ALBERT

Description: 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.

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

Description: 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.

Description: Given the need for accurate knowledge of aerosol microphysical and optical properties with height resolution, various algorithms combining vertically resolved and column-integrated aerosol information have been developed in the last years. Here we present new results of vertically resolved extensive aerosol optical properties (backscattering, scattering and extinction) and volume concentrations retrieved with the GRASP (Generalized Retrieval of Aerosol and Surface Properties) algorithm over a 3-year period. The range-corrected signal (RCS) at 1064 nm measured with a ceilometer and the aerosol optical depth (AOD) and sky radiances from a sun/sky photometer have been used as input for this algorithm. We perform a detailed evaluation of GRASP retrievals with simultaneous in situ measurements performed at the same height, at the Montsec mountaintop observatory (MSA) in the Pre-Pyrenees (northeastern Spain). This is the first long-term evaluation of various outputs of this algorithm; previous evaluations focused only on the study of aerosol volume concentration for short-term periods. In general, our results show good agreement between techniques although GRASP inversions yield higher values than those measured in situ. The statistical analysis of the extinction coefficient vertical profiles shows a clear seasonality as well as significant differences depending on the air mass origin. The observed seasonal cycle is mainly modulated by a higher development of the atmospheric boundary layer (ABL) during warm months, which favors the transport of pollutants to MSA, and higher influence of regional and North African episodes. On the other hand, in winter, MSA is frequently influenced by free-troposphere conditions and venting periods and therefore lower extinction coefficients that markedly decrease with height. This study shows the potentiality of implementing GRASP in ceilometer and lidar networks for obtaining aerosol optical properties and volume concentrations at multiple sites, which will definitely contribute to enhancing the representativeness of the aerosol vertical distribution as well as to providing useful information for satellite and global model evaluation.

Description: 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.

Description: 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 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. (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 m−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 m−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.

Description: 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).

Description: 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.

Description: This paper presents the light scattering properties of atmospheric aerosol particles measured over the past decade at 28 ACTRIS observatories, located mainly in Europe. The data include particle light scattering (σsp) and hemispheric backscattering (σbsp) coefficients, scattering Ångström exponent (SAE), backscatter fraction (BF) and asymmetry parameter (g). A large range of ssp was observed across the network. Low ssp values were on average measured in Nordic and Baltic countries and in Western Europe whereas the highest σsp were measured at regional sites in eastern and central Europe. In these regional areas the SAE was also high indicating the predominance of fine-mode particles. On average, the SAE was lower in the Nordic and Baltic, western and southern countries suggesting a lower fraction of fine-mode particle compared to central and eastern Europe. An increasing gradient of ssp was observed when moving from mountain to regional and to urban sites. Conversely, the mass-independent SAE and g parameters did not show the same gradient. At all sites, both SAE and g varied greatly with aerosol particle loading. The lowest values of g were always observed under low ssp indicating a larger contribution from particles in the smaller accumulation mode. Then, g steeply increased with increasing ssp indicating a progressive shift of the particle size distribution toward the larger end of the accumulation mode. Under periods of high particle mass concentrations, the variation of g was less pronounced whereas the SAE increased or decreased suggesting changes mostly in the coarse aerosol particles mode rather than in the fine mode. The station placement seemed to be the main parameter affecting the intra-annual variability. At mountain sites, higher σsp was measured in summer mainly because of the enhanced boundary layer influence. Conversely, less horizontal and vertical dispersion in winter led to higher σsp at all low altitude sites in central and eastern Europe compared to summer. On average, these sites also showed SAE maxima in summer (and correspondingly g minima). Large intra-annual variability of SAE and g was observed also at Nordic and Baltic countries due to seasonal-dependent transport of different air masses to these remote sites. Statistically significant decreasing trends of σsp were observed at 5 out of 13 stations included in trend analyses. The total reductions of ssp were consistent with those reported for PM2.5 and PM10 mass concentrations over similar periods across Europe.