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Two layers of Saharan dust observed over Leipzig, Germany, in February and March 2021 were used to provide the first-ever lidar measurements of the dust lidar ratio (extinction-to-backscatter ratio) and linear depolarization ratio at all three classical lidar wavelengths (355, 532 and 1064 nm). The pure-dust conditions during the first event exhibit lidar ratios of 47 ± 8, 50 ± 5 and 69 ± 14 sr and particle linear depolarization ratios of 0.242 ± 0.024, 0.299 ± 0.018 and 0.206 ± 0.010 at wavelengths of 355, 532 and 1064 nm, respectively. The second, slightly polluted-dust case shows a similar spectral behavior of the lidar and depolarization ratio with values of the lidar ratio of 49 ± 4, 46 ± 5 and 57 ± 9 sr and the depolarization ratio of 0.174 ± 0.041, 0.298 ± 0.016 and 0.242 ± 0.007 at 355, 532 and 1064 nm, respectively. The results were compared with Aerosol Robotic Network (AERONET) version 3 (v3) inversion solutions and the Generalized Retrieval of Aerosol and Surface Properties (GRASP) at six and seven wavelengths. Both retrieval schemes make use of a spheroid shape model for mineral dust. The spectral slope of the lidar ratio from 532 to 1064 nm could be well reproduced by the AERONET and GRASP retrieval schemes. Higher lidar ratios in the UV were retrieved by AERONET and GRASP. The enhancement was probably caused by the influence of fine-mode pollution particles in the boundary layer which are included in the columnar photometer measurements. Significant differences between the measured and retrieved wavelength dependence of the particle linear depolarization ratio were found. The potential sources for these uncertainties are discussed.

An advanced multiwavelength polarization Raman lidar was operated aboard the icebreaker Polarstern during the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition to continuously monitor aerosol and cloud layers in the central Arctic up to 30 km height. The expedition lasted from September 2019 to October 2020 and measurements were mostly taken between 85 and 88.5∘ N. The lidar was integrated into a complex remote-sensing infrastructure aboard the Polarstern. In this article, novel lidar techniques, innovative concepts to study aerosol–cloud interaction in the Arctic, and unique MOSAiC findings will be presented. The highlight of the lidar measurements was the detection of a 10 km deep wildfire smoke layer over the North Pole region between 7–8 km and 17–18 km height with an aerosol optical thickness (AOT) at 532 nm of around 0.1 (in October–November 2019) and 0.05 from December to March. The dual-wavelength Raman lidar technique allowed us to unambiguously identify smoke as the dominating aerosol type in the aerosol layer in the upper troposphere and lower stratosphere (UTLS). An additional contribution to the 532 nm AOT by volcanic sulfate aerosol (Raikoke eruption) was estimated to always be lower than 15 %. The optical and microphysical properties of the UTLS smoke layer are presented in an accompanying paper (Ohneiser et al., 2021). This smoke event offered the unique opportunity to study the influence of organic aerosol particles (serving as ice-nucleating particles, INPs) on cirrus formation in the upper troposphere. An example of a closure study is presented to explain our concept of investigating aerosol–cloud interaction in this field. The smoke particles were obviously able to control the evolution of the cirrus system and caused low ice crystal number concentration. After the discussion of two typical Arctic haze events, we present a case study of the evolution of a long-lasting mixed-phase cloud layer embedded in Arctic haze in the free troposphere. The recently introduced dual-field-of-view polarization lidar technique was applied, for the first time, to mixed-phase cloud observations in order to determine the microphysical properties of the water droplets. The mixed-phase cloud closure experiment (based on combined lidar and radar observations) indicated that the observed aerosol levels controlled the number concentrations of nucleated droplets and ice crystals.

An advanced multiwavelength polarization Raman lidar was operated aboard the icebreaker Polarstern during the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition, lasting from September 2019 to October 2020, to contiuously monitor aerosol and cloud layers in the Central Arctic up to 30 km height at latitudes mostly between 85° N and 88.5° N. The lidar was integrated in a complex remote sensing infrastructure aboard Polarstern. Modern aerosol lidar methods and new lidar techniques and concepts to explore aerosol-cloud interaction were applied for the first time in the Central Arctic. Aim of the introductory article is to provide an overview of the observational spectrum of the lidar products for representative measurement cases. Highlight of the lidar measurements was the detection of a 10 km deep wildfire smoke layer over the North Pole area from, on average, 7 km to 17 km height with an aerosol optical thickness (AOT) at 532 nm around 0.1 (in October–November 2019) and 0.05 from December to mid of March 2020. The wildfire smoke was trapped within the extraordinarily strong polar vortex and remained detectable until the beginning of May 2020. Arctic haze was also monitored and characterized in terms of backscatter, extinction, and extinction-to-backscatter ratio at 355 and 532 nm. High lidar ratios from 60–100 sr in lofted mixed haze and smoke plumes are indicative for the presence of strongly light-absorbing fine-mode particles. The AOT at 532 nm was of the order of 0.025 for the tropospheric haze layers. In addition, so-called cloud closure experiments were applied to Arctic mixed-phase cloud and cirrus observations. The good match between cloud condensation nucleus concentration (CCNC) and cloud droplet number concentration (CDNC) and, on the other hand, between ice-nucleating particle concentration (INPC) and ice crystal number concentration (ICNC) indicated a clear influence of aerosol particles on the evolution of the cloud systems. CDNC was mostly between 20 and 100 cm−3 in the liquid-water dominated cloud top layer. ICNC was of the order of 0.1–1 L−1. The study of the impact of wildfire smoke particles on cirrus formation revealed that heterogeneous ice formation with smoke particles (organic aerosol particles) as INPs may have prevailed. ICNC values of 10–40 L−1 were clearly below ICNC levels that would indicate homogeneous freezing.

Saharan dust is a major natural atmospheric aerosol component with significant impact on the Earth radiation budget. In this work we determine the microphysical properties of dust particles after a long-range transport over the Atlantic Ocean, using input from three depolarization channels of a multi-wavelength polarization Raman lidar. The measurements were performed at Barbados in the framework of the Saharan Aerosol Long-Range Transport and Aerosol–Cloud-Interaction Experiment (SALTRACE) in the summers of 2013 and 2014. The microphysical retrievals are performed with the software tool SphInX (Spheroidal Inversion Experiments) which uses regularization for the inversion process and a new two-dimensional (2-D) extension of the Mie model approximating dust with spheroids. The method allows us to simultaneously retrieve shape- and size-dependent particle distributions. Because dust particles are mostly non-spherical this software tool fills the gap in estimating the non-spherical particle fraction. Two cases measured on 10 July 2013 and 20 June 2014 are discussed. 2-D radius-bimodal shape-size distribution are retrieved. The ratio of spherical-to-non-spherical contributions to the particle number concentration was found to be about 3/7. A volume-weighted effective aspect ratio of 1.1 was obtained, indicating slightly prolate particles. The total effective radius for the two cases in the preselected radius range from 0.01–2.2 μm was found to be, on average, 0.75 μm. The stronger dust event (10 July 2013) showed about 24 % higher values for the total surface-area and volume concentration. Finally, we compare our results with the ones from the polarization lidar-photometer networking (POLIPHON) method and ground-based photometers as well as with airborne in situ particle counters. Considering all differences in these independent approaches, we find a qualitatively good agreement between the different results and a consistent description of the dust cases. Such an extensive comparison is a novel and fruitful exercise and corroborates that the mathematical retrieval based on Raman lidar data of particle backscattering, extinction, and depolarization is a powerful tool even in the case of dust particles.

In this paper, we present long-term observations of the multiwavelength Raman lidar PollyXT conducted in the framework of the DACAPO-PESO campaign. Regardless the relatively clean atmosphere in the southern mid-latitude oceans region, we observed regularly events of long-range transported smoke, originating either from regional sources in South America or from Australia. Two case studies will be discussed. Both cases were identified as smoke events and they occurred on 5 February 2019 and 11 March 2019. 5 For the first case considered, the lofted smoke layer was located at an altitude between 1 and 4.2 km, and apart from the predominance of smoke particles, particle linear depolarization values indicated the presence of dust particles in the layer. Mean lidar ratio values at 355 and 532 nm were 49 ± 12 and 24 ± 18 sr respectively, while the mean particle linear depolarization was 7.6 ± 3.6 % at 532 nm. The advection of smoke and dust particles above Punta Arenas affected significantly the available CCN and INP in the lower troposphere, and triggered effectively ice crystal formation processes. Regarding the second case, the thin smoke layers were observed at altitudes between 5.5–7, 9 and 11 km. The particle linear depolarization ratio at 532 nm increased rapidly with height, starting from 2 % for the lowest two layers and increasing up to 9.5 % for the highest layer, indicating the possible presence of non-spherical coated soot aggregates. INP activation was effectively facilitated. The long-term analysis of the one year of observations showed that tropospheric smoke advection over Punta Arenas occurred 16 times (lasting from 1 to 17 hours), regularly distributed over the period and with high potential to influence cloud formation in the otherwise pristine environment of the region.

North Africa is the world’s largest source of dust, a large part of which is transported across the Atlantic to the Caribbean and beyond where it can impact radiation and clouds. Many aspects of this transport and its climate effects remain speculative. The Saharan Aerosol Long-Range Transport and Aerosol–Cloud-Interaction Experiment (SALTRACE; www.pa.op.dlr.de/saltrace) linked ground-based and airborne measurements with remote sensing and modeling techniques to address these issues in a program that took place in 2013/14. Specific objectives were to 1) characterize the chemical, microphysical, and optical properties of dust in the Caribbean, 2) quantify the impact of physical and chemical changes (“aging”) on the radiation budget and cloud microphysical processes, 3) investigate the meteorological context of transatlantic dust transport, and 4) assess the roles of removal processes during transport. SALTRACE was a German-led initiative involving scientists from Europe, Cabo Verde, the Caribbean, and the United States. The Falcon research aircraft of the Deutsches Zentrum für Luft- und Raumfahrt (DLR), equipped with a comprehensive aerosol and wind lidar payload, played a central role. Several major dust outbreaks were studied with 86 h of flight time under different conditions, making it by far the most extensive investigation on long-range transported dust ever made. This article presents an overview of SALTRACE and highlights selected results including data from transatlantic flights in coherent air masses separated by more than 4,000-km distance that enabled measurements of transport effects on dust properties. SALTRACE will improve our knowledge on the role of mineral dust in the climate system and provide data for studies on dust interactions with clouds, radiation, and health.

International audience; We present smoke lidar measurements from the Canadian fires of 2017. The advected smoke layers over Europe are detected at both tropospheric and stratospheric heights, with the latter presenting non-typical values of the Linear Particle Depolarization Ratio (LPDR) with strong wavelength dependence from the UV to the Near-IR. Specifically, the LPDR values are of the order of 22, 18 and 4% at 355, 532 and 1064 nm respectively. In an attempt to interpret these results, we apply the hypothesis that smoke particles have near-spherical and/or more complicated shapes. Scattering calculations with the T-matrix code revealed that the near-spherical shape is able to reproduce the observed LPDR and LR values of the stratospheric smoke particles at the three measurement wavelengths.; Nous présentons les mesures du lidar de fumée des incendies canadiens de 2017. Les couches de fumée advectées sur l'Europe sont détectées à la fois à des hauteurs troposphériques et stratosphériques, ces dernières présentant des valeurs atypiques du rapport de dépolarisation linéaire des particules (LPDR) avec une forte dépendance de longueur d'onde de l'UV au proche IR. Plus précisément, les valeurs LPDR sont de l'ordre de 22, 18 et 4% à 355, 532 et 1064 nm respectivement. Pour tenter d'interpréter ces résultats, nous appliquons l'hypothèse que les particules de fumée ont des formes quasi sphériques et/ou plus complexes. Les calculs de diffusion avec le code de la matrice T ont révélé que la forme quasi-sphérique est capable de reproduire les valeurs LPDR et LR observées des particules de fumée stratosphériques aux trois longueurs d'onde de mesure.

ATLID (“ATmospheric LIDar”) is the lidar to be flown on the multi-instrument Earth Clouds and Radiation Explorer (EarthCARE or ECARE) joint ESA/JAXA mission now scheduled for launch in 2022. ATID is a 3 channel linearly polarized High-Spectral Resolution (HSRL) system operating at 355nm. Cloud and aerosol optical properties are key ECARE products. This paper will provide an overview of the ATLID L2a (i.e. single instrument) retrieval algorithms being developed and implemented in order to derive cloud and aerosol optical properties.

The typical multiwavelength aerosol lidar data set for inversion of optical to microphysical parameters is composed of three backscatter coefficients (β) at 355, 532, and 1064 nm and two extinction coefficients (α) at 355 and 532 nm. This data combination is referred to as a 3β+2α or 3+2 data set. This set of data is sufficient for retrieving some important microphysical particle parameters if the particles have spherical shape. Here, we investigate the effect of including the particle linear depolarization ratio (δ) as a third input parameter for the inversion of lidar data. The inversion algorithm is generally not used if measurements show values of δ that exceed 0.10 at 532 nm, i.e. in the presence of non-spherical particles such as desert dust, volcanic ash, and, under special circumstances, biomass-burning smoke. We use experimental data collected with instruments that are capable of measuring δ at all three lidar wavelengths with an inversion routine that applies the spheroidal light-scattering model of Dubovik et al. (2006) with a fixed axis-ratio distribution to replicate scattering properties of non-spherical particles. The inversion gives the fraction of spheroids required to replicate the optical data as an additional output parameter. This is the first systematic test of the effect of using all theoretically possible combinations of δ taken at 355, 532, and 1064 nm as input in the lidar data inversion. We find that depolarization information of at least one wavelength already provides useful information for the inversion of optical data that have been collected in the presence of non-spherical mineral dust particles. However, any choice of δλ will give lower values of the single-scattering albedo than the traditional 3+2 data set. We find that input data sets that include δ355 give a spheroid fraction that closely resembles the dust ratio we obtain from using β532 and δ532 in a methodology applied in aerosol-type separation. The use of δ355 in data sets of two or three δλ reduces the spheroid fraction that is retrieved when using δ532 and δ1064. Use of the latter two parameters without accounting for δ355 generally leads to high spheroid fractions that we consider not trustworthy. The use of three δλ instead of two δλ, including the constraint that one of these is measured at 355 nm does not provide any advantage over using 3+2+δ355 for the observations with varying contributions of mineral dust considered here. However, additional measurements at wavelengths different from 355 nm would be desirable for application to a wider range of aerosol scenarios that may include non-spherical smoke particles, which can have values of δ355 that are indistinguishable from those found for mineral dust. We therefore conclude that – depending on measurement capability – the future standard input for inversion of lidar data taken in the presence of mineral dust particles and using the spheroid model of Dubovik et al. (2006) might be 3+2+δ355 or 3+2+δ355+δ532.

International audience; 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.

The Saharan Aerosol Long-Range Transport and Aerosol–Cloud-Interaction Experiment (SALTRACE) was devoted to the investigation of Saharan dust properties over the Caribbean. The campaign took place in June–July 2013. A wide set of ground-based and airborne aerosol instrumentation was deployed at the island of Barbados for a comprehensive experiment. Several sun photometers performed measurements during this campaign: two AERONET (Aerosol Robotic Network) Cimel sun photometers and the Sun and Sky Automatic Radiometer (SSARA). The sun photometers were co-located with the ground-based multi-wavelength lidars BERTHA (Backscatter Extinction lidar Ratio Temperature Humidity profiling Apparatus) and POLIS (Portable Lidar System). Aerosol properties derived from direct sun and sky radiance observations are analyzed, and a comparison with the co-located lidar and in situ data is provided. The time series of aerosol optical depth (AOD) allows identifying successive dust events with short periods in between in which the marine background conditions were observed. The moderate aerosol optical depth in the range of 0.3 to 0.6 was found during the dust periods. The sun photometer infrared channel at the 1640 nm wavelength was used in the retrieval to investigate possible improvements to aerosol size retrievals, and it was expected to have a larger sensitivity to coarse particles. The comparison between column (aerosol optical depth) and surface (dust concentration) data demonstrates the connection between the Saharan Air Layer and the boundary layer in the Caribbean region, as is shown by the synchronized detection of the successive dust events in both datasets. However the differences of size distributions derived from sun photometer data and in situ observations reveal the difficulties in carrying out a column closure study.

The present study aims to validate lidar retrievals of cloud-relevant aerosol properties by using polarization lidar and coincident airborne in situ measurements in the Saharan Air Layer over the Barbados region. Vertical profiles of the number concentration of cloud condensation nuclei (CCN), large particles (diameter d > 500 nm), surface area, and ice nucleating particles (INP) are estimated from the lidar measurements and compared with CCN concentrations and the INP-relevant aerosol properties in situ measured with aircraft in the framework of the Saharan Aerosol Long-range Transport and Aerosol–Cloudinteraction Experiment (SALTRACE) in summer 2013. The CCN number concentrations derived from lidar observations were up to a factor of two higher than the ones measured in situ on board the research aircraft Falcon. However, a reasonable agreement was obtained when taking the lidar uncertainty into account. The number concentration of particles with dry radius > 250 nm and the surface area concentration obtained from the lidar observations and used as input for the INP parameterizations agreed well (3 at 0.2 % water supersaturation and 25–65 INP per L at −25 °C. During the SALTRACE winter campaign (March 2014), the dust layer from Africa was mixed with smoke particles which dominated the CCN number concentration. This example highlights the unique lidar potential to separate smoke and dust contributions to the CCN reservoir and thus to identify the sensitive role of smoke in trade wind cumuli developments over the tropical Atlantic during the winter season.

The typical multiwavelength aerosol lidar data set for inversion of optical to microphysical parameters is composed of three backscatter coefficients (β) at 355, 532, and 1064 nm and two extinction coefficients (α) at 355 and 532 nm. This data combination is referred to as 3β + 2α or 3 + 2 data set. This set of data is sufficient for retrieving some important microphysical particle parameters if the particles have spherical shape. Here, we investigate the effect of including the particle linear depolarization ratio (δ) as a third input parameter to the inversion of lidar data. The inversion algorithm is generally not used if measurements show values of δ that exceed 0.10 at 532 nm, i.e. in the presence of non-spherical particles such as desert dust, volcanic ash, and under special circumstances biomass-burning smoke. We use experimental data collected with instruments that are capable of measuring δ at all three lidar wavelengths with an inversion routine that uses the theory of light scattering by randomly oriented spheroids to replicate scattering properties of non-spherical particles. This is the first systematic test of the effect of using all theoretically possible combinations of δ taken at 355, 532, and 1064 nm as input in the lidar data inversion. We find that depolarization information at least at one wavelength already provides useful information in the inversion of optical data that describe light-scattering by non-spherical particles. However, any choice of δλ will give lower values of the single-scattering albedo than the traditional 3 + 2 data set. We find that input data sets that include δ355 give a non-spherical fraction that closely resembles the dust ratio we obtain from using β532 and δ532 in a methodology applied in aerosol-type separation. The use of δ355 in data sets of two or three δλ reduces the fraction of non-spherical particles that is retrieved when using δ532 and δ1064. Use of the latter two without accounting for δ355 generally leads to high fractions of non-spherical particles that we consider not trustworthy. The use of three δλ instead of two δλ including the constraint that one of these is measured at 355 nm does not provide any advantage over using 3 + 2 + δ355. We conclude that — depending on measurement capability — the future standard input for inversion using spheroid kernels might be 3 + 2 + δ355 or 3 + 2 + δ355 + δ532.

For the first time, vertical profiles of the 1064 nm particle extinction coefficient obtained from Raman lidar observations at 1058 nm (nitrogen and oxygen rotational Raman backscatter) are presented. We applied the new technique in the framework of test measurements and performed several cirrus observations of particle backscatter and extinction coefficients, and corresponding extinction-to-backscatter ratios at the wavelengths of 355, 532, and 1064 nm. The cirrus backscatter coefficients were found to be equal for all three wavelengths keeping the retrieval uncertainties in mind. The multiple-scattering-corrected cirrus extinction coefficients at 355 nm were on average about 20–30 % lower than the ones for 532 and 1064 nm. The cirrus-mean extinction-to-backscatter ratio (lidar ratio) was 31 ± 5 sr (355 nm), 36 ± 5 sr (532 nm), and 38 ± 5 sr (1064 nm) in this single study. We further discussed the requirements needed to obtain aerosol extinction profiles in the lower troposphere at 1064 nm with good accuracy (20 % relative uncertainty) and appropriate temporal and vertical resolution.

Vertical profiles of number concentrations of dust particles relevant for ice nucleation in clouds are derived from lidar measurements. The results are compared to coincidental airborne in-situ measurements of particle number and surface area concentrations in the dust layer. The observations were performed in long- range transported Saharan dust at Barbados and Asian dust at Cyprus. The Asian dust data analysis is ongoing. A comparison of Asian and Saharan dust will be given at the conference. Concentrations of ice nucleating particles in the order of 10 to 1000 per cm-3 in the dust layer are derived for a temperature of -25°C at Barbados. The method can be used to continuously monitor the concentration of ice nucleating dust particles vertically resolved from lidar measurements.

Extremely high particle extinction coefficients, an order of magnitude higher than after the Mt. Pinatubo eruption in 1991, were measured in the stratosphere over Leipzig, Germany, on 22 August 2017. In a series of two articles, we present our observations of this record-breaking smoke event. In part 1 (Ansmann et al., 2018), we provide an overview of the smoke situation. The particle extinction coefficients reached 500 Mm −1 at 532 nm in the lower stratosphere around 15 km height and the smoke-related aerosol optical thickness (AOT) was close to 1.0 around noon. In part 2, we present the optical and microphysical properties of the fire smoke observed in a tropospheric layer from 5–6.5 km height and in a stratospheric layer from 15–16 km height. Three Raman lidars were run at Leipzig after sunset on 22 August. As a highlight, triple-wavelength polarization/Raman lidar measurements of the particle depolarization ratio and extinction-to-backscatter ratio (lidar ratio) at all three important lidar wavelengths of 355, 532, and 1064 nm could be performed. Very different particle depolarization ratios were found in the troposphere and in the stratosphere. The obviously compact and spherical tropospheric smoke particles caused almost no depolarization of backscattered laser radiation at all three wavelength ( 3 %), whereas the particles in the stratosphere lead to high depolarization ratios of 22 % at 355 nm and 18 % at 532 nm and a comparably low value of 4 % at 1064 nm in the stratosphere. The observed strong wavelength dependence is probably attributed to the narrow size distribution (accumulation mode) of irregularly shaped soot particles and the absence of a smoke coarse mode. The layer mean particle lidar ratios, on the other hand, were 40–45 sr (355 nm), and 65–80 sr (532 nm), and 80–95 sr (1064 nm) in both, the tropospheric and stratospheric layers indicating similar scattering and absorption properties. The 532 nm single scattering albedo was 0.8 in the stratospheric layer. The smoke particles were rather small (effective radius of 0.17 μm) in the tropospheric layer and much larger (effective radius of 0.32 μm) in the very dry stratosphere.

Light extinction coefficients of 500 Mm−1, about 20 times higher than after the Pinatubo volcanic eruptions in 1991, were observed with lidar in the stratosphere over Leipzig, Germany, on 22 August 2017. A pronounced smoke layer extended from 14–16 km height and was 3–4 km above the local tropopause. Optically dense layers of Canadian wildfire smoke reached central Europe 10 days after injection into the lower stratosphere caused by rather strong pyrocumulonimbus activity over western Canada. The smoke-related aerosol optical thickness (AOT) was close to 1.0 at 532 nm over Leipzig during the noon hours. We present detailed observations of this record-breaking smoke event in a series of two articles. In part 1, we provide an overview of Aerosol Robotic Network (AERONET) sun photometer observations and Moderate Resolution Imaging Spectroradiometer (MODIS) retrievals of AOT and show lidar measurements documenting the aerosol layering and the very high particle extinction coefficients. In part 2 (Haarig et al., 2018), observations with three polarization/Raman lidars are presented, performed at Leipzig after sunset on 22 August to elucidate the optical and microphysical properties of the aged smoke. As shown in this part 1, smoke particles were found throughout the free troposphere (532 nm AOT of 0.3). A pronounced 2-km thick stratospheric smoke layer occurred from 14–16 km height (AOT of 0.6). AERONET and lidar observations indicate peak mass concentrations of 70–100 μg m−3 in the stratosphere around noon and a well-defined (accumulation mode) smoke particle size distribution characterized by a large effective radius of 0.3–0.4 μm and the absence of a particle coarse mode.

We replaced a 1064-nm interference filter of a Polly-XT lidar system by a 1058-nm filter to observe pure rotational Raman backscattering from atmospheric Nitrogen and Oxygen. Polly-XT is compact Raman lidar with a Nd:YAG laser (20 Hz, 200 mJ at 1064 nm) and a 30-cm telescope mirror which applies photomultipliers in photoncounting mode. We present the first measured signals at 1058 nm and the derived extinction profile from measurements aboard RV Polarstern and in Leipzig. In combination with another Polly-XT system we could also derive particle backscatter and lidar ratio profiles at 1064 nm.

Canadian wildfire smoke was detected in the troposphere and lower stratosphere over Europe in August and September 2017. Lidar measurements from various stations of the European Aerosol Research Lidar Network (EARLINET) observed the stratospheric smoke layer. Triple-wavelength (355, 532, and 1064 nm) lidar measurements of the depolarization and the lidar ratio are reported from Leipzig, Germany. The particle linear depolarization ratio of the wildfire smoke in the stratosphere had an exceptional strong wavelength dependence reaching from 0.22 at 355 nm, to 0.18 at 532 nm, and 0.04 at 1064 nm. The lidar ratio increased with wavelength from 40±16 sr at 355 nm, to 66±12 sr at 532 nm, and 92±27 sr at 1064 nm. The development of the stratospheric smoke plume over several months was studied by long-term lidar measurements in Cyprus. The stratospheric smoke layers increased in altitude up to 24 km height.

For the first time, vertical profiles of the 1064 nm particle extinction coefficient obtained from Raman lidar observations at 1058 nm (nitrogen rotational Raman backscatter) are presented. We applied the new technique in the framework of test measurements and performed several cirrus observations of particle backscatter and extinction coefficients, and corresponding extinction-to-backscatter ratios at the wavelengths of 355, 532m and 1064 nm.

Large eddy simulations (LESs) are performed for the area of the Caribbean island Barbados to investigate island effects on boundary layer modification, cloud generation and vertical mixing of aerosols. Due to the presence of a topographically structured island surface in the domain center, the model setup has to be designed with open lateral boundaries. In order to generate inflow turbulence consistent with the upstream marine boundary layer forcing, we use the cell perturbation method based on finite amplitude potential temperature perturbations. In this work, this method is for the first time tested and validated for moist boundary layer simulations with open lateral boundary conditions. Observational data obtained from the SALTRACE field campaign is used for both model initialization and a comparison with Doppler wind and Raman lidar data. Several numerical sensitivity tests are carried out to demonstrate the problems related to “gray zone modeling” when using coarser spatial grid spacings beyond the inertial subrange of three-dimensional turbulence or when the turbulent marine boundary layer flow is replaced by laminar winds. Especially cloud properties in the downwind area west of Barbados are markedly affected in these kinds of simulations. Results of an additional simulation with a strong trade-wind inversion reveal its effect on cloud layer depth and location. Saharan dust layers that reach Barbados via long-range transport over the North Atlantic are included as passive tracers in the model. Effects of layer thinning, subsidence and turbulent downward transport near the layer bottom at z ≈ 1800 m become apparent. The exact position of these layers and strength of downward mixing is found to be mainly controlled atmospheric stability (especially inversion strength) and wind shear. Comparisons of LES model output with wind lidar data show similarities in the downwind vertical wind structure. Additionally, the model results accurately reproduce the development of the daytime convective boundary layer measured by the Raman lidar.

For aerosol typing with lidar, sea salt particles are usually assumed to be spherical with a consequently low depolarization ratio. Evidence of dried marine particles at the top of the humid marine aerosol layer with a depolarization ratio up to 0.1 has been found at predominately maritime locations on Barbados and in the Southern Atlantic. The depolarization ratio for these probably cubic sea salt particles has been measured at three wavelengths (355, 532 and 1064 nm) simultaneously for the first time and compared to model simulations.

The present study aims to evaluate lidar retrievals of cloud-relevant aerosol properties by using polarization lidar and coincident airborne in situ measurements in the Saharan Air Layer (SAL) over the Barbados region. Vertical profiles of the number concentration of cloud condensation nuclei (CCN), large particles (diameter d>500 nm), surface area, mass, and ice-nucleating particle (INP) concentration are derived from the lidar measurements and compared with CCN concentrations and the INP-relevant aerosol properties measured in situ with aircraft. The measurements were performed in the framework of the Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) in summer 2013. The CCN number concentrations derived from lidar observations were up to a factor of 2 higher than the ones measured in situ aboard the research aircraft Falcon. Possible reasons for the difference are discussed. The number concentration of particles with a dry radius of more than 250 nm and the surface-area concentration obtained from the lidar observations and used as input for the INP parameterizations agreed well ( %–50 % deviation) with the aircraft measurements. In a pronounced lofted dust layer during summer (10 July 2013), the lidar retrieval yielded 100–300 CCN per cubic centimeter at 0.2 % water supersaturation and 10–200 INPs per liter at −25 ∘C. Excellent agreement was also obtained in the comparison of mass concentration profiles. During the SALTRACE winter campaign (March 2014), the dust layer from Africa was mixed with smoke particles which dominated the CCN number concentration. This example highlights the unique lidar potential to separate smoke and dust contributions to the CCN reservoir and thus to identify the sensitive role of smoke in trade wind cumuli developments over the tropical Atlantic during the winter season.

Long-range transport of aerosol in the Saharan Air Layer (SAL) across the Atlantic plays an important role for weather, climate, and ocean fertilization. However, processes occurring within the SAL and their effects on aerosol properties are still unclear. In this work we study particle settling and vertical mixing within the SAL based on measured and modeled vertical aerosol profiles in the upper 1 km of the transported SAL. We use ground-based lidar measurements and airborne particle counter measurements over the western Atlantic, collected during the SALTRACE campaign, as well as space-based CALIOP lidar measurements from Africa to the western Atlantic in the summer season. In our model we take account of the optical properties and the Stokes gravitational settling of irregularly shaped Saharan dust particles.We test two hypotheses about the occurrence of vertical mixing within the SAL over the Atlantic to explain the aerosol profiles observed by the lidars and the particle counter. Our first hypothesis (H1) assumes that no mixing occurs in the SAL leading to a settling-induced separation of particle sizes. The second hypothesis (H2) assumes that vertical mixing occurs in the SAL allowing large super-micron dust particles to stay airborne longer than without mixing. The uncertainties of the particle linear depolarization ratio (δl) profiles measured by the ground-based lidars are comparable to the modeled differences between H1 and H2 and do not allow us to conclude which hypothesis fits better. The SALTRACE in situ data on size-resolved particle number concentrations show a presence of large particles near the SAL top that is inconsistent with H1. The analysis of the CALIOP measurements also reveals that the average δl profile over the western Atlantic is inconsistent with H1. Furthermore, it was found that the average δl profile in the upper 1 km of the SAL does not change along its transport path over the Atlantic. These findings give evidence that vertical mixing within the SAL is a common phenomenon with significant consequences for the evolution of the size distribution of super-micron dust particles during transport over the Atlantic. Further research is needed to precisely characterize the processes that are relevant for this phenomenon.