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The purpose of this study is to investigate the ability of the Sentinel-5P TROPOspheric Monitoring Instrument (TROPOMI) to derive accurate geometrical features of lofted aerosol layers, selecting the Mediterranean Basin as the study area. Comparisons with ground-based correlative measurements constitute a key component in the validation of passive and active satellite aerosol products. For this purpose, we use ground-based observations from quality-controlled lidar stations reporting to the European Aerosol Research Lidar Network (EARLINET). An optimal methodology for validation purposes has been developed and applied using the EARLINET optical profiles and TROPOMI aerosol products, aiming at the in-depth evaluation of the TROPOMI aerosol layer height (ALH) product for the period 2018 to 2022 over the Mediterranean Basin. Seven EARLINET stations were chosen, taking into consideration their proximity to the sea, which provided 63 coincident aerosol cases for the satellite retrievals. In the following, we present the first validation results for the TROPOMI/S5P ALH using the optimized EARLINET lidar products employing the automated validation chain designed for this purpose. The quantitative validation at pixels over the selected EARLINET stations illustrates that the TROPOMI ALH product is consistent with the EARLINET lidar products, with a high correlation coefficient R=0.82 (R=0.51) and a mean bias of -0.51±0.77 km and -2.27±1.17 km over ocean and land, respectively. Overall, it appears that aerosol layer altitudes retrieved from TROPOMI are systematically lower than altitudes from the lidar retrievals. High-albedo scenes, as well as low-aerosol-load scenes, are the most challenging for the TROPOMI retrieval algorithm, and these results testify to the need to further investigate the underlying cause. This work provides a clear indication that the TROPOMI ALH product can under certain conditions achieve the required threshold accuracy and precision requirements of 1 km, especially when only ocean pixels are included in the comparison analysis. Furthermore, we describe and analyse three case studies in detail, one dust and two smoke episodes, in order to illustrate the strengths and limitations of the TROPOMI ALH product and demonstrate the presented validation methodology. The present analysis provides important additions to the existing validation studies that have been performed so far for the TROPOMI S5P ALH product, which were based only on satellite-to-satellite comparisons.

Six months of stratospheric aerosol observations with the European Aerosol Research Lidar Network (EARLINET) from August 2017 to January 2018 are presented. The decay phase of an unprecedented, record-breaking stratospheric perturbation caused by wildfire smoke is reported and discussed in terms of geometrical, optical, and microphysical aerosol properties. Enormous amounts of smoke were injected into the upper troposphere and lower stratosphere over fire areas in western Canada on 12 August 2017 during strong thunderstorm–pyrocumulonimbus activity. The stratospheric fire plumes spread over the entire Northern Hemisphere in the following weeks and months. Twenty-eight European lidar stations from northern Norway to southern Portugal and the eastern Mediterranean monitored the strong stratospheric perturbation on a continental scale. The main smoke layer (over central, western, southern, and eastern Europe) was found at heights between 15 and 20 km since September 2017 (about 2 weeks after entering the stratosphere). Thin layers of smoke were detected at heights of up to 22–23 km. The stratospheric aerosol optical thickness at 532 nm decreased from values > 0.25 on 21–23 August 2017 to 0.005–0.03 until 5–10 September and was mainly 0.003–0.004 from October to December 2017 and thus was still significantly above the stratospheric background (0.001–0.002). Stratospheric particle extinction coefficients (532 nm) were as high as 50–200 Mm−1 until the beginning of September and on the order of 1 Mm−1 (0.5–5 Mm−1) from October 2017 until the end of January 2018. The corresponding layer mean particle mass concentration was on the order of 0.05–0.5 µg m−3 over these months. Soot particles (light-absorbing carbonaceous particles) are efficient ice-nucleating particles (INPs) at upper tropospheric (cirrus) temperatures and available to influence cirrus formation when entering the tropopause from above. We estimated INP concentrations of 50–500 L−1 until the first days in September and afterwards 5–50 L−1 until the end of the year 2017 in the lower stratosphere for typical cirrus formation temperatures of −55 ∘C and an ice supersaturation level of 1.15. The measured profiles of the particle linear depolarization ratio indicated a predominance of nonspherical smoke particles. The 532 nm depolarization ratio decreased slowly with time in the main smoke layer from values of 0.15–0.25 (August–September) to values of 0.05–0.10 (October–November) and < 0.05 (December–January). The decrease of the depolarization ratio is consistent with aging of the smoke particles, growing of a coating around the solid black carbon core (aggregates), and thus change of the shape towards a spherical form. We found ascending aerosol layer features over the most southern European stations, especially over the eastern Mediterranean at 32–35∘ N, that ascended from heights of about 18–19 to 22–23 km from the beginning of October to the beginning of December 2017 (about 2 km per month). We discuss several transport and lifting mechanisms that may have had an impact on the found aerosol layering structures.

We present the evaluation activity of the European Aerosol Research Lidar Network (EARLINET) for the quantitative assessment of the Level 2 aerosol backscatter coefficient product derived by the Cloud-Aerosol Transport System (CATS) aboard the International Space Station (ISS; Rodier et al., 2015). The study employs correlative CATS and EARLINET backscatter measurements within a 50 km distance between the ground station and the ISS overpass and as close in time as possible, typically with the starting time or stopping time of the EARLINET performed measurement time window within 90 min of the ISS overpass, for the period from February 2015 to September 2016. The results demonstrate the good agreement of the CATS Level 2 backscatter coefficient and EARLINET. Three ISS overpasses close to the EARLINET stations of Leipzig, Germany; Évora, Portugal; and Dushanbe, Tajikistan, are analyzed here to demonstrate the performance of the CATS lidar system under different conditions. The results show that under cloud-free, relative homogeneous aerosol conditions, CATS is in good agreement with EARLINET, independent of daytime and nighttime conditions. CATS low negative biases are observed, partially attributed to the deficiency of lidar systems to detect tenuous aerosol layers of backscatter signal below the minimum detection thresholds; these are biases which may lead to systematic deviations and slight underestimations of the total aerosol optical depth (AOD) in climate studies. In addition, CATS misclassification of aerosol layers as clouds, and vice versa, in cases of coexistent and/or adjacent aerosol and cloud features, occasionally leads to non-representative, unrealistic, and cloud-contaminated aerosol profiles. Regarding solar illumination conditions, low negative biases in CATS backscatter coefficient profiles, of the order of 6.1 %, indicate the good nighttime performance of CATS. During daytime, a reduced signal-to-noise ratio by solar background illumination prevents retrievals of weakly scattering atmospheric layers that would otherwise be detectable during nighttime, leading to higher negative biases, of the order of 22.3 %.

An approach based on the graphical method of Gobbi and co-authors (2007) is introduced to estimate the dependence on altitude of the aerosol fine mode radius (Rf) and of the fine mode contribution (η) to the aerosol optical thickness (AOT) from three-wavelength lidar measurements. The graphical method of Gobbi and co-authors (2007) was applied to AERONET (AErosol RObotic NETwork) spectral extinction observations and relies on the combined analysis of the Ångstrom exponent (å) and its spectral curvature Δå. Lidar measurements at 355, 532 and 1064 nm were used in this study to retrieve the vertical profiles of å and Δå and to estimate the dependence on altitude of Rf and η(532 nm) from the å–Δå combined analysis. Lidar measurements were performed at the Department of Mathematics and Physics of the Universita' del Salento, in south-eastern Italy. Aerosol from continental Europe, the Atlantic, northern Africa, and the Mediterranean Sea are often advected over south-eastern Italy and as a consequence, mixed advection patterns leading to aerosol properties varying with altitude are dominant. The proposed approach was applied to ten measurement days to demonstrate its feasibility in different aerosol load conditions. The selected days were characterized by AOTs spanning the 0.26–0.67, 0.15–0.39, and 0.04–0.27 range at 355, 532, and 1064 nm, respectively. Mean lidar ratios varied within the 31–83, 32–84, and 11–47 sr range at 355, 532, and 1064 nm, respectively, for the high variability of the aerosol optical and microphysical properties. å values calculated from lidar extinction profiles at 355 and 1064 nm ranged between 0.1 and 2.5 with a mean value &pm; 1 standard deviation equal to 1.3 ± 0.7. Δå varied within the −0.1–1 range with mean value equal to 0.25 ± 0.43. Rf and η(532 nm) values spanning the 0.05–0.3 μm and the 0.3–0.99 range, respectively, were associated with the å–Δå data points. Rf and η values showed no dependence on the altitude. 60% of the data points were in the Δå–å space delimited by the η and Rf curves varying within 0.80–0.99 and 0.05–0.15 μm, respectively, for the dominance of fine-mode particles in driving the AOT over south-eastern Italy. Vertical profiles of the linear particle depolarization ratio retrieved from lidar measurements, aerosol products from AERONET sun photometer measurements collocated in space and time, analytical back trajectories, satellite true colour images, and dust concentrations from the BSC–DREAM (Barcelona Super Computing Center-Dust REgional Atmospheric Model) model were used to demonstrate the robustness of the proposed method.

The eruption of the Icelandic volcano Eyjafjallajökull in April–May 2010 represents a "natural experiment" to study the impact of volcanic emissions on a continental scale. For the first time, quantitative data about the presence, altitude, and layering of the volcanic cloud, in conjunction with optical information, are available for most parts of Europe derived from the observations by the European Aerosol Research Lidar NETwork (EARLINET). Based on multi-wavelength Raman lidar systems, EARLINET is the only instrument worldwide that is able to provide dense time series of high-quality optical data to be used for aerosol typing and for the retrieval of particle microphysical properties as a function of altitude. In this work we show the four-dimensional (4-D) distribution of the Eyjafjallajökull volcanic cloud in the troposphere over Europe as observed by EARLINET during the entire volcanic event (15 April–26 May 2010). All optical properties directly measured (backscatter, extinction, and particle linear depolarization ratio) are stored in the EARLINET database available at http://www.earlinet.org. A specific relational database providing the volcanic mask over Europe, realized ad hoc for this specific event, has been developed and is available on request at http://www.earlinet.org. During the first days after the eruption, volcanic particles were detected over Central Europe within a wide range of altitudes, from the upper troposphere down to the local planetary boundary layer (PBL). After 19 April 2010, volcanic particles were detected over southern and south-eastern Europe. During the first half of May (5–15 May), material emitted by the Eyjafjallajökull volcano was detected over Spain and Portugal and then over the Mediterranean and the Balkans. The last observations of the event were recorded until 25 May in Central Europe and in the Eastern Mediterranean area. The 4-D distribution of volcanic aerosol layering and optical properties on European scale reported here provides an unprecedented data set for evaluating satellite data and aerosol dispersion models for this kind of volcanic events.

Volcanic aerosols resulting from the Eyjafjallajökull eruption were detected in south-eastern Italy from 20 to 22 April 2010, at a distance of approximately 4000 km from the volcano, and have been characterized by lidar, sun/sky photometer, and surface in-situ measurements. Volcanic particles added to the pre-existing aerosol load and measurement data allow quantifying the impact of volcanic particles on the aerosol vertical distribution, lidar ratios, the aerosol size distribution, and the ground-level particulate-matter concentrations. Lidar measurements reveal that backscatter coefficients by volcanic particles were about one order of magnitude smaller over south-eastern Italy than over Central Europe. Mean lidar ratios at 355 nm were equal to 64 ± 5 sr inside the volcanic aerosol layer and were characterized by smaller values (47 ± 2 sr) in the underlying layer on 20 April, 19:30 UTC. Lidar ratios and their dependence with the height reduced in the following days, mainly because of the variability of the volcanic particle contributions. Size distributions from sun/sky photometer measurements reveal the presence of volcanic particles with radii r > 0.5 μm on 21 April and that the contribution of coarse volcanic particles increased from 20 to 22 April. The aerosol fine mode fraction from sun/sky photometer measurements varied between values of 0.85 and 0.94 on 20 April and decreased to values between 0.25 and 0.82 on 22 April. Surface measurements of particle size distributions were in good accordance with column averaged particle size distributions from sun/sky photometer measurements. PM1/PM2.5 mass concentration ratios of 0.69, 0.66, and 0.60 on 20, 21, and 22 April, respectively, support the increase of super-micron particles at ground. Measurements from the Regional Air Quality Agency show that PM10 mass concentrations on 20, 21, and 22 April 2010 were enhanced in the entire Apulia Region. More specifically, PM10 mass concentrations have on average increased over Apulia Region 22%, 50%, and 28% on 20, 21, and 22 April, respectively, compared to values on 19 April. Finally, the comparison of measurement data with numerical simulations by the FLEXPART dispersion model demonstrates the ability of FLEXPART to model the advection of the volcanic ash over the 4000 km from the Eyjafjallajökull volcano to Southern Italy.

The regional climate model RegCM3 coupled with a radiatively active aerosol model with online feedback is used to investigate direct and semi-direct radiative aerosol effects over the Sahara and Europe in a test case of July 2003. The aerosol model includes dust particles in addition to sulfates, hydrophobic and hydrophilic black carbon and organic carbon. The role of the aerosol online feedback on the radiation budget and the direct radiative forcing (short-wave and long-wave) by dust particles are investigated by intercomparing results from three experiments: REF, including all interactive aerosol components, Exp1, not accounting for the aerosol radiative feedback, and Exp2 not accounting for desert dust particles. The comparison of results in the REF experiment with satellite observations, sun/sky radiometer measurements, and lidar profiles at selected Central Mediterranean sites reveals that the spatio-temporal evolution of the aerosol optical depth is reasonably well reproduced by the model during the entire month of July. Results for the dust outbreaks of 17 and 24 July, averaged over the simulation domain, show that the daily-mean SW direct radiative forcing by all particles is −24 Wm−2 and −3.4 Wm−2 on 17 July and −25 Wm−2 and −3.5 Wm−2 on 24 July at the surface and top of the atmosphere, respectively. This is partially offset by the LW direct radiative forcing, which is 7.6 Wm−2 and 1.9 Wm−2 on 17 July and 8.4 Wm−2 and 1.9 Wm−2 on 24 July at the surface and top of the atmosphere, respectively. Hence, the daily-mean SW forcing is offset by the LW forcing of ~30% at the surface and of ~50% at the ToA. It is also shown that atmospheric dynamics and hence dust production and advection processes are dependent on the simulation assumptions and may significantly change within few tens of kilometers. The comparison of REF and Exp1 shows that the aerosol online feedback on the radiation budget decreases the domain-average daily-mean value of the 2 m-temperature, aerosol column burden (CB), and short-wave (SW) atmospheric forcing by −0.52 °C, 14%, and 0.9%, respectively on 17 July and by −0.39 °C, 12% and 12%, respectively on 24 July. The comparison of REF and Exp2 reveals that on 17 July, radiatively-active dust particles decrease the daily-mean 2 m-temperature averaged over the whole simulation domain by 0.4% even if are responsible for 99.8% and 97% of the daily-mean aerosol column burden and SW atmospheric forcing, respectively.

The all-sky direct radiative effect by anthropogenic aerosol (DREa) is calculated in the solar (0.3–4 μm) and infrared (4–200 μm) spectral ranges for six Mediterranean sites. The sites are differently affected by pollution and together reflect typical aerosol impacts that are expected over land and coastal sites of the central Mediterranean basin. Central to the simulations are aerosol optical properties from AERONET sun-/sky-photometer statistics for the year 2003. A discussion on the variability of the overall (natural + anthropogenic) aerosol properties with site location is provided. Supplementary data include MODIS satellite sensor based solar surface albedos, ISCCP products for high- mid- and low cloud cover and estimates for the anthropogenic aerosol fraction from global aerosol models. Since anthropogenic aerosol particles are considered to be smaller than 1 μm in size, mainly the solar radiation transfer is affected with impacts only during sun-light hours. At all sites the (daily average) solar DREa is negative all year round at the top of the atmosphere (ToA). Hence, anthropogenic particles produce over coastal and land sites of the central Mediterranean a significant cooling effect. Monthly DREa values vary from site to site and are seasonally dependent as a consequence of the seasonal dependence of available sun-light and microphysical aerosol properties. At the ToA the monthly average DREa is −(4±1) W m−2 during spring-summer (SS, April–September) and −(2±1) W m−2 during autumn-winter (AW, October–March) at the polluted sites. In contrast, it varies between −(3±1) W m−2 and −(1±1) W m−2 on SS and AW, respectively at the less polluted site. Due to atmospheric absorption the DREa at the surface is larger than at the ToA. At the surface the monthly average DREa varies between the most and the least polluted site between −(7±1) W m−2 and −(4±1) W m−2 during SS, and between −(4±3) W m−2 and −(1±1) W m−2 during AW. The DREa at infrared wavelengths is positive but negligible, especially at the ToA (−2). The average of DREa monthly-means referring to all sites has allowed getting a ToA- and sfc-DREa yearly-mean value of −(3±2) and −(5±3) W m−2, respectively at solar wavelengths. Last data, even if refer to a particular year, indicate that the radiative energy-balance of Central Mediterranean land and coastal sites is quite affected by anthropogenic particles.

Aerosol products by AERONET sun-sky radiometer measurements combined with air-mass backtrajectories were analyzed to identify source regions and pathways of air masses carrying aerosols to south-east Italy, and to determine the dependence of aerosol mean optical properties on advection patterns. Aerosol optical depth (AOD), fine mode fraction (η ), single scattering albedo (SSA), asymmetry factor (g), and lidar ratio (Lr) at 440 nm were used to characterize aerosol properties. The analysis of 5-day-backtrajectories ending in Lecce on south-east Italy and referring to 240 measurement days of the 2003–2004 years revealed that 32% of the measurement days were characterized by air masses coming from all continental European sources with the exception of Spain. 3% of the measurement days were characterized by air masses coming from both the Southern Mediterranean Sea and the Africa continent, and the Western Mediterranean, the Iberian Peninsula, and the Atlantic Ocean. 62% of the measurement days were characterized by mixed advection patterns. We found that AOD, SSA and g average values were not significantly dependent on air mass source regions. In contrast, η and Lr average values were quite affected by the air mass source region. AOD, &eta, SSA, g, and Lr average values, which were equal to 0.29±0.15, 0.93±0.03, 0.93±0.03, 0.67±0.03, and 72±20 sr, respectively indicated that the aerosol advected from all continental European sources with the exception of Spain, could be considered representative of "continental average aerosol", mostly made of water soluble and a small amount of soot and insoluble components. Polluted-desert dust particles characterized by AOD=0.29±0.05, η=0.72±0.05, SSA=0.94±0.03, g=0.69±0.02, Lr=56±13 sr, were advected over south-east Italy from the Southern Mediterranean Sea and the Africa continent. The Western Mediterranean, the Iberian Peninsula, and the Atlantic Ocean were instead responsible of the advection of maritime-polluted particles, which were characterized by AOD=0.27±0.17, η=0.8±0.1, SSA=0.94±0.03, g=0.67±0.03, Lr=58±24 sr. Hence, we found that the aerosol load over south-east Italy was dominated by moderately-absorbing, fine-mode particles even if it was also affected by the minor contribution of desert and maritime type aerosol. The application of an aerosol mask to the data points retrieved on measurement days characterized by mixed advection patterns, supported last comment

Dust samples from rainfall residues have been collected in southeast Italy (40º 20' N, 18º 6' E) during dust outbreaks occurred from April to June 2002 to characterize morphological and elemental particle composition by different techniques, and investigate the dependence of particle properties on source regions. Four-day analytical back trajectories and satellite images have been used to infer source regions of the investigated dust samples. It has been found that the TOMS absorbing aerosol index was in the range 0.7-2.2 over Southern Italy when samples have been collected. The particle-size and -shape analysis by a scanning electron microscope (SEM) has revealed either that the particle-diameter distribution was between 0.3 and 30 mm with median-diameter values between 1.7-2.4 mm, and that the particles were characterized by a roundness factor varying from 0.8 to 2.5. The infrared transmission spectra have allowed recognizing that all dust samples contained a significant amount of illite. The X-ray energy dispersive (EDX) measurements have revealed that the Al/Si ratio of the transported dust varies from 0.41 to 0.50, and that the Al/Si, Ca/Al, K/Ca, and Fe/Ca ratios differ according to source regions and therefore can be used as indicators of dust source regions. Indeed, it has been found that dust samples with larger Ca/Al and Si/Al ratios and lower Fe/Ca and K/Ca ratios, have been collected along dust events with a source region in northwestern Sahara. On the contrary, the samples collected along dust events with the origin mainly in Chad, Niger, Algeria and Lybia were characterized by larger Fe/Ca and K/Ca ratios.