W m−2 (−17 ± 7 W m−2) for sector A, −70 ± 14 W m−2 (−20 ± 9 W m−2) for sector B, and −65 ± 16 W m−2 (−22 ± 10 W m−2) for sector C, and thus comparable between the three sectors in all seasons.This work was supported by the Andalusia Regional Government through projects P08-RNM-3568 and P10-RNM-6299, by the Spanish Ministry of Science and Technology through projects CGL2010-18782, CSD2007-00067 and CGL2011-13580-E/CLI; and by EU through ACTRIS project (EU INFRA-2010-1.1.16-262254). The authors thankfully acknowledge the computer resources, technical expertise and assistance provided by the Barcelona Supercomputing Center. ALFA database computation was partly supported by RES (Spanish Supercomputation Network) computing resources (projects AECT-2009-1-0012, AECT-2011-3-0016)

Aerosol properties over the western Mediterranean basin: temporal and spatial variability

This study focuses on the analysis of Aerosol Robotic Network (AERONET) aerosol data obtained over Alborán Island (35.90° N, 3.03° W, 15 m a.s.l.) in the western Mediterranean from July 2011 to January 2012. Additional aerosol data from the three nearest AERONET stations (Málaga, Oujda and Palma de Mallorca) and the Maritime Aerosol Network (MAN) were also analyzed in order to investigate the temporal and spatial variations of aerosol over this scarcely explored region. High aerosol loads over Alborán were mainly associated with desert dust transport from North Africa and occasional advection of anthropogenic fine particles from central European urban-industrial areas. The fine particle load observed over Alborán was surprisingly similar to that obtained over the other three nearest AERONET stations, suggesting homogeneous spatial distribution of fine particle loads over the four studied sites in spite of the large differences in local sources. The results from MAN acquired over the Mediterranean Sea, Black Sea and Atlantic Ocean from July to November 2011 revealed a pronounced predominance of fine particles during the cruise period.This work was supported by the Andalusia Regional Government through projects P12-RNM-2409 and P10-RNM-6299, by the Spanish Ministry of Science and Technology through projects CGL2010-18782, and CGL2013-45410-R; and by the EU through ACTRIS project (EU INFRA-2010-1.1.16-262254). CIMEL Calibration was performed at the AERONET-EUROPE calibration center, supported by ACTRIS (European Union Seventh Framework Program (FP7/2007-2013) under grant agreement no. 262254

Determination and analysis of in situ spectral aerosol optical properties by a multi-instrumental approach

Continuous in situ measurements of aerosol optical properties were conducted from 29 June to 29 July 2012 in Granada (Spain) with a seven-wavelength Aethalometer, a Multi-Angle Absorption Photometer, and a three-wavelength integrating nephelometer. The aim of this work is to describe a methodology to obtain the absorption coefficients (babs) for the different Aethalometer wavelengths. In this way, data have been compensated using algorithms which best estimate the compensation factors needed. Two empirical factors are used to infer the absorption coefficients from the Aethalometer measurements: C – the parameter describing the enhancement of absorption by particles in the filter matrix due to multiple scattering of light in the filter matrix – and f, the parameter compensating for non-linear loading effects in the filter matrix. Spectral dependence of f found in this study is not very strong. Values for the campaign lie in the range from 1.15 at 370 nm to 1.11 at 950 nm. Wavelength dependence in C proves to be more important, and also more difficult to calculate. The values obtained span from 3.42 at 370 nm to 4.59 at 950 nm. Furthermore, the temporal evolution of the Ångström exponent of absorption (αabs) and the single-scattering albedo (ω0) is presented. On average αabs is around 1.1 ± 0.3, and ω0 is 0.78 ± 0.08 and 0.74 ± 0.09 at 370 and 950 nm, respectively. These are typical values for sites with a predominance of absorbing particles, and the urban measurement site in this study is such. The babs average values are of 16 ± 10 Mm−1 (at 370 nm) and 5 ± 3 Mm−1 (at 950 nm), respectively. Finally, differences between workdays and Sundays have been further analysed, obtaining higher babs and lower ω0 during the workdays than on Sundays as a consequence of the diesel traffic influence.This work was financed jointly by the Spanish Ministry of Economy and Competitiveness and the European Regional Development Fund through projects CGL2011-24290, CGL2010-18782, CSD2007-00067, and CGL2012-33294; by the Valencia Autonomous Government through project PROMETEO/2010/064; the Andalusia Regional Government through projects P08-RNM-3568 and P10-RNM-6299; and by the Slovenian Ministry of Economic Development and Technology JR-KROP grant 3211-11-000519. The research leading to these results has received funding from the European Union Seventh Framework Programme (FP7/2007-2013) under grant agreement no. 262254 (ACTRIS). The collaboration of S. Segura in this work was possible thanks to fellowship BES-2010-031626