Aircraft vertical profiles during summertime regional and Saharan dust scenarios over the north-western Mediterranean basin: aerosol optical and physical properties

We acknowledge support of the publication fee by the CSIC Open Access Publication Support Initiative through its Unit of Information Resources for Research (URICI).This research has been supported by the Generalitat de Catalunya, Agencia de Gestio d'Ajuts Universitaris i de Recerca (grant nos. AGAUR 2014 SGR33 and AGAUR 2017 SGR41); the Ministerio de Economia, Industria y Competitividad, Gobierno de Espana (HOUSE; grant no. CGL2016-78594-R); and the European Commission's Horizon 2020 Framework Programme (ACTRIS-2; grant no. 654109).Accurate measurements of the horizontal and vertical distribution of atmospheric aerosol particle optical properties are key for a better understanding of their impact on the climate. Here we present the results of a measurement campaign based on instrumented flights over north-eastern Spain. We measured vertical profiles of size-segregated atmospheric particulate matter (PM) mass concentrations and multi-wavelength scattering and absorption coefficients in the western Mediterranean basin (WMB). The campaign took place during typical summer conditions, characterized by the development of a vertical multi-layer structure, under both summer regional pollution episodes (REGs) and Saharan dust events (SDEs). REG patterns in the region form under high insolation and scarce precipitation in summer, favouring layering of highly aged fine-PM strata in the lower few kma.s.l. The REG scenario prevailed during the entire measurement campaign. Additionally, African dust outbreaks and plumes from northern African wildfires influenced the study area. The vertical profiles of climate-relevant intensive optical parameters such as single-scattering albedo (SSA); the asymmetry parameter (g); scattering, absorption and SSA Ångström exponents (SAE, AAE and SSAAE); and PM mass scattering and absorption cross sections (MSC and MAC) were derived from the measurements. Moreover, we compared the aircraft measurements with those performed at two GAW–ACTRIS (Global Atmosphere Watch–Aerosol, Clouds and Trace Gases) surface measurement stations located in north-eastern Spain, namely Montseny (MSY; regional background) and Montsec d'Ares (MSA; remote site). Airborne in situ measurements and ceilometer ground-based remote measurements identified aerosol air masses at altitudes up to more than 3.5 kma.s.l. The vertical profiles of the optical properties markedly changed according to the prevailing atmospheric scenarios. During SDE the SAE was low along the profiles, reaching values  2.0, and the asymmetry parameter g was rather low (0.5–0.6) due to the prevalence of fine PM, which was characterized by an AAE close to 1.0, suggesting a fossil fuel combustion origin. During REG, some of the layers featured larger AAE (> 1.5), relatively low SSA at 525 nm ( 9 m2 g−1) and were associated with the influence of PM from wildfires. Overall, the SSA and MSC near the ground ranged around 0.85 and 3 m2 g−1, respectively, and increased at higher altitudes, reaching values above 0.95 and up to 9 m2 g−1. The PM, MSC and MAC were on average larger during REG compared to SDE due to the larger scattering and absorption efficiency of fine PM compared with dust. The SSA and MSC had quite similar vertical profiles and often both increased with height indicating the progressive shift toward PM with a larger scattering efficiency with altitude. This study contributes to our understanding of regional-aerosol vertical distribution and optical properties in the WMB, and the results will be useful for improving future climate projections and remote sensing or satellite retrieval algorithms.Generalitat de Catalunya, Agencia de Gestio d'Ajuts Universitaris i de Recerca AGAUR 2014 SGR33 AGAUR 2017 SGR41Ministerio de Economia, Industria y Competitividad, Gobierno de Espana (HOUSE) CGL2016-78594-REuropean Commission's Horizon 2020 Framework Programme (ACTRIS-2) 65410

Comparing black-carbon- and aerosol-absorption-measuring instruments

We report on an inter-comparison of black-carbon- and aerosol-absorption-measuring instruments with laboratory-generated soot particles coated with controlled amounts of secondary organic matter (SOM). The aerosol generation setup consisted of a miniCAST 5201 Type BC burner for the generation of soot particles and a new automated oxidation flow reactor based on the micro smog chamber (MSC) for the generation of SOM from the ozonolysis of α-pinene. A series of test aerosols was generated with elemental to total carbon (EC  TC) mass fraction ranging from about 90 % down to 10 % and single-scattering albedo (SSA at 637 nm) from almost 0 to about 0.7. A dual-spot Aethalometer AE33, a photoacoustic extinctiometer (PAX, 870 nm), a multi-angle absorption photometer (MAAP), a prototype photoacoustic instrument, and two prototype photo-thermal interferometers (PTAAM-2λ and MSPTI) were exposed to the test aerosols in parallel. Significant deviations in the response of the instruments were observed depending on the amount of secondary organic coating. We believe that the setup and methodology described in this study can easily be standardised and provide a straightforward and reproducible procedure for the inter-comparison and characterisation of both filter-based and in situ black-carbon-measuring (BC-measuring) instruments based on realistic test aerosols

Quantification of source specific black carbon scavenging using an aethalometer and a disdrometer

[EN] Aerosol black carbon (BC) is the second strongest contributor to global warming, after CO2, and it is linked to many adverse health effects. A sampling campaign of 15 months was carried out in León (Spain) in order to evaluate the scavenging of BC with an ensemble aethalometer-disdrometer. The aethalometer provides the concentration of equivalent black carbon (eBC), and the disdrometer, the raindrop size distribution. A total of seventy-five rain events were studied and in 73% of them there was an effective (eBCinitial > eBCfinal) scavenging, with a mean decrease of 48 ± 37% in long rain events (>8 h) and 39 ± 38% in short rain events. The scavenging of BC is strongly related to its source. Thus, the scavenging coefficient (SC) mean value of the BC from fossil fuel (eBCff) for short and long rain events was 5.1 10−5 and 1.3 10−5 s−1, respectively. For the BC from biomass burning (eBCbb), the SC values were 1.6 10−4 and 2.8 10−5 s−1 in short and long events, respectively. There was a significant positive correlation between the SC and the number of drops with diameters between 0.375 and 2.5 mm. Rain scavenging of eBC was analyzed depending on the air mass origin obtaining an effective scavenging for air masses from Atlantic, Arctic and Africa. A linear model (R2 = 0.72) was built to estimate the ΔeBC values with variables from an aethalometer, a disdrometer and a weather station: eBC concentration before rain, swept volume and precipitation accumulated. A Kolmogorov-Smirnov statistical test confirmed the goodness of fit of the model to the measured dataSIThis work was partially supported by the Spanish Ministry of Economy and Competitiveness (Grant TEC2014-57821-R), the University of León (Programa Propio 2015/00054/001) and the AERORAIN project (Ministry of Economy and Competitiveness, Grant CGL2014-52556-R, co-financed with FEDER funds). F. Oduber acknowledges the grant BES-2015-074473 from the Ministry of Economy and Competitiveness. C. del Blanco Alegre acknowledges the grant FPU16/05764 from the Ministry of Education, Culture and Sport

Biomass burning and urban emission impacts in the Andes Cordillera region based on in situ measurements from the Chacaltaya observatory, Bolivia (5240a.s.l.)

This study documents and analyses a 4-year continuous record of aerosol optical properties measured at the Global Atmosphere Watch (GAW) station of Chacaltaya (CHC; 5240a.s.l.), in Bolivia. Records of particle light scattering and particle light absorption coefficients are used to investigate how the high Andean Cordillera is affected by both long-range transport and by the fast-growing agglomeration of La Paz-El Alto, located approximately 20km away and 1.5km below the sampling site. The extended multi-year record allows us to study the properties of aerosol particles for different air mass types, during wet and dry seasons, also covering periods when the site was affected by biomass burning in the Bolivian lowlands and the Amazon Basin. The absorption, scattering, and extinction coefficients (median annual values of 0.74, 12.14, and 12.96Mm-1 respectively) show a clear seasonal variation with low values during the wet season (0.57, 7.94, and 8.68Mm-1 respectively) and higher values during the dry season (0.80, 11.23, and 14.51Mm-1 respectively). The record is driven by variability at both seasonal and diurnal scales. At a diurnal scale, all records of intensive and extensive aerosol properties show a pronounced variation (daytime maximum, night-time minimum), as a result of the dynamic and convective effects. The particle light absorption, scattering, and extinction coefficients are on average 1.94, 1.49, and 1.55 times higher respectively in the turbulent thermally driven conditions than the more stable conditions, due to more efficient transport from the boundary layer. Retrieved intensive optical properties are significantly different from one season to the other, reflecting the changing aerosol emission sources of aerosol at a larger scale. Using the wavelength dependence of aerosol particle optical properties, we discriminated between contributions from natural (mainly mineral dust) and anthropogenic (mainly biomass burning and urban transport or industries) emissions according to seasons and local circulation. The main sources influencing measurements at CHC are from the urban area of La Paz-El Alto in the Altiplano and from regional biomass burning in the Amazon Basin. Results show a 28% to 80% increase in the extinction coefficients during the biomass burning season with respect to the dry season, which is observed in both tropospheric dynamic conditions. From this analysis, long-term observations at CHC provide the first direct evidence of the impact of biomass burning emissions of the Amazon Basin and urban emissions from the La Paz area on atmospheric optical properties at a remote site all the way to the free troposphere. © Author(s) 2019

Biomass burning and urban emission impacts in the Andes Cordillera region based on in situ measurements from the Chacaltaya observatory, Bolivia (5240 m a.s.l.)

This study documents and analyses a 4-year continuous record of aerosol optical properties measured at the Global Atmosphere Watch (GAW) station of Chacaltaya (CHC; 5240 m a.s.l.), in Bolivia. Records of particle light scattering and particle light absorption coefficients are used to investigate how the high Andean Cordillera is affected by both long-range transport and by the fast-growing agglomeration of La Paz-El Alto, located approximately 20 km away and 1.5 km below the sampling site. The extended multiyear record allows us to study the properties of aerosol particles for different air mass types, during wet and dry seasons, also covering periods when the site was affected by biomass burning in the Bolivian lowlands and the Amazon Basin. The absorption, scattering, and extinction coefficients (median annual values of 0.74, 12.14, and 12.96 Mm(-1) respectively) show a clear seasonal variation with low values during the wet season (0.57, 7.94, and 8.68 Mm(-1) respectively) and higher values during the dry season (0.80, 11.23, and 14.51 Mm(-1) respectively). The record is driven by variability at both seasonal and diurnal scales. At a diurnal scale, all records of intensive and extensive aerosol properties show a pronounced variation (daytime maximum, night-time minimum), as a result of the dynamic and convective effects. The particle light absorption, scattering, and extinction coefficients are on average 1.94, 1.49, and 1.55 times higher respectively in the turbulent thermally driven conditions than the more stable conditions, due to more efficient transport from the boundary layer. Retrieved intensive optical properties are significantly different from one season to the other, reflecting the changing aerosol emission sources of aerosol at a larger scale. Using the wavelength dependence of aerosol particle optical properties, we discriminated between contributions from natural (mainly mineral dust) and anthropogenic (mainly biomass burning and urban transport or industries) emissions according to seasons and local circulation. The main sources influencing measurements at CHC are from the urban area of La Paz-El Alto in the Altiplano and from regional biomass burning in the Amazon Basin. Results show a 28 % to 80 % increase in the extinction coefficients during the biomass burning season with respect to the dry season, which is observed in both tropospheric dynamic conditions. From this analysis, long-term observations at CHC provide the first direct evidence of the impact of biomass burning emissions of the Amazon Basin and urban emissions from the La Paz area on atmospheric optical properties at a remote site all the way to the free troposphere.Peer reviewe

Determination of the multiple-scattering correction factor and its cross-sensitivity to scattering and wavelength dependence for different AE33 Aethalometer filter tapes: a multi-instrumental approach

Providing reliable observations of aerosol particles' absorption properties at spatial and temporal resolutions suited to climate models is of utter importance to better understand the effects that atmospheric particles have on climate. Nowadays, one of the instruments most widely used in international monitoring networks for in situ surface measurements of light absorption properties of atmospheric aerosol particles is the multi-wavelength dual-spot Aethalometer, AE33. The AE33 derives the absorption coefficients of aerosol particles at seven different wavelengths from the measurements of the optical attenuation of light through a filter where particles are continuously collected. An accurate determination of the absorption coefficients from the AE33 instrument relies on the quantification of the non-linear processes related to the sample collection on the filter. The multiple-scattering correction factor (C), which depends on the filter tape used and on the optical properties of the collected particles, is the parameter with both the greatest uncertainty and the greatest impact on the absorption coefficients derived from the AE33 measurements. Here we present an in-depth analysis of the AE33 multiple-scattering correction factor C and its wavelength dependence for two different and widely used filter tapes, namely the old, and most referenced, TFE-coated glass, or M8020, filter tape and the currently, and most widely used, M8060 filter tape. For performing this analysis, we compared the attenuation measurements from AE33 with the absorption coefficients measured with different filter-based techniques. On-line co-located multi-angle absorption photometer (MAAP) measurements and off-line PP_UniMI polar photometer measurements were employed as reference absorption measurements for this work. To this aim, we used data from three different measurement stations located in the north-east of Spain, namely an urban background station (Barcelona, BCN), a regional background station (Montseny, MSY) and a mountaintop station (Montsec d'Ares, MSA). The median C values (at 637 nm) measured at the three stations ranged between 2.29 (at BCN and MSY, lowest 5th percentile of 1.97 and highest 95th percentile of 2.68) and 2.51 (at MSA, lowest 5th percentile of 2.06 and highest 95th percentile of 3.06). The analysis of the cross-sensitivity to scattering, for the two filter tapes considered here, revealed a large increase in the C factor when the single-scattering albedo (SSA) of the collected particles was above a given threshold, up to a 3-fold increase above the average C values. The SSA threshold appeared to be site dependent and ranged between 0.90 to 0.95 for the stations considered in the study. The results of the cross-sensitivity to scattering displayed a fitted constant multiple-scattering parameter, Cf, of 2.21 and 1.96, and a cross-sensitivity factor, ms, of 1.8 % and 3.4 % for the MSY and MSA stations, respectively, for the TFE-coated glass filter tape. For the M8060 filter tape, Cf values of 2.50, 1.96 and 1.82 and ms values of 1.6 %, 3.0 % and 4.9 % for the BCN, MSY and MSA stations, respectively, were obtained. SSA variations also influenced the spectral dependence of C, which showed an increase with wavelength when SSA was above the site-dependent threshold. Below the SSA threshold, no statistically significant dependence of C on the wavelength was observed. For the measurement stations considered here, the wavelength dependence of C was to some extent driven by the presence of dust particles during Saharan dust outbreaks that had the potential to increase the SSA above the average values. At the mountaintop station, an omission of the wavelength dependence of the C factor led to an underestimation of the absorption Ångström exponent (AAE) by up to 12 %. Differences in the absorption coefficient determined from AE33 measurements at BCN, MSY and MSA of around 35 %–40 % can be expected when using the site-dependent experimentally obtained C value instead of the nominal C value. Due to the fundamental role that the SSA of the particles collected on the filter tape has in the multiple-scattering parameter C, we present a methodology that allows the recognition of the conditions upon which the use of a constant and wavelength-independent C is feasible.This research has been supported by the Ministerio de Economía, Industria y Competitividad, Gobierno de España (CAIAC project (grant no. PID2019-108990PB-100)); the European Cooperation in Science and Technology (Action CA16109 COLOSSAL); the Agència de Gestió d'Ajuts Universitaris i de Recerca (AGAUR 2017 SGR41); and the European Commission, Horizon 2020 Framework Programme (ACTRIS IMP (grant no. 871115)).Peer reviewe

On-flight intercomparison of three miniature aerosol absorption sensors using unmanned aerial systems (UASs)

The present study investigates and compares the ground and in-flight performance of three miniaturized aerosol absorption sensors integrated on board small-sized Unmanned Aerial Systems (UASs). These sensors were evaluated during two contrasted field campaigns performed at an urban site, impacted mainly by local traffic and domestic wood burning sources (Athens, Greece), and at a remote regional background site, impacted by long-range transported sources including dust (Cyprus Atmospheric Observatory, Agia Marina Xyliatou, Cyprus). The miniaturized sensors were first intercompared at the ground-level against two commercially available instruments used as a reference. The measured signal of the miniaturized sensors was converted into the absorption coefficient and equivalent black carbon concentration (eBC). When applicable, signal saturation corrections were applied, following the suggestions of the manufacturers. The aerosol absorption sensors exhibited similar behavior against the reference instruments during the two campaigns, despite the diversity of the aerosol origin, chemical composition, sources, and concentration levels. The deviation from the reference during both campaigns concerning (eBC) mass was less than 8 %, while for the absorption coefficient it was at least 15 %. This indicates that those sensors that report black carbon mass are tuned and corrected to measure eBC more accurately than the absorption coefficient. The overall potential use of miniature aerosol absorption sensors on board small UASs is also illustrated. UAS-based absorption measurements were used to investigate the vertical distribution of eBC over Athens up to 1 km above sea level during January 2016, exceeding the top of the planetary boundary layer (PBL). Our results reveal a heterogeneous boundary layer concentration of absorbing aerosol within the PBL intensified in the early morning hours due to the concurrent peak traffic emissions at ground-level and the fast development of the boundary layer. After the full development of the PBL, homogenous concentrations are observed from 100 m a.g.l. to the PBL top

Intercomparison and characterization of 23 Aethalometers under laboratory and ambient air conditions : procedures and unit-to-unit variabilities

Aerosolized black carbon is monitored worldwide to quantify its impact on air quality and climate. Given its importance, measurements of black carbon mass concentrations must be conducted with instruments operating in quality-checked and ensured conditions to generate data which are reliable and comparable temporally and geographically. In this study, we report the results from the largest characterization and intercomparison of filter-based absorption photometers, the Aethalometer model AE33, belonging to several European monitoring networks. Under controlled laboratory conditions, a total of 23 instruments measured mass concentrations of black carbon from three well-characterized aerosol sources: synthetic soot, nigrosin particles, and ambient air from the urban background of Leipzig, Germany. The objective was to investigate the individual performance of the instruments and their comparability; we analyzed the response of the instruments to the different aerosol sources and the impact caused by the use of obsolete filter materials and the application of maintenance activities. Differences in the instrument-to-instrument variabilities from equivalent black carbon (eBC) concentrations reported at 880 nm were determined before maintenance activities (for soot measurements, average deviation from total least square regression was -2.0% and the range -16% to 7 %; for nigrosin measurements, average deviation was 0.4% and the range -15% to 17 %), and after they were carried out (for soot measurements, average deviation was 1:0% and the range -14% to 8 %; for nigrosin measurements, the average deviation was 0.5% and the range -12% to 15 %). The deviations are in most of the cases explained by the type of filter material employed by the instruments, the total particle load on the filter, and the flow calibration. The results of this intercomparison activity show that relatively small unit-to-unit variability of AE33-based particle light absorbing measurements is possible with well-maintained instruments. It is crucial to follow the guidelines for maintenance activities and the use of the proper filter tape in the AE33 to ensure high quality and comparable black carbon (BC) measurements among international observational networks.Peer reviewe