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High-altitude remote sites are unique places to study aerosol–cloud interactions, since they are located at the altitude where clouds may form. At these remote sites, organic aerosols (OAs) are the main constituents of the overall aerosol population, playing a crucial role in defining aerosol hygroscopicity (κ). To estimate the cloud condensation nuclei (CCN) budget at OA-dominated sites, it is crucial to accurately characterize OA hygroscopicity (κOA) and how its temporal variability affects the CCN activity of the aerosol population, since κOA is not well established due to the complex nature of ambient OA. In this study, we performed CCN closures at a high-altitude remote site during summer to investigate the role of κOA in predicting CCN concentrations under different atmospheric conditions. In addition, we performed an OA source apportionment using positive matrix factorization (PMF). Three OA factors were identified from the PMF analysis: hydrocarbon-like OA (HOA), less-oxidized oxygenated OA (LO-OOA), and more-oxidized oxygenated OA (MO-OOA), with average contributions of 5 %, 36 %, and 59 % of the total OA, respectively. This result highlights the predominance of secondary organic aerosol (SOA) with a high degree of oxidation at this high-altitude site. To understand the impact of each OA factor on the overall OA hygroscopicity, we defined three κOA schemes that assume different hygroscopicity values for each OA factor. Our results show that the different κOA schemes lead to similar CCN closure results between observations and predictions (slope and correlation ranging between 1.08–1.40 and 0.89–0.94, respectively). However, the predictions were not equally accurate across the day. During the night, CCN predictions underestimated observations by 6 %–16 %, while, during morning and midday hours, when the aerosol was influenced by vertical transport of particles and/or new particle formation events, CCN concentrations were overestimated by 0 %–20 %. To further evaluate the role of κOA in CCN predictions, we established a new OA scheme that uses the OA oxidation level (parameterized by the f44 factor) to calculate κOA and predict CCN. This method also shows a large bias, especially during midday hours (up to 40 %), indicating that diurnal information about the oxygenation degree does not improve CCN predictions. Finally, we used a neural network model with four inputs to predict CCN: N80 (number concentration of particles with diameter > 80 nm), OA fraction, f44, and solar global irradiance. This model matched the observations better than the previous approaches, with a bias within ± 10 % and with no daily variation, reproducing the CCN variability throughout the day. Therefore, neural network models seem to be an appropriate tool to estimate CCN concentrations using ancillary parameters accordingly.

The south-central interior of Andalusia experiences intricate precipitation patterns as a result of its semi-arid Mediterranean climate and the impact of Saharan dust and human-made pollutants. The primary aim of this study is to monitor the inter-relations between various factors, such as aerosols, clouds, and meteorological variables, and precipitation systems in Granada using ground-based remote sensing and in situ instruments including a microwave radiometer, ceilometer, cloud radar, nephelometer, and weather station. Over an 11-year period, we detected rain events using a physical retrieval method that employed microwave radiometer measurements. A composite analysis was applied to them to construct a climatology of the temporal evolution of precipitation. It was found that convective rain is the dominant precipitation type in Granada, accounting for 68 % of the rain events. The height of the cloud base is mainly distributed at an altitude of 2 to 7 km. Integrated water vapor (IWV) and integrated cloud liquid water (ILW) increase rapidly before the onset of rain. Aerosol scattering at the surface level and hence the aerosol concentration are reduced during rain, and the predominant mean size distribution of aerosol particles before, during, and after rain is almost the same. A meteorological environment favorable for virga formation is observed in Granada. The surface weather station detected rainfall later than the microwave radiometer, indicating virga according to ceilometer and cloud radar data. We used 889 rain-day events identified by weather station data to determine precipitation intensity classes and found that light rain is the main precipitation intensity class in Granada, accounting for 72 % of the rain-day events. This can be a result of the high tropospheric temperature induced by the Andalusian climate and the reduction of cloud droplet size by the high availability of aerosol particles in the urban atmosphere. This study provides evidence that aerosols, clouds, and meteorological variables have a combined impact on precipitation which can be considered for water resource management and improving rain forecasting accuracy.

The European Aerosol Research Lidar Network (EARLINET), part of the Aerosols, Clouds and Trace gases Research Infrastructure (ACTRIS), organized an intensive observational campaign in May 2020, with the objective of monitoring the atmospheric state over Europe during the COVID-19 lockdown and relaxation period. Besides the standard operational processing of the lidar data in EARLINET, for seven EARLINET sites having collocated sun-photometric observations in the Aerosol Robotic Network (AERONET), a network exercise was held in order to derive profiles of the concentration and effective column size distributions of the aerosols in the atmosphere, by applying the GRASP/GARRLiC (from Generalized Aerosol Retrieval from Radiometer and Lidar Combined data – GARRLiC – part of the Generalized Retrieval of Atmosphere and Surface Properties – GRASP) inversion algorithm. The objective of this network exercise was to explore the possibility of identifying the anthropogenic component and of monitoring its spatial and temporal characteristics in the COVID-19 lockdown and relaxation period. While the number of cases is far from being statistically significant so as to provide a conclusive description of the atmospheric aerosols over Europe during this period, this network exercise was fundamental to deriving a common methodology for applying GRASP/GARRLiC to a network of instruments with different characteristics. The limits of the approach are discussed, in particular the missing information close to the ground in the lidar measurements due to the instrument geometry and the sensitivity of the GRASP/GARRLiC retrieval to the settings used, especially for cases with low aerosol optical depth (AOD) like the ones we show here. We found that this sensitivity is well-characterized in the GRASP/GARRLiC products, since it is included in their retrieval uncertainties.

Detailed knowledge on the formation of new aerosol particles in the atmosphere from precursor gases, and their subsequent growth, commonly known as new particle formation (NPF) events, is one of the largest challenges in atmospheric aerosol science. High pre-existing particle loadings are expected to suppress the formation of new atmospheric aerosol particles due to high coagulation and condensation (CS) sinks. However, NPF events are regularly observed in conditions with high concentrations of pre-existing particles and even during intense desert dust intrusions that imply discrepancies between the observations and theory. In this study, we present a multi-site analysis of the occurrence of NPF events under the presence of desert dust particles in dust-influenced areas. Characterization of NPF events at five different locations highly influenced by desert dust outbreaks was done under dusty and non-dusty conditions using continuous measurements of aerosol size distribution in both fine and coarse size fractions. Contrary to common thought, our results show that the occurrence of NPF events is highly frequent during desert dust outbreaks, showing that NPF event frequencies during dusty conditions are similar to those observed during non-dusty conditions. Furthermore, our results show that NPF events also occur during intense desert dust outbreaks at all the studied sites, even at remote sites where the amounts of precursor vapours are expected to be low. Our results show that the condensation sink associated with coarse particles (CSC) represents up to the 60 % of the total CS during dusty conditions, which highlights the importance of considering coarse-fraction particles for NPF studies in desert-dust-influenced areas. However, we did not find a clear pattern of the effect of desert dust outbreaks on the strength of NPF events, with differences from site to site. The particle growth rate (GR) did not present a clear dependence on the CS during dusty and non-dusty conditions. This result, together with the fact that desert dust has different effects on the growth and formation rates at each site, suggests different formation and growth mechanisms at each site between dusty and non-dusty conditions, probably due to differences in precursor vapours' origins and concentrations as well as changes in the oxidative capacity of pre-existing particles and their effectiveness acting as CS. Further investigation based on multiplatform measurement campaigns and chamber experiments with state-of-the-art gaseous and particulate physical and chemical properties measurements is needed to better understand the role of catalyst components present in desert dust particles in NPF. Finally, our results reveal a significant impact of NPF events on the cloud condensation nuclei (CCN) budget during desert dust outbreaks at the studied sites. Therefore, since desert dust contributes to a major fraction of the global aerosol mass load, and since there is a foreseeable increase in the frequency, duration and intensity of desert dust episodes due to climate change, it is imperative to improve our understanding of the effect of desert dust outbreaks on NPF and the CCN budget for better climate change prediction.

In 2018, the European Space Agency launched the first Doppler wind lidar system into space, providing wind observation profiles from the lower stratosphere down to the surface in two different channels based on the scene classification: cloudy or clear. A statistical validation campaign of Aeolus wind products has been performed with a ground-based Doppler lidar system and radiosondes at the Aerosol, Clouds and Trace Gases Research Infrastructure (ACTRIS)–Andalusian Global ObseRvatory of the Atmosphere (AGORA) facility in Granada (Spain). The validation activities with the automatic ground-based lidar system lasted from July 2019 to the orbit shift of June 2021. Aeolus data from two different processing baselines (10 and 11) were validated with 30 min averages of coincident ground-based lidar measurements, using a 100 km horizontal spatial collocation criterion. This resulted in 109 collocations and a mean observation distance from the ground-based lidar system of ∼50 km. The comparison did not raise any significant over- or underestimation of Aeolus horizontal line-of-sight wind speed during that period for the Rayleigh-clear and Mie-cloudy configurations. However, the ground-based lidar measurements were limited to the lower 3.5 km of the atmosphere and, consequently, the obtained results. Multiple analyses were performed varying the criteria of maximum distance and the average period for the ground-based lidar measurements in order to confirm the reliability of the criteria considered. A separate study was performed with Aeolus products after the orbit shift (baseline 12) with different collocation criteria (mean observation distance of ∼75 km, to the station), from July 2021 to May 2022. A set of seven radiosondes were launched with the aim of increasing their coincidence in space and time with the satellite overpass (∼30 min before). The radiosondes could provide full vertical coverage of Aeolus profiles (from the surface up to ∼20 km above sea level), and the comparison did not yield any significant over- or underestimation of the Rayleigh-clear wind speed, while the Mie-cloudy wind speed was significantly overestimated. Multiple analyses were performed in order to test how the spatiotemporal collocation of the radiosonde affected the results. Radiosondes not ideally collocated were proven to still be useful for comparison with the Rayleigh-clear observations but not with the Mie-cloudy observations.

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.

An intense and long-lasting Saharan dust outbreak crossed the Iberian Peninsula (IP) from the southwest (SW) to the northeast (NE) from 25 March until 7 April 2021. This work aims to assess the optical and mass contribution of both fine and coarse dust particles along their transport. Five Iberian lidar stations were monitoring the transport and evolution of the Saharan dust particles, i.e. El Arenosillo/Huelva, Granada, Torrejón/Madrid and Barcelona in Spain, and Évora in Portugal. The particular meteorological conditions determined the aerosol scenario along the overall dust event, differing in the first part of the event (25–31 March), in which the strongest dust incidence occurred on 29–31 March at the south and central stations and 1 April at Barcelona, from the second one (1–7 April). The use of the two-step POLIPHON algorithm showed the relevance of using polarized lidar measurements for separating the aerosol properties of dust fine and coarse particles as an added value. Both the fine dust (Df) and coarse dust (Dc) components of the total particle backscatter coefficient (total dust, DD = Dc + Df) were separately derived. The dust plume was well-mixed with height and no significant differences were found in the vertical structure of both the Dc and Df particle backscatter coefficients. From the beginning of the dust outbreak until 1 April, the vertical Df / DD mass ratio was nearly constant in time at each station and also in altitude with values of ∼ 10 %. Moreover, the mean dust optical depth at 532 nm was decreasing along that dust pathway, reporting values from SW to NE stations of 0.34 at El Arenosillo/Huelva, 0.28 at Granada, 0.20 at Évora, 0.28 at Torrejón/Madrid, and 0.14 at Barcelona, although its Df / DD ratio remained almost constant (28 %–30 %). A similar pattern was found for the total dust mass loading and its Df / DD ratio, i.e. mostly decreasing mean mass values were reported, being constant in its Df / DD ratio (∼ 10 %) along the SW–NE dust pathway. In addition, the episode-mean centre-of-mass height increased with latitude overall, showing a high variability, being greater than 0.5 km at the southern sites (El Arenosillo/Huelva, Granada, Évora) and ∼ 1.0 km at Torrejón/Madrid and Barcelona. However, despite the relatively high intensity of the dust intrusion, the expected ageing of the dust particles was hardly observed, by taking into account the minor changes found in the contribution and properties of the coarse and fine dust particles. This is on the basis that the IP is relatively close to the Saharan dust sources and then, under certain dust transport conditions, any potential ageing processes in the dust particles remained unappreciated. The following must be highlighted: the different relative contribution of the fine dust particles to the total dust found for their optical properties (∼ 30 %) associated with the radiative effect of dust, with respect to that for the mass features (∼ 10 %) linked to air quality issues, along the overall dust event by crossing the IP.

The atmospheric boundary layer (ABL) defines the volume of air adjacent to the Earth's surface for the dilution of heat, moisture, and trace substances. Quantitative knowledge on the temporal and spatial variations in the heights of the ABL and its sub-layers is still scarce, despite their importance for a series of applications (including, for example, air quality, numerical weather prediction, greenhouse gas assessment, and renewable energy production). Thanks to recent advances in ground-based remote-sensing measurement technology and algorithm development, continuous profiling of the entire ABL vertical extent at high temporal and vertical resolution is increasingly possible. Dense measurement networks of autonomous ground-based remote-sensing instruments, such as microwave radiometers, radar wind profilers, Doppler wind lidars or automatic lidars and ceilometers are hence emerging across Europe and other parts of the world. This review summarises the capabilities and limitations of various instrument types for ABL monitoring and provides an overview on the vast number of retrieval methods developed for the detection of ABL sub-layer heights from different atmospheric quantities (temperature, humidity, wind, turbulence, aerosol). It is outlined how the diurnal evolution of the ABL can be monitored effectively with a combination of methods, pointing out where instrumental or methodological synergy are considered particularly promising. The review highlights the fact that harmonised data acquisition across carefully designed sensor networks as well as tailored data processing are key to obtaining high-quality products that are again essential to capture the spatial and temporal complexity of the lowest part of the atmosphere in which we live and breathe.

The Global Observing System (GOS) has encountered some limitations due to a lack of worldwide real-time wind measurements. In this context, the European Space Agency (ESA) has developed the Aeolus satellite mission, based on the ALADIN (Atmospheric Laser Doppler Instrument) Doppler wind lidar; this mission aims to obtain near-real-time wind retrievals at the global scale. As spin-off products, the instrument retrieves aerosol optical properties such as particle backscatter and extinction coefficients. In this work, a validation of Aeolus reprocessed (baseline 10) co-polar backscatter coefficients (βAeoluspart) is presented through an intercomparison with analogous ground-based measurements taken at the ACTRIS (Aerosols, Clouds and Trace gases Research InfraStructure Network)/EARLINET (European Aerosol Research Lidar Network) stations of Granada (Spain), Évora (Portugal) and Barcelona (Spain) over the period from July 2019 until October 2020. Case studies are first presented, followed by a statistical analysis. The stations are located in a hot spot between Africa and the rest of Europe, which guarantees a variety of aerosol types, from mineral dust layers to continental/anthropogenic aerosol, and allows us to test Aeolus performance under different scenarios. The so called Aeolus-like profiles (βAeoluslike,355part) are obtained from total particle backscatter coefficient and linear particle depolarization ratio (δlinearpart) profiles at 355 and 532 nm measured from the surface, through a thorough bibliographic review of dual-polarization measurements for relevant aerosol types. Finally, the study proposes a relation for the spectral conversion of δlinearpart, which is implemented in the Aeolus-like profile calculation. The statistical results show the ability of the satellite to detect and characterize significant aerosol layers under cloud-free conditions, along with the surface effect on the lowermost measurements, which causes the satellite to largely overestimate co-polar backscatter coefficients. Finally, the Aeolus standard correct algorithm middle bin (SCAmb) shows a better agreement with ground-based measurements than the standard correct algorithm (SCA), which tends to retrieve negative and meaningless coefficients in the clear troposphere. The implementation of Aeolus quality flags entails a vast reduction in the number of measurements available for comparison, which affects the statistical significance of the results.

The scattering and backscattering enhancement factors (f(RH) and fb(RH)) describe how aerosol particle light scattering and backscattering, respectively, change with relative humidity (RH). They are important parameters in estimating direct aerosol radiative forcing (DARF). In this study we use the dataset presented in Burgos et al. (2019) that compiles f(RH) and fb(RH) measurements at three wavelengths (i.e., 450, 550 and 700 nm) performed with tandem nephelometer systems at multiple sites around the world. We present an overview of f(RH) and fb(RH) based on both long-term and campaign observations from 23 sites representing a range of aerosol types. The scattering enhancement shows a strong variability from site to site, with no clear pattern with respect to the total scattering coefficient. In general, higher f(RH) is observed at Arctic and marine sites, while lower values are found at urban and desert sites, although a consistent pattern as a function of site type is not observed. The backscattering enhancement fb(RH) is consistently lower than f(RH) at all sites, with the difference between f(RH) and fb(RH) increasing for aerosol with higher f(RH). This is consistent with Mie theory, which predicts higher enhancement of the light scattering in the forward than in the backward direction as the particle takes up water. Our results show that the scattering enhancement is higher for PM1 than PM10 at most sites, which is also supported by theory due to the change in scattering efficiency with the size parameter that relates particle size and the wavelength of incident light. At marine-influenced sites this difference is enhanced when coarse particles (likely sea salt) predominate. For most sites, f(RH) is observed to increase with increasing wavelength, except at sites with a known dust influence where the spectral dependence of f(RH) is found to be low or even exhibit the opposite pattern. The impact of RH on aerosol properties used to calculate radiative forcing (e.g., single-scattering albedo, ω0, and backscattered fraction, b) is evaluated. The single-scattering albedo generally increases with RH, while b decreases. The net effect of aerosol hygroscopicity on radiative forcing efficiency (RFE) is an increase in the absolute forcing effect (negative sign) by a factor of up to 4 at RH = 90 % compared to dry conditions (RH < 40 %). Because of the scarcity of scattering enhancement measurements, an attempt was made to use other more commonly available aerosol parameters (i.e., ω0 and scattering Ångström exponent, αsp) to parameterize f(RH). The majority of sites (75 %) showed a consistent trend with ω0 (higher f(RH = 85 %) for higher ω0), while no clear pattern was observed between f(RH = 85 %) and αsp. This suggests that aerosol ω0 is more promising than αsp as a surrogate for the scattering enhancement factor, although neither parameter is ideal. Nonetheless, the qualitative relationship observed between ω0 and f(RH) could serve as a constraint on global model simulations.

The Sierra Nevada Lidar aerOsol Profiling Experiment I and II (SLOPE I and II) campaigns were intended to determine the vertical structure of aerosols by remote sensing instruments and test the various retrieval schemes for obtaining aerosol microphysical and optical properties with in situ measurements. The SLOPE I and II campaigns were developed during the summers of 2016 and 2017, respectively, combining active and passive remote sensing with in situ measurements at stations belonging to the AGORA observatory (Andalusian Global ObseRvatory of the Atmosphere) in the Granada area (Spain). In this work, we use the in situ measurements of these campaigns to evaluate aerosol properties retrieved by the GRASP code (Generalized Retrieval of Atmosphere and Surface Properties) combining lidar and sun–sky photometer measurements. We show an overview of aerosol properties retrieved by GRASP during the SLOPE I and II campaigns. In addition, we evaluate the GRASP retrievals of total aerosol volume concentration (discerning between fine and coarse modes), extinction and scattering coefficients, and for the first time we present an evaluation of the absorption coefficient. The statistical analysis of aerosol optical and microphysical properties, both column-integrated and vertically resolved, from May to July 2016 and 2017 shows a large variability in aerosol load and types. The results show a strong predominance of desert dust particles due to North African intrusions. The vertically resolved analysis denotes a decay of the atmospheric aerosols with an altitude up to 5 km a.s.l. Finally, desert dust and biomass burning events were chosen to show the high potential of GRASP to retrieve vertical profiles of aerosol properties (e.g. absorption coefficient and single scattering albedo) for different aerosol types. The aerosol properties retrieved by GRASP show good agreement with simultaneous in situ measurements (nephelometer, aethalometer, scanning mobility particle sizer, and aerodynamic particle sizer) performed at the Sierra Nevada Station (SNS) in Granada. In general, GRASP overestimates the in situ data at the SNS with a mean difference lower than 6 µm3 cm−3 for volume concentration, and 11 and 2 Mm−1 for the scattering and absorption coefficients. On the other hand, the comparison of GRASP with airborne measurements also shows an overestimation with mean absolute differences of 14 ± 10 and 1.2 ± 1.2 Mm−1 for the scattering and absorption coefficients, showing a better agreement for the absorption (scattering) coefficient with higher (lower) aerosol optical depth. The potential of GRASP shown in this study will contribute to enhancing the representativeness of the aerosol vertical distribution and provide information for satellite and global model evaluation.

Following the emergence of the severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) responsible for COVID-19 in December 2019 in Wuhan (China) and its spread to the rest of the world, the World Health Organization declared a global pandemic in March 2020. Without effective treatment in the initial pandemic phase, social distancing and mandatory quarantines were introduced as the only available preventative measure. In contrast to the detrimental societal impacts, air quality improved in all countries in which strict lockdowns were applied, due to lower pollutant emissions. Here we investigate the effects of the COVID-19 lockdowns in Europe on ambient black carbon (BC), which affects climate and damages health, using in situ observations from 17 European stations in a Bayesian inversion framework. BC emissions declined by 23 kt in Europe (20 % in Italy, 40 % in Germany, 34 % in Spain, 22 % in France) during lockdowns compared to the same period in the previous 5 years, which is partially attributed to COVID-19 measures. BC temporal variation in the countries enduring the most drastic restrictions showed the most distinct lockdown impacts. Increased particle light absorption in the beginning of the lockdown, confirmed by assimilated satellite and remote sensing data, suggests residential combustion was the dominant BC source. Accordingly, in central and Eastern Europe, which experienced lower than average temperatures, BC was elevated compared to the previous 5 years. Nevertheless, an average decrease of 11 % was seen for the whole of Europe compared to the start of the lockdown period, with the highest peaks in France (42 %), Germany (21 %), UK (13 %), Spain (11 %) and Italy (8 %). Such a decrease was not seen in the previous years, which also confirms the impact of COVID-19 on the European emissions of BC.

Remote sensing measurements of aerosols using depolarization Raman lidar systems from four EARLINET (European Aerosol Research Lidar Network) stations are used for a comprehensive analysis of Saharan dust events over the Mediterranean basin in the period 2014–2017. In this period, 51 dust events regarding the geometrical, optical and microphysical properties of dust were selected, classified and assessed according to their radiative forcing effect on the atmosphere. From west to east, the stations of Granada, Potenza, Athens and Limassol were selected as representative Mediterranean cities regularly affected by Saharan dust intrusions. Emphasis was given on lidar measurements in the visible (532 nm) and specifically on the consistency of the particle linear depolarization ratio (δp532), the extinction-to-backscatter lidar ratio (LR532) and the aerosol optical thickness (AOT532) within the observed dust layers. We found mean δp532 values of 0.24±0.05, 0.26±0.06, 0.28±0.05 and 0.28±0.04, mean LR532 values of 52±8, 51±9, 52±9 and 49±6 sr and mean AOT532 values of 0.40±0.31, 0.11±0.07, 0.12±0.10 and 0.32±0.17, for Granada, Potenza, Athens and Limassol, respectively. The mean layer thickness values were found to range from ∼ 1700 to ∼ 3400 m a.s.l. Additionally, based also on a previous aerosol type classification scheme provided by airborne High Spectral Resolution Lidar (HSRL) observations and on air mass backward trajectory analysis, a clustering analysis was performed in order to identify the mixing state of the dusty layers over the studied area. Furthermore, a synergy of lidar measurements and modeling was used to analyze the solar and thermal radiative forcing of airborne dust in detail. In total, a cooling behavior in the solar range and a significantly lower heating behavior in the thermal range was estimated. Depending on the dust optical and geometrical properties, the load intensity and the solar zenith angle (SZA), the estimated solar radiative forcing values range from −59 to −22 W m−2 at the surface and from −24 to −1 W m−2 at the top of the atmosphere (TOA). Similarly, in the thermal spectral range these values range from +2 to +4 W m−2 for the surface and from +1 to +3 W m−2 for the TOA. Finally, the radiative forcing seems to be inversely proportional to the dust mixing ratio, since higher absolute values are estimated for less mixed dust layers.

The emergence of Moon photometers is allowing measurements of lunar irradiance over the world and increasing the potential to derive aerosol optical depth (AOD) at night-time, which is very important in polar areas. Actually, new photometers implement the latest technological advances that permit lunar-irradiance measurements together with classical Sun photometry measurements. However, a proper use of these instruments for AOD retrieval requires accurate time-dependent knowledge of the extraterrestrial lunar irradiance over time due to its fast change throughout the Moon's cycle. This paper uses the RIMO (ROLO Implementation for Moon's Observation) model (an implementation of the ROLO – RObotic Lunar Observatory – model) to estimate the AOD at night-time assuming that the calibration of the solar channels can be transferred to the Moon by a vicarious method. However, the obtained AOD values using a Cimel CE318-T Sun–sky–Moon photometer for 98 pristine nights with low and stable AOD at the Izaña Observatory (Tenerife, Spain) are not in agreement with the expected (low and stable) AOD values estimated by linear interpolations from daytime values obtained during the previous evening and the following morning. Actually, AOD calculated using RIMO shows negative values and with a marked cycle dependent on the optical air mass. The differences between the AOD obtained using RIMO and the expected values are assumed to be associated with inaccuracies in the RIMO model, and these differences are used to calculate the RIMO correction factor (RCF). The RCF is a proposed correction factor that, multiplied by the RIMO value, gives an effective extraterrestrial lunar irradiance that provides AOD closer to the expected values. The RCF varies with the Moon phase angle (MPA) and with wavelength, ranging from 1.01 to 1.14, which reveals an overall underestimation of RIMO compared to the lunar irradiance. These obtained RCF values are modelled for each photometer wavelength to a second-order polynomial as a function of MPA. The AOD derived by this proposed method is compared with the independent AOD measurements obtained by a star photometer at Granada (Spain) for 2 years. The mean of the Moon–star AOD differences is between −0.015 and −0.005, and the standard deviation (SD) is between 0.03 and 0.04 (which is reduced to about 0.01 if 1 month of data affected by instrumental issues is not included in the analysis) for 440, 500, 675, and 870 nm; however, for 380 nm, the mean and standard deviation of these differences are higher. The Moon–star AOD differences are also analysed as a function of MPA, showing no significant dependence.

A substantial fraction of the atmospheric aerosols originates from secondary new particle formation (NPF), where atmospheric vapours are transformed into particles that subsequently grow to larger sizes, affecting human health and the climate. In this study, we investigate aerosol size distributions at two stations located close to each other (∼ 20 km) but at different altitudes: urban (UGR; 680 m a.s.l., metres above sea level) and high-altitude remote (SNS; 2500 m a.s.l.) sites, both in the area of Granada, Spain, and part of AGORA observatory (Andalusian Global ObseRvatory of the Atmosphere). The analysis shows a significant contribution of nucleation mode aerosol particles to the total aerosol number concentration at both sites, with a contribution of 47 % and 48 % at SNS and UGR, respectively. Due to the important contribution of NPF events to the total aerosol number concentrations and their high occurrence frequency (> 70 %) during the study period, a detailed analysis of NPF events is done in order to get insight into the possible mechanisms and processes involved in NPF events at these contrastive sites. At SNS, NPF is found to be associated with the transport of gaseous precursors from lower altitudes by orographic buoyant upward flows. NPF events at the SNS site are always observed from the smallest measured sizes of the aerosol size distribution (4 nm), implying that NPF takes place in or in the vicinity of the high-altitude SNS station rather than being transported from lower altitudes. Although NPF events at the mountain site seem to be connected with those occurring at the urban site, growth rates (GRs) at SNS are higher than those at the UGR site (GR7−25 of 6.9 and 4.5 nm h−1 and GR4−7 of 4.1 and 3.6 nm h−1 at SNS and UGR, respectively). This fact could have special importance for the production of cloud condensation nuclei (CCN) and therefore for cloud formations which may affect regional/global climate, since larger GRs at mountain sites could translate to a larger survival probability of NPF particles reaching CCN sizes, due to the shorter time period needed for the growth. The analysis of sulfuric acid (H2SO4) shows that the contribution of H2SO4 is able to explain a minimal fraction contribution to the observed GRs at both sites (< 1 % and < 10 % for the 7–25 and 4–7 nm size ranges, respectively), indicating that other condensing vapours are responsible for the majority of particle growth, as well as the differing growth rates between the two sites. Results also show that the condensation sink (CS) does not play a relevant role in NPF processes at both sites and points to the availability of volatile organic compounds (VOCs) as one of the main factors controlling the NPF events at both sites. Finally, a closer analysis of the NPF events that were observed at the SNS site during a Saharan dust episode that occurred during the field campaign was carried out, evidencing the role of TiO2 and F2O3 together with VOCs in promoting new particle formation during this dust intrusion event. Although further investigation is needed to improve our understanding in this topic, this result suggests that climate effects of mineral dust and NPF are not disconnected from each other as it was commonly thought. Therefore, since mineral dust contributes to a major fraction of the global aerosol mass load, dust–NPF interaction should be taken into account in global aerosol-climate modelling for better climate change prediction.

The uptake of water by atmospheric aerosols has a pronounced effect on particle light scattering properties, which in turn are strongly dependent on the ambient relative humidity (RH). Earth system models need to account for the aerosol water uptake and its influence on light scattering in order to properly capture the overall radiative effects of aerosols. Here we present a comprehensive model–measurement evaluation of the particle light scattering enhancement factor f(RH), defined as the particle light scattering coefficient at elevated RH (here set to 85 %) divided by its dry value. The comparison uses simulations from 10 Earth system models and a global dataset of surface-based in situ measurements. In general, we find a large diversity in the magnitude of predicted f(RH) amongst the different models, which can not be explained by the site types. Based on our evaluation of sea salt scattering enhancement and simulated organic mass fraction, there is a strong indication that differences in the model parameterizations of hygroscopicity and model chemistry are driving at least some of the observed diversity in simulated f(RH). Additionally, a key point is that defining dry conditions is difficult from an observational point of view and, depending on the aerosol, may influence the measured f(RH). The definition of dry also impacts our model evaluation, because several models exhibit significant water uptake between RH = 0 % and 40 %. The multisite average ratio between model outputs and measurements is 1.64 when RH = 0 % is assumed as the model dry RH and 1.16 when RH = 40 % is the model dry RH value. The overestimation by the models is believed to originate from the hygroscopicity parameterizations at the lower RH range which may not implement all phenomena taking place (i.e., not fully dried particles and hysteresis effects). This will be particularly relevant when a location is dominated by a deliquescent aerosol such as sea salt. Our results emphasize the need to consider the measurement conditions in such comparisons and recognize that measurements referred to as dry may not be dry in model terms. Recommendations for future model–measurement evaluation and model improvements are provided.

A stand-alone lidar-based method for detecting airborne hazards for aviation in near real time (NRT) is presented. A polarization lidar allows for the identification of irregular-shaped particles such as volcanic dust and desert dust. The Single Calculus Chain (SCC) of the European Aerosol Research Lidar Network (EARLINET) delivers high-resolution preprocessed data: the calibrated total attenuated backscatter and the calibrated volume linear depolarization ratio time series. From these calibrated lidar signals, the particle backscatter coefficient and the particle depolarization ratio can be derived in temporally high resolution and thus provide the basis of the NRT early warning system (EWS). In particular, an iterative method for the retrieval of the particle backscatter is implemented. This improved capability was designed as a pilot that will produce alerts for imminent threats for aviation. The method is applied to data during two diverse aerosol scenarios: first, a record breaking desert dust intrusion in March 2018 over Finokalia, Greece, and, second, an intrusion of volcanic particles originating from Mount Etna, Italy, in June 2019 over Antikythera, Greece. Additionally, a devoted observational period including several EARLINET lidar systems demonstrates the network's preparedness to offer insight into natural hazards that affect the aviation sector.

Aerosol particles are essential constituents of the Earth's atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.

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.

This study evaluates the potential of the GRASP algorithm (Generalized Retrieval of Aerosol and Surface Properties) to retrieve continuous day-to-night aerosol properties, both column-integrated and vertically resolved. The study is focused on the evaluation of GRASP retrievals during an intense Saharan dust event that occurred during the Sierra Nevada Lidar aerOsol Profiling Experiment I (SLOPE I) field campaign. For daytime aerosol retrievals, we combined the measurements of the ground-based lidar from EARLINET (European Aerosol Research Lidar Network) station and sun–sky photometer from AERONET (Aerosol Robotic Network), both instruments co-located in Granada (Spain). However, for night-time retrievals three different combinations of active and passive remote-sensing measurements are proposed. The first scheme (N0) uses lidar night-time measurements in combination with the interpolation of sun–sky daytime measurements. The other two schemes combine lidar night-time measurements with night-time aerosol optical depth obtained by lunar photometry either using intensive properties of the aerosol retrieved during sun–sky daytime measurements (N1) or using the Moon aureole radiance obtained by sky camera images (N2). Evaluations of the columnar aerosol properties retrieved by GRASP are done versus standard AERONET retrievals. The coherence of day-to-night evolutions of the different aerosol properties retrieved by GRASP is also studied. The extinction coefficient vertical profiles retrieved by GRASP are compared with the profiles calculated by the Raman technique at night-time with differences below 30 % for all schemes at 355, 532 and 1064 nm. Finally, the volume concentration and scattering coefficient retrieved by GRASP at 2500 m a.s.l. are evaluated by in situ measurements at this height at Sierra Nevada Station. The differences between GRASP and in situ measurements are similar for the different schemes, with differences below 30 % for both volume concentration and scattering coefficient. In general, for the scattering coefficient, the GRASP N0 and N1 show better results than the GRASP N2 schemes, while for volume concentration, GRASP N2 shows the lowest differences against in situ measurements (around 10 %) for high aerosol optical depth values.

The lowest region of the troposphere is a turbulent layer known as the atmospheric boundary layer (ABL) and characterized by high daily variability due to the influence of surface forcings. This is the reason why detecting systems with high spatial and temporal resolution, such as lidar, have been widely applied for researching this region. In this paper, we present a comparative analysis on the use of lidar-backscattered signals at three wavelengths (355, 532 and 1064 nm) to study the ABL by investigating the high-order moments, which give us information about the ABL height (derived by the variance method), aerosol layer movement (skewness) and mixing conditions (kurtosis) at several heights. Previous studies have shown that the 1064 nm wavelength, due to the predominance of particle signature in the total backscattered atmospheric signal and practically null presence of molecular signal (which can represent noise in high-order moments), provides an appropriate description of the turbulence field, and thus in this study it was considered a reference. We analyze two case studies that show us that the backscattered signal at 355 nm, even after applying some corrections, has a limited applicability for turbulence studies using the proposed methodology due to the strong contribution of the molecular signature to the total backscatter signal. This increases the noise associated with the high-order profiles and, consequently, generates misinformation. On the other hand, the information on the turbulence field derived from the backscattered signal at 532 nm is similar to that obtained at 1064 nm due to the appropriate attenuation of the noise, generated by molecular component of backscattered signal by the application of the corrections proposed.

An experimental setup to study aerosol hygroscopicity is proposed based on the temporal evolution of attenuated backscatter coefficients from a ceilometer colocated with an instrumented tower equipped with meteorological sensors at different heights. This setup is used to analyze a 4.5-year database at the ACTRIS SIRTA observatory in Palaiseau (Paris, France, 2.208∘ E, 48.713∘ N; 160 m above sea level). A strict criterion-based procedure has been established to identify hygroscopic growth cases using ancillary information, such as online chemical composition, resulting in 8 hygroscopic growth cases from a total of 107 potential cases. For these eight cases, hygroscopic growth-related properties, such as the attenuated backscatter enhancement factor fβ (RH) and the hygroscopic growth coefficient γ, are evaluated. This study shows that the hygroscopicity parameter γ is negatively correlated with the aerosol organic mass fraction but shows a positive correlation with the aerosol inorganic mass fraction. Among inorganic species, nitrate exhibited the highest correlation. This is the first time that hygroscopic enhancement factors are directly retrieved under ambient aerosols using remote-sensing techniques, which are combined with online chemical composition in situ measurements to evaluate the role of the different aerosol species in aerosol hygroscopicity.

Aerosol radiative properties are investigated in southeastern Spain during a dust event on 16–17 June 2013 in the framework of the ChArMEx/ADRIMED (Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) campaign. Particle optical and microphysical properties from ground-based sun/sky photometer and lidar measurements, as well as in situ measurements on board the SAFIRE ATR 42 French research aircraft, are used to create a set of different levels of input parameterizations, which feed the 1-D radiative transfer model (RTM) GAME (Global Atmospheric ModEl). We consider three datasets: (1) a first parameterization based on the retrievals by an advanced aerosol inversion code (GRASP; Generalized Retrieval of Aerosol and Surface Properties) applied to combined photometer and lidar data, (2) a parameterization based on the photometer columnar optical properties and vertically resolved lidar retrievals with the two-component Klett–Fernald algorithm, and (3) a parameterization based on vertically resolved optical and microphysical aerosol properties measured in situ by the aircraft instrumentation. Once retrieved, the outputs of the RTM in terms of both shortwave and longwave radiative fluxes are compared against ground and in situ airborne measurements. In addition, the outputs of the model in terms of the aerosol direct radiative effect are discussed with respect to the different input parameterizations. Results show that calculated atmospheric radiative fluxes differ no more than 7 % from the measured ones. The three parameterization datasets produce a cooling effect due to mineral dust both at the surface and the top of the atmosphere. Aerosol radiative effects with differences of up to 10 W m−2 in the shortwave spectral range (mostly due to differences in the aerosol optical depth) and 2 W m−2 for the longwave spectral range (mainly due to differences in the aerosol optical depth but also to the coarse mode radius used to calculate the radiative properties) are obtained when comparing the three parameterizations. The study reveals the complexity of parameterizing 1-D RTMs as sizing and characterizing the optical properties of mineral dust is challenging. The use of advanced remote sensing data and processing, in combination with closure studies on the optical and microphysical properties from in situ aircraft measurements when available, is recommended.

The planetary boundary layer (PBL) is the lowermost region of troposphere and is endowed with turbulent characteristics, which can have mechanical and/or thermodynamic origins. This behavior gives this layer great importance, mainly in studies about pollutant dispersion and weather forecasting. However, the instruments usually applied in studies of turbulence in the PBL have limitations in spatial resolution (anemometer towers) or temporal resolution (instrumentation aboard an aircraft). Ground-based remote sensing, both active and passive, offers an alternative for studying the PBL. In this study we show the capabilities of combining different remote sensing systems (microwave radiometer – MWR, Doppler lidar – DL – and elastic lidar – EL) for retrieving a detailed picture on the PBL turbulent features. The statistical moments of the high frequency distributions of the vertical wind velocity, derived from DL, and of the backscattered coefficient, derived from EL, are corrected by two methodologies, namely first lag correction and -2/3 law correction. The corrected profiles, obtained from DL data, present small differences when compared with the uncorrected profiles, showing the low influence of noise and the viability of the proposed methodology. Concerning EL, in addition to analyzing the influence of noise, we explore the use of different wavelengths that usually include EL systems operated in extended networks, like the European Aerosol Research Lidar Network (EARLINET), Latin American Lidar Network (LALINET), NASA Micro-Pulse Lidar Network (MPLNET) or Skyradiometer Network (SKYNET). In this way we want to show the feasibility of extending the capability of existing monitoring networks without strong investments or changes in their measurements protocols. Two case studies were analyzed in detail, one corresponding to a well-defined PBL and another corresponding to a situation with presence of a Saharan dust lofted aerosol layer and clouds. In both cases we discuss results provided by the different instruments showing their complementarity and the precautions to be applied in the data interpretation. Our study shows that the use of EL at 532 nm requires a careful correction of the signal using the first lag time correction in order to get reliable turbulence information on the PBL.

Soil erosion aerosols can be transported considerable distances, the Sahara being one of the major sources in the world. In June 2016 the volume scattering function of the atmospheric aerosol was determined in the Sierra Nevada, Spain, at an altitude of 2500 m. Measurements were performed with a polar nephelometer permitting measurements between scattering angles of 5 to 175∘. The values at the missing angles could be estimated to a high accuracy, using the shape of the scattering function adjacent to the missing angles, and thus a complete volume scattering function was available. During the measuring period intrusions of long-range transported Sahara aerosol happened several times. The classification of the aerosol was done by back trajectories and by the Angström exponent of the wavelength-dependent scattering coefficient, which was determined by a three-wavelength Integrating Nephelometer. The phase function of the Sahara aerosol had a stronger forward scattering, and less backscattering compared to the non-Sahara aerosol, which is in agreement with other findings for irregular particles. The asymmetry parameter of the phase function is the best characteristic to distinguish Sahara aerosol from non-Sahara aerosol. In this study the asymmetry parameter for the Sahara aerosol was larger than 0.65, whereas the non-Sahara aerosol had an asymmetry parameter below 0.6. A comparison with measurements performed with long-range transported Gobi desert aerosols observed in Kyoto, Japan, showed very similar results.

We present an automatic aerosol classification method based solely on the European Aerosol Research Lidar Network (EARLINET) intensive optical parameters with the aim of building a network-wide classification tool that could provide near-real-time aerosol typing information. The presented method depends on a supervised learning technique and makes use of the Mahalanobis distance function that relates each unclassified measurement to a predefined aerosol type. As a first step (training phase), a reference dataset is set up consisting of already classified EARLINET data. Using this dataset, we defined 8 aerosol classes: clean continental, polluted continental, dust, mixed dust, polluted dust, mixed marine, smoke, and volcanic ash. The effect of the number of aerosol classes has been explored, as well as the optimal set of intensive parameters to separate different aerosol types. Furthermore, the algorithm is trained with literature particle linear depolarization ratio values. As a second step (testing phase), we apply the method to an already classified EARLINET dataset and analyze the results of the comparison to this classified dataset. The predictive accuracy of the automatic classification varies between 59 % (minimum) and 90 % (maximum) from 8 to 4 aerosol classes, respectively, when evaluated against pre-classified EARLINET lidar. This indicates the potential use of the automatic classification to all network lidar data. Furthermore, the training of the algorithm with particle linear depolarization values found in the literature further improves the accuracy with values for all the aerosol classes around 80 %. Additionally, the algorithm has proven to be highly versatile as it adapts to changes in the size of the training dataset and the number of aerosol classes and classifying parameters. Finally, the low computational time and demand for resources make the algorithm extremely suitable for the implementation within the single calculus chain (SCC), the EARLINET centralized processing suite.

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.

This study focuses on the analysis of aerosol hygroscopic growth during the Sierra Nevada Lidar AerOsol Profiling Experiment (SLOPE I) campaign by using the synergy of active and passive remote sensors at the ACTRIS Granada station and in situ instrumentation at a mountain station (Sierra Nevada, SNS). To this end, a methodology based on simultaneous measurements of aerosol profiles from an EARLINET multi-wavelength Raman lidar (RL) and relative humidity (RH) profiles obtained from a multi-instrumental approach is used. This approach is based on the combination of calibrated water vapor mixing ratio (r) profiles from RL and continuous temperature profiles from a microwave radiometer (MWR) for obtaining RH profiles with a reasonable vertical and temporal resolution. This methodology is validated against the traditional one that uses RH from co-located radiosounding (RS) measurements, obtaining differences in the hygroscopic growth parameter (γ) lower than 5 % between the methodology based on RS and the one presented here. Additionally, during the SLOPE I campaign the remote sensing methodology used for aerosol hygroscopic growth studies has been checked against Mie calculations of aerosol hygroscopic growth using in situ measurements of particle number size distribution and submicron chemical composition measured at SNS. The hygroscopic case observed during SLOPE I showed an increase in the particle backscatter coefficient at 355 and 532 nm with relative humidity (RH ranged between 78 and 98 %), but also a decrease in the backscatter-related Ångström exponent (AE) and particle linear depolarization ratio (PLDR), indicating that the particles became larger and more spherical due to hygroscopic processes. Vertical and horizontal wind analysis is performed by means of a co-located Doppler lidar system, in order to evaluate the horizontal and vertical dynamics of the air masses. Finally, the Hänel parameterization is applied to experimental data for both stations, and we found good agreement on γ measured with remote sensing (γ532 = 0.48 ± 0.01 and γ355 = 0.40 ± 0.01) with respect to the values calculated using Mie theory (γ532 = 0.53 ± 0.02 and γ355 = 0.45 ± 0.02), with relative differences between measurements and simulations lower than 9 % at 532 nm and 11 % at 355 nm.

Particle depolarization ratio retrieved from lidar measurements are commonly used for aerosol-typing studies, microphysical inversion, or mass concentration retrievals. The particle depolarization ratio is one of the primary parameters that can differentiate several major aerosol components but only if the measurements are accurate enough. The accuracy related to the retrieval of particle depolarization ratios is the driving factor for assessing and improving the uncertainties of the depolarization products. This paper presents different depolarization calibration procedures used to improve the quality of the depolarization data. The results illustrate a significant improvement of the depolarization lidar products for all the selected lidar stations that have implemented depolarization calibration procedures. The calibrated volume and particle depolarization profiles at 532 nm show values that fall within a range that is generally accepted in the literature.

In this study, vertical profiles and column-integrated aerosol properties retrieved by the GRASP (Generalized Retrieval of Atmosphere and Surface Properties) algorithm are evaluated with in situ airborne measurements made during the ChArMEx-ADRIMED field campaign in summer 2013. In the framework of this campaign, two different flights took place over Granada (Spain) during a desert dust episode on 16 and 17 June. The GRASP algorithm, which combines lidar and sun–sky photometer data measured at Granada, was used to retrieve aerosol properties. Two sun-photometer datasets are used: one co-located with the lidar system and the other in the Cerro Poyos station, approximately 1200 m higher than the lidar system but at a short horizontal distance. Column-integrated aerosol microphysical properties retrieved by GRASP are compared with AERONET products showing a good agreement. Differences between GRASP retrievals and airborne extinction profiles are in the range of 15 to 30 %, depending on the instrument on board the aircraft used as reference. On 16 June, a case where the dust layer was coupled to the aerosol layer close to surface, the total volume concentration differences between in situ data and GRASP retrieval are 15 and 36 % for Granada and Cerro Poyos retrievals, respectively. In contrast, on 17 June the dust layer was decoupled from the aerosol layer close to the surface, and the differences are around 17 % for both retrievals. In general, all the discrepancies found are within the uncertainly limits, showing the robustness and reliability of the GRASP algorithm. However, the better agreement found for the Cerro Poyos retrieval with the aircraft data and the vertical homogeneity of certain properties retrieved with GRASP, such as the scattering Ångström exponent, for cases with aerosol layers characterized by different aerosol types, shows that uncertainties in the vertical distribution of the aerosol properties have to be considered. The comparison presented here between GRASP and other algorithms (i.e. AERONET and LIRIC) and with airborne in situ measurements shows the potential to retrieve the optical and microphysical profiles of the atmospheric aerosol properties. Also, the advantage of GRASP versus LIRIC is that GRASP does not assume the results of the AERONET inversion as a starting point.

The interest in the use of ceilometers for optical aerosol characterization has increased in the last few years. They operate continuously almost unattended and are also much less expensive than lidars; hence, they can be distributed in dense networks over large areas. However, due to the low signal-to-noise ratio it is not always possible to obtain particle backscatter coefficient profiles, and the vast number of data generated require an automated and unsupervised method that ensures the quality of the profiles inversions. In this work we describe a method that uses aerosol optical depth (AOD) measurements from the AERONET network that it is applied for the calibration and automated quality assurance of inversion of ceilometer profiles. The method is compared with independent inversions obtained by co-located multiwavelength lidar measurements. A difference smaller than 15 % in backscatter is found between both instruments. This method is continuously and automatically applied to the Iberian Ceilometer Network (ICENET) and a case example during an unusually intense dust outbreak affecting the Iberian Peninsula between 20 and 24 February 2016 is shown. Results reveal that it is possible to obtain quantitative optical aerosol properties (particle backscatter coefficient) and discriminate the quality of these retrievals with ceilometers over large areas. This information has a great potential for alert systems and model assimilation and evaluation.

The automatic and non-supervised detection of the planetary boundary layer height (zPBL) by means of lidar measurements was widely investigated during the last several years. Despite considerable advances, the experimental detection still presents difficulties such as advected aerosol layers coupled to the planetary boundary layer (PBL) which usually produces an overestimation of the zPBL. To improve the detection of the zPBL in these complex atmospheric situations, we present a new algorithm, called POLARIS (PBL height estimation based on lidar depolarisation). POLARIS applies the wavelet covariance transform (WCT) to the range-corrected signal (RCS) and to the perpendicular-to-parallel signal ratio (δ) profiles. Different candidates for zPBL are chosen and the selection is done based on the WCT applied to the RCS and δ. We use two ChArMEx (Chemistry-Aerosol Mediterranean Experiment) campaigns with lidar and microwave radiometer (MWR) measurements, conducted in 2012 and 2013, for the POLARIS' adjustment and validation. POLARIS improves the zPBL detection compared to previous methods based on lidar measurements, especially when an aerosol layer is coupled to the PBL. We also compare the zPBL provided by the Weather Research and Forecasting (WRF) numerical weather prediction (NWP) model with respect to the zPBL determined with POLARIS and the MWR under Saharan dust events. WRF underestimates the zPBL during daytime but agrees with the MWR during night-time. The zPBL provided by WRF shows a better temporal evolution compared to the MWR during daytime than during night-time.

Strong events of long-range transported biomass burning aerosol were detected during July 2013 at three EARLINET (European Aerosol Research Lidar Network) stations, namely Granada (Spain), Leipzig (Germany) and Warsaw (Poland). Satellite observations from MODIS (Moderate Resolution Imaging Spectroradiometer) and CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) instruments, as well as modeling tools such as HYSPLIT (Hybrid Single-Particle Lagrangian Integrated Trajectory) and NAAPS (Navy Aerosol Analysis and Prediction System), have been used to estimate the sources and transport paths of those North American forest fire smoke particles. A multiwavelength Raman lidar technique was applied to obtain vertically resolved particle optical properties, and further inversion of those properties with a regularization algorithm allowed for retrieving microphysical information on the studied particles. The results highlight the presence of smoke layers of 1–2 km thickness, located at about 5 km a.s.l. altitude over Granada and Leipzig and around 2.5 km a.s.l. at Warsaw. These layers were intense, as they accounted for more than 30 % of the total AOD (aerosol optical depth) in all cases, and presented optical and microphysical features typical for different aging degrees: color ratio of lidar ratios (LR532 ∕ LR355) around 2, α-related ångström exponents of less than 1, effective radii of 0.3 µm and large values of single scattering albedos (SSA), nearly spectrally independent. The intensive microphysical properties were compared with columnar retrievals form co-located AERONET (Aerosol Robotic Network) stations. The intensity of the layers was also characterized in terms of particle volume concentration, and then an experimental relationship between this magnitude and the particle extinction coefficient was established.

The effects of atmospheric aerosol particles on the Earth's climate mainly depend on their optical, microphysical and chemical properties, which modify the Earth's radiative budget. The aerosol radiative effects can be divided into direct and semi-direct effects, produced by the aerosol–radiation interactions (ARIs), and indirect effects, produced by aerosol–cloud interactions (ACIs). In this sense the objective of this work is to assess whether the inclusion of aerosol radiative feedbacks in the online coupled WRF-Chem model improves the modelling outputs over the Iberian Peninsula (IP) and surrounding water areas. For this purpose, the methodology is based on the evaluation of modelled aerosol optical properties under different simulation scenarios. The evaluated data come from two WRF-Chem simulations for the IP differing in the inclusion/no-inclusion of ARIs and ACIs (RF/NRF simulations). The case studies cover two episodes with different aerosol types over the IP in 2010, namely a Saharan dust outbreak and a forest fire episode. The evaluation uses observational data from AERONET (Aerosol Robotic Network) stations and MODIS (Moderate Resolution Imaging Spectroradiometer) sensor, including aerosol optical depth (AOD) and Ångström exponent (AE). Experimental data of aerosol vertical distribution from the EARLINET (European Aerosol Research Lidar Network) Granada station are used for checking the models. The results indicate that for the spatial distribution the best-represented variable is AOD and the largest improvements when including the aerosol radiative feedbacks are found for the vertical distribution. In the case of the dust outbreak, a slight improvement (worsening) is produced over the areas with medium (high/low) levels of AOD(−9 % / +12 % of improvement) when including the aerosol radiative feedbacks. For the wildfire episode, improvements of AOD representation (up to 11 %) over areas further away from emission sources are estimated, which compensates for the computational effort of including aerosol feedbacks in the simulations. No clear improvement is observed for the AE representation, the variability of which is largely underpredicted by both simulations.

Lidar depolarization measurements distinguish between spherical and non-spherical aerosol particles based on the change of the polarization state between the emitted and received signal. The particle shape information in combination with other aerosol optical properties allows the characterization of different aerosol types and the retrieval of aerosol particle microphysical properties. Regarding the microphysical inversions, the lidar depolarization technique is becoming a key method since particle shape information can be used by algorithms based on spheres and spheroids, optimizing the retrieval procedure. Thus, the identification of the depolarization error sources and the quantification of their effects are crucial. This work presents a new tool to assess the systematic error of the volume linear depolarization ratio (δ), combining the Stokes–Müller formalism and the complete sampling of the error space using the lidar model presented in Freudenthaler (2016a). This tool is applied to a synthetic lidar system and to several EARLINET lidars with depolarization capabilities at 355 or 532 nm. The lidar systems show relative errors of δ larger than 100 % for δ values around molecular linear depolarization ratios (∼ 0.004 and up to ∼ 10 % for δ = 0.45). However, one system shows only relative errors of 25 and 0.22 % for δ = 0.004 and δ = 0.45, respectively, and gives an example of how a proper identification and reduction of the main error sources can drastically reduce the systematic errors of δ. In this regard, we provide some indications of how to reduce the systematic errors.

In the framework of the ChArMEx (the Chemistry-Aerosol Mediterranean Experiment; http://charmex.lsce.ipsl.fr/) program, the seasonal variability of the aerosol optical, microphysical and radiative properties derived from AERONET (Aerosol Robotic Network; http://aeronet.gsfc.nasa.gov/) is examined in two regional background insular sites in the western Mediterranean Basin: Ersa (Corsica Island, France) and Palma de Mallorca (Mallorca Island, Spain). A third site, Alborán (Alborán Island, Spain), with only a few months of data is considered for examining possible northeast–southwest (NE–SW) gradients of the aforementioned aerosol properties. The AERONET dataset is exclusively composed of level 2.0 inversion products available during the 5-year period 2011–2015. AERONET solar radiative fluxes are compared with ground- and satellite-based flux measurements. To the best of our knowledge this is the first time that AERONET fluxes are compared with measurements at the top of the atmosphere. Strong events (with an aerosol optical depth at 440 nm greater than 0.4) of long-range transport aerosols, one of the main drivers of the observed annual cycles and NE–SW gradients, are (1) mineral dust outbreaks predominant in spring and summer in the north and in summer in the south and (2) European pollution episodes predominant in autumn. A NE–SW gradient exists in the western Mediterranean Basin for the aerosol optical depth and especially its coarse-mode fraction, which all together produces a similar gradient for the aerosol direct radiative forcing. The aerosol fine mode is rather homogeneously distributed. Absorption properties are quite variable because of the many and different sources of anthropogenic particles in and around the western Mediterranean Basin: North African and European urban areas, the Iberian and Italian peninsulas, most forest fires and ship emissions. As a result, the aerosol direct forcing efficiency, more dependent to absorption than the absolute forcing, has no marked gradient.

The simultaneous analysis of aerosol microphysical properties profiles at different European stations is made in the framework of the ChArMEx/EMEP 2012 field campaign (9–11 July 2012). During and in support of this campaign, five lidar ground-based stations (Athens, Barcelona, Bucharest, Évora, and Granada) performed 72 h of continuous lidar measurements and collocated and coincident sun-photometer measurements. Therefore it was possible to retrieve volume concentration profiles with the Lidar Radiometer Inversion Code (LIRIC). Results indicated the presence of a mineral dust plume affecting the western Mediterranean region (mainly the Granada station), whereas a different aerosol plume was observed over the Balkans area. LIRIC profiles showed a predominance of coarse spheroid particles above Granada, as expected for mineral dust, and an aerosol plume composed mainly of fine and coarse spherical particles above Athens and Bucharest. Due to the exceptional characteristics of the ChArMEx database, the analysis of the microphysical properties profiles' temporal evolution was also possible. An in-depth analysis was performed mainly at the Granada station because of the availability of continuous lidar measurements and frequent AERONET inversion retrievals. The analysis at Granada was of special interest since the station was affected by mineral dust during the complete analyzed period. LIRIC was found to be a very useful tool for performing continuous monitoring of mineral dust, allowing for the analysis of the dynamics of the dust event in the vertical and temporal coordinates. Results obtained here illustrate the importance of having collocated and simultaneous advanced lidar and sun-photometer measurements in order to characterize the aerosol microphysical properties in both the vertical and temporal coordinates at a regional scale. In addition, this study revealed that the use of the depolarization information as input in LIRIC in the stations of Bucharest, Évora, and Granada was crucial for the characterization of the aerosol types and their distribution in the vertical column, whereas in stations lacking depolarization lidar channels, ancillary information was needed. Results obtained were also used for the validation of different mineral dust models. In general, the models better forecast the vertical distribution of the mineral dust than the column-integrated mass concentration, which was underestimated in most of the cases.

This paper introduces the recent European Aerosol Research Lidar Network (EARLINET) quality-assurance efforts at instrument level. Within two dedicated campaigns and five single-site intercomparison activities, 21 EARLINET systems from 18 EARLINET stations were intercompared between 2009 and 2013. A comprehensive strategy for campaign setup and data evaluation has been established. Eleven systems from nine EARLINET stations participated in the EARLINET Lidar Intercomparison 2009 (EARLI09). In this campaign, three reference systems were qualified which served as traveling standards thereafter. EARLINET systems from nine other stations have been compared against these reference systems since 2009. We present and discuss comparisons at signal and at product level from all campaigns for more than 100 individual measurement channels at the wavelengths of 355, 387, 532, and 607 nm. It is shown that in most cases, a very good agreement of the compared systems with the respective reference is obtained. Mean signal deviations in predefined height ranges are typically below ±2 %. Particle backscatter and extinction coefficients agree within ±2 × 10−4 km−1 sr−1 and ± 0.01 km−1, respectively, in most cases. For systems or channels that showed larger discrepancies, an in-depth analysis of deficiencies was performed and technical solutions and upgrades were proposed and realized. The intercomparisons have reinforced confidence in the EARLINET data quality and allowed us to draw conclusions on necessary system improvements for some instruments and to identify major challenges that need to be tackled in the future.

In this work we present an analysis of aerosol microphysical properties during a mineral dust event taking advantage of the combination of different state-of-the-art retrieval techniques applied to active and passive remote sensing measurements and the evaluation of some of those techniques using independent data acquired from in situ aircraft measurements. Data were collected in a field campaign performed during a mineral dust outbreak at the Granada, Spain, experimental site (37.16° N, 3.61° W, 680 m a.s.l.) on 27 June 2011. Column-integrated properties are provided by sun- and star-photometry, which allows for a continuous evaluation of the mineral dust optical properties during both day and nighttime. Both the linear estimation and AERONET (Aerosol Robotic Network) inversion algorithms are applied for the retrieval of the column-integrated microphysical particle properties. In addition, vertically resolved microphysical properties are obtained from a multi-wavelength Raman lidar system included in EARLINET (European Aerosol Research Lidar Network), by using both LIRIC (Lidar Radiometer Inversion Code) algorithm during daytime and an algorithm applied to the Raman measurements based on the regularization technique during nighttime. LIRIC retrievals reveal the presence of dust layers between 3 and 5 km a.s.l. with volume concentrations of the coarse spheroid mode up to 60 µm3 cm−3. The combined use of the regularization and LIRIC methods reveals the night-to-day evolution of the vertical structure of the mineral dust microphysical properties and offers complementary information to that from column-integrated variables retrieved from passive remote sensing. Additionally, lidar depolarization profiles and LIRIC retrieved volume concentration are compared with aircraft in situ measurements. This study presents for the first time a comparison of the total volume concentration retrieved with LIRIC with independent in situ measurements, obtaining agreement within the estimated uncertainties for both methods and quite good agreement for the vertical distribution of the aerosol layers. Regarding the depolarization, the first published data set of the CAS-POL for polarization ratios is presented here and qualitatively compared with the lidar technique.

This paper presents the new photometer CE318-T, able to perform daytime and night-time photometric measurements using the sun and the moon as light source. Therefore, this new device permits a complete cycle of diurnal aerosol and water vapour measurements valuable to enhance atmospheric monitoring to be extracted. In this study we have found significantly higher precision of triplets when comparing the CE318-T master instrument and the Cimel AErosol RObotic NETwork (AERONET) master (CE318-AERONET) triplets as a result of the new CE318-T tracking system. Regarding the instrument calibration, two new methodologies to transfer the calibration from a reference instrument using only daytime measurements (Sun Ratio and Sun-Moon gain factor techniques) are presented and discussed. These methods allow the reduction of the previous complexities inherent to nocturnal calibration. A quantitative estimation of CE318-T AOD uncertainty by means of error propagation theory during daytime revealed AOD uncertainties (uDAOD) for Langley-calibrated instruments similar to the expected values for other reference instruments (0.002–0.009). We have also found uDAOD values similar to the values reported in sun photometry for field instruments ( ∼ 0.015). In the case of the night-time period, the CE318-T-estimated standard combined uncertainty (uNAOD) is dependent not only on the calibration technique but also on illumination conditions and the instrumental noise. These values range from 0.011–0.018 for Lunar Langley-calibrated instruments to 0.012–0.021 for instruments calibrated using the Sun Ratio technique. In the case of moon-calibrated instruments using the Sun-Moon gain factor method and sun-calibrated using the Langley technique, we found uNAOD ranging from 0.016 to 0.017 (up to 0.019 in 440 nm channel), not dependent on any lunar irradiance model.A subsequent performance evaluation including CE318-T and collocated measurements from independent reference instruments has served to assess the CE318-T performance as well as to confirm its estimated uncertainty. Daytime AOD evaluation, performed at Izaña station from March to June 2014, encompassed measurements from a reference CE318-T, a CE318-AERONET master instrument, a Precision Filter Radiometer (PFR) and a Precision Spectroradiometer (PSR) prototype, reporting low AOD discrepancies between the four instruments (up to 0.006). The nocturnal AOD evaluation was performed using CE318-T- and star-photometer-collocated measurements and also by means of a day/night coherence transition test using the CE318-T master instrument and the CE318 daytime data from the CE318-AERONET master instrument. Results showed low discrepancies with the star photometer at 870 and 500 nm channels ( ≤ 0.013) and differences with AERONET daytime data (1 h after and before sunset and sunrise) in agreement with the estimated uNAOD values at all illumination conditions in the case of channels within the visible spectral range, and only for high moon's illumination conditions in the case of near-infrared channels.Precipitable water vapour (PWV) validation showed a good agreement between CE318-T and Global Navigation Satellite System (GNSS) PWV values for all illumination conditions, within the expected precision for sun photometry.Finally, two case studies have been included to highlight the ability of the new CE318-T to capture the diurnal cycle of aerosols and water vapour as well as short-term atmospheric variations, critical for climate studies.

The CALIPSO Level 3 (CL3) product is the most recent data set produced by the observations of the Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument onboard the Cloud–Aerosol Lidar and Pathfinder Satellite Observations (CALIPSO) space platform. The European Aerosol Research Lidar Network (EARLINET), based mainly on multi-wavelength Raman lidar systems, is the most appropriate ground-based reference for CALIPSO calibration/validation studies on a continental scale. In this work, CALIPSO data are compared against EARLINET monthly averaged profiles obtained by measurements performed during CALIPSO overpasses. In order to mitigate uncertainties due to spatial and temporal differences, we reproduce a modified version of CL3 data starting from CALIPSO Level 2 (CL2) data. The spatial resolution is finer and nearly 2° × 2° (latitude × longitude) and only simultaneous measurements are used for ease of comparison. The CALIPSO monthly mean profiles following this approach are called CALIPSO Level 3*, CL3*. We find good agreement on the aerosol extinction coefficient, yet in most of the cases a small CALIPSO underestimation is observed with an average bias of 0.02 km−1 up to 4 km and 0.003 km−1 higher above. In contrast to CL3 standard product, the CL3* data set offers the possibility to assess the CALIPSO performance also in terms of the particle backscatter coefficient keeping the same quality assurance criteria applied to extinction profiles. The mean relative difference in the comparison improved from 25 % for extinction to 18 % for backscatter, showing better performances of CALIPSO backscatter retrievals. Additionally, the aerosol typing comparison yielded a robust identification of dust and polluted dust. Moreover, the CALIPSO aerosol-type-dependent lidar ratio selection is assessed by means of EARLINET observations, so as to investigate the performance of the extinction retrievals. The aerosol types of dust, polluted dust, and clean continental showed noticeable discrepancy. Finally, the potential improvements of the lidar ratio assignment have been examined by adjusting it according to EARLINET-derived values.

The Chemistry-Aerosol Mediterranean Experiment (ChArMEx; http://charmex.lsce.ipsl.fr) is a collaborative research program federating international activities to investigate Mediterranean regional chemistry-climate interactions. A special observing period (SOP-1a) including intensive airborne measurements was performed in the framework of the Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region (ADRIMED) project during the Mediterranean dry season over the western and central Mediterranean basins, with a focus on aerosol-radiation measurements and their modeling. The SOP-1a took place from 11 June to 5 July 2013. Airborne measurements were made by both the ATR-42 and F-20 French research aircraft operated from Sardinia (Italy) and instrumented for in situ and remote-sensing measurements, respectively, and by sounding and drifting balloons, launched in Minorca. The experimental setup also involved several ground-based measurement sites on islands including two ground-based reference stations in Corsica and Lampedusa and secondary monitoring sites in Minorca and Sicily. Additional measurements including lidar profiling were also performed on alert during aircraft operations at EARLINET/ACTRIS stations at Granada and Barcelona in Spain, and in southern Italy. Remote-sensing aerosol products from satellites (MSG/SEVIRI, MODIS) and from the AERONET/PHOTONS network were also used. Dedicated meso-scale and regional modeling experiments were performed in relation to this observational effort. We provide here an overview of the different surface and aircraft observations deployed during the ChArMEx/ADRIMED period and of associated modeling studies together with an analysis of the synoptic conditions that determined the aerosol emission and transport. Meteorological conditions observed during this campaign (moderate temperatures and southern flows) were not favorable to producing high levels of atmospheric pollutants or intense biomass burning events in the region. However, numerous mineral dust plumes were observed during the campaign, with the main sources located in Morocco, Algeria and Tunisia, leading to aerosol optical depth (AOD) values ranging between 0.2 and 0.6 (at 440 nm) over the western and central Mediterranean basins. One important point of this experiment concerns the direct observations of aerosol extinction onboard the ATR-42, using the CAPS system, showing local maxima reaching up to 150 M m−1 within the dust plume. Non-negligible aerosol extinction (about 50 M m−1) has also been observed within the marine boundary layer (MBL). By combining the ATR-42 extinction coefficient observations with absorption and scattering measurements, we performed a complete optical closure revealing excellent agreement with estimated optical properties. This additional information on extinction properties has allowed calculation of the dust single scattering albedo (SSA) with a high level of confidence over the western Mediterranean. Our results show a moderate variability from 0.90 to 1.00 (at 530 nm) for all flights studied compared to that reported in the literature on this optical parameter. Our results underline also a relatively low difference in SSA with values derived near dust sources. In parallel, active remote-sensing observations from the surface and onboard the F-20 aircraft suggest a complex vertical structure of particles and distinct aerosol layers with sea spray and pollution located within the MBL, and mineral dust and/or aged North American smoke particles located above (up to 6–7 km in altitude). Aircraft and balloon-borne observations allow one to investigate the vertical structure of the aerosol size distribution showing particles characterized by a large size (> 10 µm in diameter) within dust plumes. In most of cases, a coarse mode characterized by an effective diameter ranging between 5 and 10 µm, has been detected above the MBL. In terms of shortwave (SW) direct forcing, in situ surface and aircraft observations have been merged and used as inputs in 1-D radiative transfer codes for calculating the aerosol direct radiative forcing (DRF). Results show significant surface SW instantaneous forcing (up to −90 W m−2 at noon). Aircraft observations provide also original estimates of the vertical structure of SW and LW radiative heating revealing significant instantaneous values of about 5° K per day in the solar spectrum (for a solar angle of 30°) within the dust layer. Associated 3-D modeling studies from regional climate (RCM) and chemistry transport (CTM) models indicate a relatively good agreement for simulated AOD compared with observations from the AERONET/PHOTONS network and satellite data, especially for long-range dust transport. Calculations of the 3-D SW (clear-sky) surface DRF indicate an average of about −10 to −20 W m−2 (for the whole period) over the Mediterranean Sea together with maxima (−50 W m−2) over northern Africa. The top of the atmosphere (TOA) DRF is shown to be highly variable within the domain, due to moderate absorbing properties of dust and changes in the surface albedo. Indeed, 3-D simulations indicate negative forcing over the Mediterranean Sea and Europe and positive forcing over northern Africa. Finally, a multi-year simulation, performed for the 2003 to 2009 period and including an ocean–atmosphere (O–A) coupling, underlines the impact of the aerosol direct radiative forcing on the sea surface temperature, O–A fluxes and the hydrological cycle over the Mediterranean.

In the framework of ACTRIS (Aerosols, Clouds, and Trace Gases Research Infrastructure Network) summer 2012 measurement campaign (8 June–17 July 2012), EARLINET organized and performed a controlled exercise of feasibility to demonstrate its potential to perform operational, coordinated measurements and deliver products in near-real time. Eleven lidar stations participated in the exercise which started on 9 July 2012 at 06:00 UT and ended 72 h later on 12 July at 06:00 UT. For the first time, the single calculus chain (SCC) – the common calculus chain developed within EARLINET for the automatic evaluation of lidar data from raw signals up to the final products – was used. All stations sent in real-time measurements of a 1 h duration to the SCC server in a predefined netcdf file format. The pre-processing of the data was performed in real time by the SCC, while the optical processing was performed in near-real time after the exercise ended. 98 and 79 % of the files sent to SCC were successfully pre-processed and processed, respectively. Those percentages are quite large taking into account that no cloud screening was performed on the lidar data. The paper draws present and future SCC users' attention to the most critical parameters of the SCC product configuration and their possible optimal value but also to the limitations inherent to the raw data. The continuous use of SCC direct and derived products in heterogeneous conditions is used to demonstrate two potential applications of EARLINET infrastructure: the monitoring of a Saharan dust intrusion event and the evaluation of two dust transport models. The efforts made to define the measurements protocol and to configure properly the SCC pave the way for applying this protocol for specific applications such as the monitoring of special events, atmospheric modeling, climate research and calibration/validation activities of spaceborne observations.

Systematic measurements of dust concentration profiles at a continental scale were recently made possible by the development of synergistic retrieval algorithms using combined lidar and sun photometer data and the establishment of robust remote-sensing networks in the framework of Aerosols, Clouds, and Trace gases Research InfraStructure Network (ACTRIS)/European Aerosol Research Lidar Network (EARLINET). We present a methodology for using these capabilities as a tool for examining the performance of dust transport models. The methodology includes considerations for the selection of a suitable data set and appropriate metrics for the exploration of the results. The approach is demonstrated for four regional dust transport models (BSC-DREAM8b v2, NMMB/BSC-DUST, DREAMABOL, DREAM8-NMME-MACC) using dust observations performed at 10 ACTRIS/EARLINET stations. The observations, which include coincident multi-wavelength lidar and sun photometer measurements, were processed with the Lidar-Radiometer Inversion Code (LIRIC) to retrieve aerosol concentration profiles. The methodology proposed here shows advantages when compared to traditional evaluation techniques that utilize separately the available measurements such as separating the contribution of dust from other aerosol types on the lidar profiles and avoiding model assumptions related to the conversion of concentration fields to aerosol extinction values. When compared to LIRIC retrievals, the simulated dust vertical structures were found to be in good agreement for all models with correlation values between 0.5 and 0.7 in the 1–6 km range, where most dust is typically observed. The absolute dust concentration was typically underestimated with mean bias values of -40 to -20 μg m−3 at 2 km, the altitude of maximum mean concentration. The reported differences among the models found in this comparison indicate the benefit of the systematic use of the proposed approach in future dust model evaluation studies.

This work deals with the applicability of the linear estimation technique (LE) to invert spectral measurements of aerosol optical depth (AOD) provided by AERONET CIMEL sun photometers. The inversion of particle properties using only direct-sun AODs allows the evaluation of parameters such as effective radius (reff) and columnar volume aerosol content (V) with significantly better temporal resolution than the operational AERONET algorithm which requires both direct sun and sky radiance measurements. Sensitivity studies performed demonstrate that the constraints on the range of the inversion are very important to minimize the uncertainties, and therefore estimates of reff can be obtained with uncertainties less than 30 % and of V with uncertainties below 40 %. The LE technique is applied to data acquired at five AERONET sites influenced by different aerosol types and the retrievals are compared with the results of the operational AERONET code. Good agreement between the two techniques is obtained when the fine mode predominates, while for coarse mode cases the LE results systematically underestimate both reff and V. The highest differences are found for cases where no mode predominates. To minimize these biases, correction functions are developed using the multi-year database of observations at selected sites, where the AERONET retrieval is used as the reference. The derived corrections are tested using data from 18 other AERONET stations offering a range of aerosol types. After correction, the LE retrievals provide better agreement with AERONET for all the sites considered. Finally, the LE approach developed here is applied to AERONET and star-photometry measurements in the city of Granada (Spain) to obtain day-to-night time evolution of columnar aerosol microphysical properties.

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.

A new methodology based on combining active and passive remote sensing and simultaneous and collocated radiosounding data to study the aerosol hygroscopic growth effects on the particle optical and microphysical properties is presented. The identification of hygroscopic growth situations combines the analysis of multispectral aerosol particle backscatter coefficient and particle linear depolarization ratio with thermodynamic profiling of the atmospheric column. We analyzed the hygroscopic growth effects on aerosol properties, namely the aerosol particle backscatter coefficient and the volume concentration profiles, using data gathered at Granada EARLINET station. Two study cases, corresponding to different aerosol loads and different aerosol types, are used for illustrating the potential of this methodology. Values of the aerosol particle backscatter coefficient enhancement factors range from 2.1 ± 0.8 to 3.9 ± 1.5, in the ranges of relative humidity 60–90 and 40–83%, being similar to those previously reported in the literature. Differences in the enhancement factor are directly linked to the composition of the atmospheric aerosol. The largest value of the aerosol particle backscatter coefficient enhancement factor corresponds to the presence of sulphate and marine particles that are more affected by hygroscopic growth. On the contrary, the lowest value of the enhancement factor corresponds to an aerosol mixture containing sulphates and slight traces of mineral dust. The Hänel parameterization is applied to these case studies, obtaining results within the range of values reported in previous studies, with values of the γ exponent of 0.56 ± 0.01 (for anthropogenic particles slightly influenced by mineral dust) and 1.07 ± 0.01 (for the situation dominated by anthropogenic particles), showing the convenience of this remote sensing approach for the study of hygroscopic effects of the atmospheric aerosol under ambient unperturbed conditions. For the first time, the retrieval of the volume concentration profiles for these cases using the Lidar Radiometer Inversion Code (LIRIC) allows us to analyze the aerosol hygroscopic growth effects on aerosol volume concentration, observing a stronger increase of the fine mode volume concentration with increasing relative humidity.

A better understanding of aerosol radiative properties is a crucial challenge for climate change studies. This study aims at providing a complete characterization of aerosol radiative effects in different spectral ranges within the shortwave (SW) solar spectrum. For this purpose, long-term data sets of aerosol properties from six AERONET stations located in the Iberian Peninsula (southwestern Europe) have been analyzed in terms of climatological characterization and inter-annual changes. Aerosol information was used as input for the libRadtran model in order to determine the aerosol radiative effect (ARE) at the surface in the ultraviolet (AREUV), visible (AREVIS), near-infrared (ARENIR), and the entire SW range (ARESW) under cloud-free conditions. Over the whole Iberian Peninsula, yearly aerosol radiative effects in the different spectral ranges were found to be −1.1 < AREUV < −0.7, −5.7 < AREVIS < −3.5, −2.6 < ARENIR < −1.6, and −8.8 < ARESW < −5.7 (in W m−2). Monthly means of ARE showed a seasonal pattern with larger values in spring and summer. The aerosol forcing efficiency (AFE), ARE per unit of aerosol optical depth, has also been evaluated in the four spectral ranges. AFE exhibited a dependence on single scattering albedo as well as a weaker one on the Ångström exponent. AFE is larger (in absolute value) for small and absorbing particles. The contributions of the UV, VIS, and NIR ranges to the SW efficiency varied with the aerosol types. The predominant aerosol size determined the fractions AFEVIS/AFESW and AFENIR/AFESW. The AFEVIS was the dominant contributor for all aerosol types, although non-absorbing large particles caused more even contribution of VIS and NIR intervals. The AFEUV / AFESW ratio showed a higher value in the case of absorbing fine particles.

This paper presents a new application of assimilating lidar signals to aerosol forecasting. It aims at investigating the impact of a ground-based lidar network on the analysis and short-term forecasts of aerosols through a case study in the Mediterranean basin. To do so, we employ a data assimilation (DA) algorithm based on the optimal interpolation method developed in the Polair3D chemistry transport model (CTM) of the Polyphemus air quality modelling platform. We assimilate hourly averaged normalised range-corrected lidar signals (PR2) retrieved from a 72 h period of intensive and continuous measurements performed in July 2012 by ground-based lidar systems of the European Aerosol Research Lidar Network (EARLINET) integrated into the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) network and an additional system in Corsica deployed in the framework of the pre-ChArMEx (Chemistry-Aerosol Mediterranean Experiment)/TRAQA (TRAnsport à longue distance et Qualité de l'Air) campaign. This lidar campaign was dedicated to demonstrating the potential operationality of a research network like EARLINET and the potential usefulness of assimilation of lidar signals to aerosol forecasts. Particles with an aerodynamic diameter lower than 2.5 μm (PM2.5) and those with an aerodynamic diameter higher than 2.5 μm but lower than 10 μm (PM10–2.5) are analysed separately using the lidar observations at each DA step. First, we study the spatial and temporal influences of the assimilation of lidar signals on aerosol forecasting. We conduct sensitivity studies on algorithmic parameters, e.g. the horizontal correlation length (Lh) used in the background error covariance matrix (50 km, 100 km or 200 km), the altitudes at which DA is performed (0.75–3.5 km, 1.0–3.5 km or 1.5–3.5 km a.g.l.) and the assimilation period length (12 h or 24 h). We find that DA with Lh = 100 km and assimilation from 1.0 to 3.5 km a.g.l. during a 12 h assimilation period length leads to the best scores for PM10 and PM2.5 during the forecast period with reference to available measurements from surface networks. Secondly, the aerosol simulation results without and with lidar DA using the optimal parameters (Lh = 100 km, an assimilation altitude range from 1.0 to 3.5 km a.g.l. and a 12 h DA period) are evaluated using the level 2.0 (cloud-screened and quality-assured) aerosol optical depth (AOD) data from AERONET, and mass concentration measurements (PM10 or PM2.5) from the French air quality (BDQA) network and the EMEP-Spain/Portugal network. The results show that the simulation with DA leads to better scores than the one without DA for PM2.5, PM10and AOD. Additionally, the comparison of model results to evaluation data indicates that the temporal impact of assimilating lidar signals is longer than 36 h after the assimilation period.

The European Aerosol Research Lidar Network, EARLINET, was founded in 2000 as a research project for establishing a quantitative, comprehensive, and statistically significant database for the horizontal, vertical, and temporal distribution of aerosols on a continental scale. Since then EARLINET has continued to provide the most extensive collection of ground-based data for the aerosol vertical distribution over Europe. This paper gives an overview of the network's main developments since 2000 and introduces the dedicated EARLINET special issue, which reports on the present innovative and comprehensive technical solutions and scientific results related to the use of advanced lidar remote sensing techniques for the study of aerosol properties as developed within the network in the last 13 years. Since 2000, EARLINET has developed greatly in terms of number of stations and spatial distribution: from 17 stations in 10 countries in 2000 to 27 stations in 16 countries in 2013. EARLINET has developed greatly also in terms of technological advances with the spread of advanced multiwavelength Raman lidar stations in Europe. The developments for the quality assurance strategy, the optimization of instruments and data processing, and the dissemination of data have contributed to a significant improvement of the network towards a more sustainable observing system, with an increase in the observing capability and a reduction of operational costs. Consequently, EARLINET data have already been extensively used for many climatological studies, long-range transport events, Saharan dust outbreaks, plumes from volcanic eruptions, and for model evaluation and satellite data validation and integration. Future plans are aimed at continuous measurements and near-real-time data delivery in close cooperation with other ground-based networks, such as in the ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) www.actris.net, and with the modeling and satellite community, linking the research community with the operational world, with the aim of establishing of the atmospheric part of the European component of the integrated global observing system.