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We present spectrally resolved optical and microphysical properties of western Canadian wildfire smoke observed in a tropospheric layer from 5–6.5 km height and in a stratospheric layer from 15–16 km height during a record-breaking smoke event on 22 August 2017. Three polarization/Raman lidars were run at the European Aerosol Research Lidar Network (EARLINET) station of Leipzig, Germany, after sunset on 22 August. For the first time, the linear depolarization ratio and extinction-to-backscatter ratio (lidar ratio) of aged smoke particles were measured at all three important lidar wavelengths of 355, 532, and 1064 nm. 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 wavelengths (<3 %), whereas the dry irregularly shaped soot 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. The lidar ratios were 40–45 sr (355 nm), 65–80 sr (532 nm), and 80–95 sr (1064 nm) in both the tropospheric and stratospheric smoke layers indicating similar scattering and absorption properties. The strong wavelength dependence of the stratospheric depolarization ratio was probably caused by the absence of a particle coarse mode (particle mode consisting of particles with radius >500 nm). The stratospheric smoke particles formed a pronounced accumulation mode (in terms of particle volume or mass) centered at a particle radius of 350–400 nm. The effective particle radius was 0.32 µm. The tropospheric smoke particles were much smaller (effective radius of 0.17 µm). Mass concentrations were of the order of 5.5 µg m−3 (tropospheric layer) and 40 µg m−3 (stratospheric layer) in the night of 22 August 2017. The single scattering albedo of the stratospheric particles was estimated to be 0.74, 0.8, and 0.83 at 355, 532, and 1064 nm, respectively.

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.

We present particle optical properties of stratospheric smoke layers observed with multiwavelength polarization Raman lidar over Punta Arenas (53.2∘ S, 70.9∘ W), Chile, at the southernmost tip of South America in January 2020. The smoke originated from the record-breaking bushfires in Australia. The stratospheric aerosol optical thickness reached values up to 0.85 at 532 nm in mid-January 2020. The main goal of this rapid communication letter is to provide first stratospheric measurements of smoke extinction-to-backscatter ratios (lidar ratios) and particle linear depolarization ratios at 355 and 532 nm wavelengths. These aerosol parameters are important input parameters in the analysis of spaceborne CALIPSO and Aeolus lidar observations of the Australian smoke spreading over large parts of the Southern Hemisphere in January and February 2020 up to heights of around 30 km. Lidar and depolarization ratios, simultaneously measured at 355 and 532 nm, are of key importance regarding the homogenization of the overall Aeolus (355 nm wavelength) and CALIPSO (532 nm wavelength) lidar data sets documenting the spread of the smoke and the decay of the stratospheric perturbation, which will be observable over the entire year of 2020. We found typical values and spectral dependencies of the lidar ratio and linear depolarization ratio for aged stratospheric smoke. At 355 nm, the lidar ratio and depolarization ratio ranged from 53 to 97 sr (mean 71 sr) and 0.2 to 0.26 (mean 0.23), respectively. At 532 nm, the lidar ratios were higher (75–112 sr, mean 97 sr) and the depolarization ratios were lower with values of 0.14–0.22 (mean 0.18). The determined depolarization ratios for aged Australian smoke are in very good agreement with respective ones for aged Canadian smoke, observed with lidar in stratospheric smoke layers over central Europe in the summer of 2017. The much higher 532 nm lidar ratios, however, indicate stronger absorption by the Australian smoke particles.

Triple-wavelength lidar observations of the depolarization ratio and the backscatter coefficient of marine aerosol as a function of relative humidity (RH) are presented with a 5 min time resolution. The measurements were performed at Barbados (13° N, 59° W) during the Saharan Aerosol Long-range Transport and Aerosol-Cloud interaction Experiment (SALTRACE) winter campaign in February 2014. The phase transition from spherical sea salt particles to cubic-like sea salt crystals was observed with a polarization lidar. The radiosonde and water-vapor Raman lidar observations show a drop in RH below 50 % in the marine aerosol layer simultaneously with a strong increase in particle linear depolarization ratio, which reaches values up to 0.12 ± 0.08 (at 355 nm), 0.15 ± 0.03 (at 532 nm), and 0.10 ± 0.01 (at 1064 nm). The lidar ratio (extinction-to-backscatter ratio) increased from 19 and 23 sr for spherical sea salt particles to 27 and 25 sr (at 355 and 532 nm, respectively) for cubic-like particle ensembles. Furthermore the scattering enhancement due to hygroscopic growth of the marine aerosol particles under atmospheric conditions was measured. Extinction enhancement factors from 40 to 80 % RH of 1.94 ± 0.94 at 355 nm, 3.70 ± 1.14 at 532 nm, and 5.37 ± 1.66 at 1064 nm were found. The enhanced depolarization ratios and lidar ratios were compared to modeling studies of cubic sea salt particles.

Light extinction coefficients of 500 Mm−1, about 20 times higher than after the Pinatubo volcanic eruptions in 1991, were observed by European Aerosol Research Lidar Network (EARLINET) lidars in the stratosphere over central Europe on 21–22 August 2017. Pronounced smoke layers with a 1–2 km vertical extent were found 2–5 km above the local tropopause. Optically dense layers of Canadian wildfire smoke reached central Europe 10 days after their injection into the upper troposphere and lower stratosphere which was caused by rather strong pyrocumulonimbus activity over western Canada. The smoke-related aerosol optical thickness (AOT) identified by lidar was close to 1.0 at 532 nm over Leipzig during the noon hours on 22 August 2017. Smoke particles were found throughout the free troposphere (AOT of 0.3) and in the pronounced 2 km thick stratospheric smoke layer at an altitude of 14–16 km (AOT of 0.6). The lidar observations indicated peak mass concentrations of 70–100 µg m−3 in the stratosphere. In addition to the lidar profiles, we analyzed Moderate Resolution Imaging Spectroradiometer (MODIS) fire radiative power (FRP) over Canada, and the distribution of MODIS AOT and Ozone Monitoring Instrument (OMI) aerosol index across the North Atlantic. These instruments showed a similar pattern and a clear link between the western Canadian fires and the aerosol load over Europe. In this paper, we also present Aerosol Robotic Network (AERONET) sun photometer observations, compare photometer and lidar-derived AOT, and discuss an obvious bias (the smoke AOT is too low) in the photometer observations. Finally, we compare the strength of this record-breaking smoke event (in terms of the particle extinction coefficient and AOT) with major and moderate volcanic events observed over the northern midlatitudes.

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.

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.

Triple-wavelength polarization lidar measurements in Saharan dust layers were performed at Barbados (13.1° N, 59.6° W), 5000–8000 km west of the Saharan dust sources, in the framework of the Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE-1, June–July 2013, SALTRACE-3, June–July 2014). Three case studies are discussed. High quality was achieved by comparing the dust linear depolarization ratio profiles measured at 355, 532, and 1064 nm with respective dual-wavelength (355, 532 nm) depolarization ratio profiles measured with a reference lidar. A unique case of long-range transported dust over more than 12 000 km is presented. Saharan dust plumes crossing Barbados were measured with an airborne triple-wavelength polarization lidar over Missouri in the midwestern United States 7 days later. Similar dust optical properties and depolarization features were observed over both sites indicating almost unchanged dust properties within this 1 week of travel from the Caribbean to the United States. The main results of the triple-wavelength polarization lidar observations in the Caribbean in the summer seasons of 2013 and 2014 are summarized. On average, the particle linear depolarization ratios for aged Saharan dust were found to be 0.252 ± 0.030 at 355 nm, 0.280 ± 0.020 at 532 nm, and 0.225 ± 0.022 at 1064 nm after approximately 1 week of transport over the tropical Atlantic. Based on published simulation studies we present an attempt to explain the spectral features of the depolarization ratio of irregularly shaped mineral dust particles, and conclude that most of the irregularly shaped coarse-mode dust particles (particles with diameters > 1 µm) have sizes around 1.5–2 µm. The SALTRACE results are also set into the context of the SAMUM-1 (Morocco, 2006) and SAMUM-2 (Cabo Verde, 2008) depolarization ratio studies. Again, only minor changes in the dust depolarization characteristics were observed on the way from the Saharan dust sources towards the Caribbean.

At the end of May 2025, extremely strong wildfires in Canada produced several pyrocumulonimbus clouds lifting the smoke particles up to the lower stratosphere. Stratospheric aerosol optical depths of more than 2.5 were observed by the ATmospheric LiDAR (ATLID) onboard of the Earth Cloud, Aerosol and Radiation Explorer (EarthCARE) satellite. ATLID observations showed that the smoke layer top ascended from 13.6 km over Canada to 17.4 km over Europe. The enhanced depolarization ratio of 0.24 ±$\\pm $0.02 stayed constant during transport and indicated non‐spherical smoke particles. ATLID is the first space lidar that is able to measure the extinction‐to‐backscatter ratio (lidar ratio) at 355 nm. A decrease of the lidar ratio with increasing transport time was observed from values of 68 ±$\\pm $5 to 49 ±$\\pm $5 sr. EarthCARE observed the substantial downmixing of the stratospheric smoke into the troposphere at tropopause folds over the Mediterranean revealing an important removal process of stratospheric smoke.

The extension of the Hybrid End-To-End Aerosol Classification (HETEAC) model with respect to stratospheric targets is presented. The methodology follows the HETEAC approach, i.e., a suitable set of basic feature types is defined to allow for scattering calculations. The most appropriate microphysical representation is selected based on the agreement between optical properties derived from scattering calculations and ground-based lidar observations. The extended HETEAC model (2.0), considers stratospheric features such as sulfate, volcanic ash, and smoke particles and also polar stratospheric clouds (PSCs). HETEAC 2.0 ensures consistency with the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) approach, which is of great importance for the harmonization of long-term satellite records.