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    Ozone depletion in the Arctic and Antarctic stratosphere induced by wildfire smoke
    (Katlenburg-Lindau : EGU, 2022) Ansmann, Albert; Ohneiser, Kevin; Chudnovsky, Alexandra; Knopf, Daniel A.; Eloranta, Edwin W.; Villanueva, Diego; Seifert, Patric; Radenz, Martin; Barja, Boris; Zamorano, Félix; Jimenez, Cristofer; Engelmann, Ronny; Baars, Holger; Griesche, Hannes; Hofer, Julian; Althausen, Dietrich; Wandinger, Ulla
    A record-breaking stratospheric ozone loss was observed over the Arctic and Antarctica in 2020. Strong ozone depletion occurred over Antarctica in 2021 as well. The ozone holes developed in smoke-polluted air. In this article, the impact of Siberian and Australian wildfire smoke (dominated by organic aerosol) on the extraordinarily strong ozone reduction is discussed. The study is based on aerosol lidar observations in the North Pole region (October 2019-May 2020) and over Punta Arenas in southern Chile at 53.2°S (January 2020-November 2021) as well as on respective NDACC (Network for the Detection of Atmospheric Composition Change) ozone profile observations in the Arctic (Ny-Ålesund) and Antarctica (Neumayer and South Pole stations) in 2020 and 2021. We present a conceptual approach on how the smoke may have influenced the formation of polar stratospheric clouds (PSCs), which are of key importance in the ozone-depleting processes. The main results are as follows: (a) the direct impact of wildfire smoke below the PSC height range (at 10-12 km) on ozone reduction seems to be similar to well-known volcanic sulfate aerosol effects. At heights of 10-12 km, smoke particle surface area (SA) concentrations of 5-7 μm2 cm-3 (Antarctica, spring 2021) and 6-10 μm2 cm-3 (Arctic, spring 2020) were correlated with an ozone reduction in terms of ozone partial pressure of 0.4-1.2 mPa (about 30 % further ozone reduction over Antarctica) and of 2-3.5 mPa (Arctic, 20 %-30 % reduction with respect to the long-term springtime mean). (b) Within the PSC height range, we found indications that smoke was able to slightly increase the PSC particle number and surface area concentration. In particular, a smoke-related additional ozone loss of 1-2 mPa (10 %-20 % contribution to the total ozone loss over Antarctica) was observed in the 14-23 km PSC height range in September-October 2020 and 2021. Smoke particle number concentrations ranged from 10 to 100 cm-3 and were about a factor of 10 (in 2020) and 5 (in 2021) above the stratospheric aerosol background level. Satellite observations indicated an additional mean column ozone loss (deviation from the long-term mean) of 26-30 Dobson units (9 %-10 %, September 2020, 2021) and 52-57 Dobson units (17 %-20 %, October 2020, 2021) in the smoke-polluted latitudinal Antarctic belt from 70-80°S. Copyright:
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    Wildfire smoke, Arctic haze, and aerosol effects on mixed-phase and cirrus clouds over the North Pole region during MOSAiC: an introduction
    (Katlenburg-Lindau : European Geosciences Union, 2021) Engelmann, Ronny; Ansmann, Albert; Ohneiser, Kevin; Griesche, Hannes; Radenz, Martin; Hofer, Julian; Althausen, Dietrich; Dahlke, Sandro; Maturilli, Marion; Veselovskii, Igor; Jimenez, Cristofer; Wiesen, Robert; Baars, Holger; Bühl, Johannes; Gebauer, Henriette; Haarig, Moritz; Seifert, Patric; Wandinger, Ulla; Macke, Andreas
    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 30gkm height. The expedition lasted from September 2019 to October 2020 and measurements were mostly taken between 85 and 88.5ggN. 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 10gkm deep wildfire smoke layer over the North Pole region between 7-8gkm and 17-18gkm height with an aerosol optical thickness (AOT) at 532gnm 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 532gnm AOT by volcanic sulfate aerosol (Raikoke eruption) was estimated to always be lower than 15g%. The optical and microphysical properties of the UTLS smoke layer are presented in an accompanying paper . 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.
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    The vertical aerosol type distribution above Israel – 2 years of lidar observations at the coastal city of Haifa
    (Katlenburg-Lindau : EGU, 2022) Heese, Birgit; Floutsi, Athena Augusta; Baars, Holger; Althausen, Dietrich; Hofer, Julian; Herzog, Alina; Mewes, Silke; Radenz, Martin; Schechner, Yoav Y.
    For the first time, vertically resolved long-term lidar measurements of the aerosol distribution were conducted in Haifa, Israel. The measurements were performed by a PollyXT multi-wavelength Raman and polarization lidar. The lidar was measuring continuously over a 2-year period from March 2017 to May 2019. The resulting data set is a series of manually evaluated lidar optical property profiles. To identify the aerosol types in the observed layers, a novel aerosol typing method that was developed at TROPOS is used. This method applies optimal estimation to a combination of lidar-derived intensive aerosol properties to determine the statistically most-likely contribution per aerosol component in terms of relative volume. A case study that shows several elevated aerosol layers illustrates this method and shows, for example, that coarse dust particles are observed up to 5ĝ€¯km height over Israel. From the whole data set, the seasonal distribution of the observed aerosol components over Israel is derived. Throughout all seasons, coarse spherical particles like sea salt and hygroscopically grown continental aerosol were observed. These particles originate from continental Europe and were transported over the Mediterranean Sea. Sea-salt particles were observed frequently due to the coastal site of Haifa. The highest contributions of coarse spherical particles are present in summer, autumn, and winter. During spring, mostly coarse non-spherical particles that are attributed to desert dust were observed. This is consistent with the distinct dust season in spring in Israel. An automated time-height-resolved air mass source attribution method identifies the origin of the dust in the Sahara and the Arabian deserts. Fine-mode spherical particles contribute significantly to the observed aerosol mixture during all seasons. These particles originate mainly from the industrial region at the bay of Haifa.
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    Calibration of Raman lidar water vapor profiles by means of AERONET photometer observations and GDAS meteorological data
    (München : European Geopyhsical Union, 2018) Dai, Guangyao; Althausen, Dietrich; Hofer, Julian; Engelmann, Ronny; Seifert, Patric; Bühl, Johannes; Mamouri, Rodanthi-Elisavet; Wu, Songhua; Ansmann, Albert
    We present a practical method to continuously calibrate Raman lidar observations of water vapor mixing ratio profiles. The water vapor profile measured with the multiwavelength polarization Raman lidar PollyXT is calibrated by means of co-located AErosol RObotic NETwork (AERONET) sun photometer observations and Global Data Assimilation System (GDAS) temperature and pressure profiles. This method is applied to lidar observations conducted during the Cyprus Cloud Aerosol and Rain Experiment (CyCARE) in Limassol, Cyprus. We use the GDAS temperature and pressure profiles to retrieve the water vapor density. In the next step, the precipitable water vapor from the lidar observations is used for the calibration of the lidar measurements with the sun photometer measurements. The retrieved calibrated water vapor mixing ratio from the lidar measurements has a relative uncertainty of 11 % in which the error is mainly caused by the error of the sun photometer measurements. During CyCARE, nine measurement cases with cloud-free and stable meteorological conditions are selected to calculate the precipitable water vapor from the lidar and the sun photometer observations. The ratio of these two precipitable water vapor values yields the water vapor calibration constant. The calibration constant for the PollyXT Raman lidar is 6.56 g kg−1 ± 0.72 g kg−1 (with a statistical uncertainty of 0.08 g kg−1 and an instrumental uncertainty of 0.72 g kg−1). To check the quality of the water vapor calibration, the water vapor mixing ratio profiles from the simultaneous nighttime observations with Raman lidar and Vaisala radiosonde sounding are compared. The correlation of the water vapor mixing ratios from these two instruments is determined by using all of the 19 simultaneous nighttime measurements during CyCARE. Excellent agreement with the slope of 1.01 and the R2 of 0.99 is found. One example is presented to demonstrate the full potential of a well-calibrated Raman lidar. The relative humidity profiles from lidar, GDAS (simulation) and radiosonde are compared, too. It is found that the combination of water vapor mixing ratio and GDAS temperature profiles allow us to derive relative humidity profiles with the relative uncertainty of 10–20 %.
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    Validation of Aeolus wind products above the Atlantic Ocean
    (Katlenburg-Lindau : Copernicus, 2020) Baars, Holger; Herzog, Alina; Heese, Birgit; Ohneiser, Kevin; Hanbuch, Karsten; Hofer, Julian; Yin, Zhenping; Engelmann, Ronny; Wandinger, Ulla
    In August 2018, the first Doppler wind lidar in space called Atmospheric Laser Doppler Instrument (ALADIN) was launched on board the satellite Aeolus by the European Space Agency (ESA). Aeolus measures profiles of one horizontal wind component (i.e., mainly the west-east direction) in the troposphere and lower stratosphere on a global basis. Furthermore, profiles of aerosol and cloud properties can be retrieved via the high spectral resolution lidar (HSRL) technique. The Aeolus mission is supposed to improve the quality of weather forecasts and the understanding of atmospheric processes. We used the opportunity to perform a unique validation of the wind products of Aeolus by utilizing the RV Polarstern cruise PS116 from Bremerhaven to Cape Town in November/December 2018. Due to concerted course modifications, six direct intersections with the Aeolus ground track could be achieved in the Atlantic Ocean west of the African continent. For the validation of the Aeolus wind products, we launched additional radiosondes and used the EARLINET/ACTRIS lidar Polly XT for atmospheric scene analysis. The six analyzed cases prove that Aeolus is able to measure horizontal wind speeds in the nearly west-east direction. Good agreements with the radiosonde observations could be achieved for both Aeolus wind products-the winds observed in clean atmospheric regions called Rayleigh winds and the winds obtained in cloud layers called Mie winds (according to the responsible scattering regime). Systematic and statistical errors of the Rayleigh winds were less than 1.5 and 3.3ms-1, respectively, when compared to radiosonde values averaged to the vertical resolution of Aeolus. For the Mie winds, a systematic and random error of about 1ms-1 was obtained from the six comparisons in different climate zones. However, it is also shown that the coarse vertical resolution of 2km in the upper troposphere, which was set in this early mission phase 2 months after launch, led to an underestimation of the maximum wind speed in the jet stream regions. In summary, promising first results of the first wind lidar space mission are shown and prove the concept of Aeolus for global wind observations. © 2020 Author(s).
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    EARLINET evaluation of the CATS Level 2 aerosol backscatter coefficient product
    (Katlenburg-Lindau : EGU, 2019) Proestakis, Emmanouil; Amiridis, Vassilis; Marinou, Eleni; Binietoglou, Ioannis; Ansmann, Albert; Wandinger, Ulla; Hofer, Julian; Yorks, John; Nowottnick, Edward; Makhmudov, Abduvosit; Papayannis, Alexandros; Pietruczuk, Aleksander; Gialitaki, Anna; Apituley, Arnoud; Szkop, Artur; Muñoz Porcar, Constantino; Bortoli, Daniele; Dionisi, Davide; Althausen, Dietrich; Mamali, Dimitra; Balis, Dimitris; Nicolae, Doina; Tetoni, Eleni; Liberti, Gian Luigi; Baars, Holger; Mattis, Ina; Stachlewska, Iwona Sylwia; Voudouri, Kalliopi Artemis; Mona, Lucia; Mylonaki, Maria; Perrone, Maria Rita; Costa, Maria João; Sicard, Michael; Papagiannopoulos, Nikolaos; Siomos, Nikolaos; Burlizzi, Pasquale; Pauly, Rebecca; Engelmann, Ronny; Abdullaev, Sabur; Pappalardo, Gelsomina
    We present the evaluation activity of the European Aerosol Research Lidar Network (EARLINET) for the quantitative assessment of the Level 2 aerosol backscatter coefficient product derived by the Cloud-Aerosol Transport System (CATS) aboard the International Space Station (ISS; Rodier et al., 2015). The study employs correlative CATS and EARLINET backscatter measurements within a 50km distance between the ground station and the ISS overpass and as close in time as possible, typically with the starting time or stopping time of the EARLINET performed measurement time window within 90min of the ISS overpass, for the period from February 2015 to September 2016. The results demonstrate the good agreement of the CATS Level 2 backscatter coefficient and EARLINET. Three ISS overpasses close to the EARLINET stations of Leipzig, Germany; Évora, Portugal; and Dushanbe, Tajikistan, are analyzed here to demonstrate the performance of the CATS lidar system under different conditions. The results show that under cloud-free, relative homogeneous aerosol conditions, CATS is in good agreement with EARLINET, independent of daytime and nighttime conditions. CATS low negative biases are observed, partially attributed to the deficiency of lidar systems to detect tenuous aerosol layers of backscatter signal below the minimum detection thresholds; these are biases which may lead to systematic deviations and slight underestimations of the total aerosol optical depth (AOD) in climate studies. In addition, CATS misclassification of aerosol layers as clouds, and vice versa, in cases of coexistent and/or adjacent aerosol and cloud features, occasionally leads to non-representative, unrealistic, and cloud-contaminated aerosol profiles. Regarding solar illumination conditions, low negative biases in CATS backscatter coefficient profiles, of the order of 6.1%, indicate the good nighttime performance of CATS. During daytime, a reduced signal-to-noise ratio by solar background illumination prevents retrievals of weakly scattering atmospheric layers that would otherwise be detectable during nighttime, leading to higher negative biases, of the order of 22.3%. © Author(s) 2019.
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    Differences and Similarities of Central Asian, African, and Arctic Dust Composition from a Single Particle Perspective
    (Basel, Switzerland : MDPI AG, 2020) Kandler, Konrad; Schneiders, Kilian; Heuser, Johannes; Waza, Andebo; Aryasree, Sudharaj; Althausen, Dietrich; Hofer, Julian; Abdullaev, Sabur F.; Makhmudov, Abduvosit N.
    Mineral dust composition affects a multitude of processes in the atmosphere and adjacent compartments. Dust dry deposition was collected near source in northwest Africa, in Central Asia, and on Svalbard and at three locations of the African outflow regime. Samples were subjected to automated scanning electron microscopy with energy-dispersive X-ray analysis to obtain size and composition of 216,000 individual particles. Results show low temporal variation in estimated optical properties for each location, but considerable differences between the African, Central Asian, and Arctic regimes. No significant difference was found between the K-feldspar relative abundances, indicating comparable related ice-nucleation abilities. The mixing state between calcium and iron compounds was different for near source and transport regimes, potentially in part due to size sorting effects. As a result, in certain situations (high acid availability, limited time) atmospheric processing of the dust is expected to lead to less increased iron solubility for near-source dusts (in particular for Central Asian ones) than for transported ones (in particular of Sahelian origin). © 2020 by the authors. Licensee MDPI, Basel, Switzerland.
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    Ice-nucleating particle versus ice crystal number concentrationin altocumulus and cirrus layers embedded in Saharan dust: a closure study
    (Katlenburg-Lindau : EGU, 2019) Ansmann, Albert; Mamouri, Rodanthi-Elisavet; Bühl, Johannes; Seifert, Patric; Engelmann, Ronny; Hofer, Julian; Nisantzi, Argyro; Atkinson, James D.; Kanji, Zamin A.; Sierau, Berko; Vrekoussis, Mihalis; Sciare, Jean
    For the first time, a closure study of the relationship between the ice-nucleating particle concentration (INP; INPC) and ice crystal number concentration (ICNC) in altocumulus and cirrus layers, solely based on groundbased active remote sensing, is presented. Such aerosol- cloud closure experiments are required (a) to better understand aerosol-cloud interaction in the case of mixed-phase clouds, (b) to explore to what extent heterogeneous ice nucleation can contribute to cirrus formation, which is usually controlled by homogeneous freezing, and (c) to check the usefulness of available INPC parameterization schemes, applied to lidar profiles of aerosol optical and microphysical properties up to the tropopause level. The INPC-ICNC closure studies were conducted in Cyprus (Limassol and Nicosia) during a 6-week field campaign in March-April 2015 and during the 17-month CyCARE (Cyprus Clouds Aerosol and Rain Experiment) campaign. The focus was on altocumulus and cirrus layers which developed in pronounced Saharan dust layers at heights from 5 to 11 km. As a highlight, a long-lasting cirrus event was studied which was linked to the development of a very strong dust-infused baroclinic storm (DIBS) over Algeria. The DIBS was associated with strong convective cloud development and lifted large amounts of Saharan dust into the upper troposphere, where the dust influenced the evolution of an unusually large anvil cirrus shield and the subsequent transformation into an cirrus uncinus cloud system extending from the eastern Mediterranean to central Asia, and thus over more than 3500 km. Cloud top temperatures of the three discussed closure study cases ranged from - 20 to -57 °C. The INPC was estimated from polarization/Raman lidar observations in combination with published INPC parameterization schemes, whereas the ICNC was retrieved from combined Doppler lidar, aerosol lidar, and cloud radar observations of the terminal velocity of falling ice crystals, radar reflectivity, and lidar backscatter in combination with the modeling of backscattering at the 532 and 8.5 mm wavelengths. A good-to-acceptable agreement between INPC (observed before and after the occurrence of the cloud layer under investigation) and ICNC values was found in the discussed three proof-of-concept closure experiments. In these case studies, INPC and ICNC values matched within an order of magnitude (i.e., within the uncertainty ranges of the INPC and ICNC estimates), and they ranged from 0.1 to 10 L-1 in the altocumulus layers and 1 to 50 L-1 in the cirrus layers observed between 8 and 11 km height. The successful closure experiments corroborate the important role of heterogeneous ice nucleation in atmospheric ice formation processes when mineral dust is present. The observed longlasting cirrus event could be fully explained by the presence of dust, i.e., without the need for homogeneous ice nucleation processes. © 2019 Author(s).
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    Modifications in aerosol physical, optical and radiative properties during heavy aerosol events over Dushanbe, Central Asia
    (Amsterdam [u.a.] : Elsevier, 2021) Rupakheti, Dipesh; Rupakheti, Maheswar; Yin, Xiufeng; Hofer, Julian; Rai, Mukesh; Hu, Yuling; Abdullaev, Sabur F.; Kang, Shichang
    The location of Central Asia, almost at the center of the global dust belt region, makes it susceptible for dust events. The studies on atmospheric impact of dust over the region are very limited despite the large area occupied by the region and its proximity to the mountain regions (Tianshan, Hindu Kush-Karakoram-Himalayas, and Tibetan Plateau). In this study, we analyse and explain the modification in aerosols’ physical, optical and radiative properties during various levels of aerosol loading observed over Central Asia utilizing the data collected during 2010–2018 at the AERONET station in Dushanbe, Tajikistan. Aerosol episodes were classified as strong anthropogenic, strong dust and extreme dust. The mean aerosol optical depth (AOD) during these three types of events was observed a factor of ~3, 3.5 and 6.6, respectively, higher than the mean AOD for the period 2010–2018. The corresponding mean fine-mode fraction was 0.94, 0.20 and 0.16, respectively, clearly indicating the dominance of fine-mode anthropogenic aerosol during the first type of events, whereas coarse-mode dust aerosol dominated during the other two types of events. This was corroborated by the relationships among various aerosol parameters (AOD vs. AE, and EAE vs. AAE, SSA and RRI). The mean aerosol radiative forcing (ARF) at the top of the atmosphere (ARFTOA), the bottom of the atmosphere (ARFBOA), and in the atmosphere (ARFATM) were −35 ± 7, −73 ± 16, and 38 ± 17 Wm−2 during strong anthropogenic events, −48 ± 12, −85 ± 24, and 37 ± 15 Wm−2 during strong dust event, and −68 ± 19, −117 ± 38, and 49 ± 21 Wm−2 during extreme dust events. Increase in aerosol loading enhanced the aerosol-induced atmospheric heating rate to 0.5–1.6 K day−1 (strong anthropogenic events), 0.4–1.9 K day−1 (strong dust events) and 0.8–2.7 K day−1 (extreme dust events). The source regions of air masses to Dushanbe during the onset of such events are also identified. Our study contributes to the understanding of dust and anthropogenic aerosols, in particular the extreme events and their disproportionally high radiative impacts over Central Asia.
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    Long-term profiling of mineral dust and pollution aerosol with multiwavelength polarization Raman lidar at the Central Asian site of Dushanbe, Tajikistan: Case studies
    (München : European Geopyhsical Union, 2017) Hofer, Julian; Althausen, Dietrich; Abdullaev, Sabur F.; Makhmudov, Abduvosit N.; Nazarov, Bakhron I.; Schettler, Georg; Engelmann, Ronny; Baars, Holger; Fomba, K.Wadinga; Müller, Konrad; Heinold, Bernd; Kandler, Konrad; Ansmann, Albert
    For the first time, continuous vertically resolved aerosol measurements were performed by lidar in Tajikistan, Central Asia. Observations with the multiwavelength polarization Raman lidar PollyXT were conducted during CADEX (Central Asian Dust EXperiment) in Dushanbe, Tajikistan, from March 2015 to August 2016. Co-located with the lidar, a sun photometer was also operated. The goal of CADEX is to provide an unprecedented data set on vertically resolved aerosol optical properties in Central Asia, an area highly affected by climate change but largely missing vertically resolved aerosol measurements. During the 18-month measurement campaign, mineral dust was detected frequently from ground to the cirrus level height. In this study, an overview of the measurement period is given and four typical but different example measurement cases are discussed in detail. Three of them are dust cases and one is a contrasting pollution aerosol case. Vertical profiles of the measured optical properties and the calculated dust and non-dust mass concentrations are presented. Dust source regions were identified by means of backward trajectory analyses. A lofted layer of Middle Eastern dust with an aerosol optical thickness (AOT) of 0.4 and an extinction-related Ångström exponent of 0.41 was measured. In comparison, two near-ground dust cases have Central Asian sources. One is an extreme dust event with an AOT of 1.5 and Ångström exponent of 0.12 and the other one is a most extreme dust event with an AOT of above 4 (measured by sun photometer) and an Ångström exponent of −0.08. The observed lidar ratios (and particle linear depolarization ratios) in the presented dust cases range from 40.3 to 46.9sr (and 0.18–0.29) at 355nm and from 35.7 to 42.9sr (0.31–0.35) at 532nm wavelength. The particle linear depolarization ratios indicate almost unpolluted dust in the case of a lofted dust layer and pure dust in the near-ground dust cases. The lidar ratio values are lower than typical lidar ratio values for Saharan dust (50–60sr) and comparable to Middle Eastern or west-Asian dust lidar ratios (35–45sr). In contrast, the presented case of pollution aerosol of local origin has an Ångström exponent of 2.07 and a lidar ratio (particle linear depolarization ratio) of 55.8sr (0.03) at 355nm and 32.8sr (0.08) at 532nm wavelength.