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Ozone depletion in the Arctic and Antarctic stratosphere induced by wildfire smoke

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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GARRLiC and LIRIC: Strengths and limitations for the characterization of dust and marine particles along with their mixtures

2017, Tsekeri, Alexandra, Lopatin, Anton, Amiridis, Vassilis, Marinou, Eleni, Igloffstein, Julia, Siomos, Nikolaos, Solomos, Stavros, Kokkalis, Panagiotis, Engelmann, Ronny, Baars, Holger, Gratsea, Myrto, Raptis, Panagiotis I., Binietoglou, Ioannis, Mihalopoulos, Nikolaos, Kalivitis, Nikolaos, Kouvarakis, Giorgos, Bartsotas, Nikolaos, Kallos, George, Basart, Sara, Schuettemeyer, Dirk, Wandinger, Ulla, Ansmann, Albert, Chaikovsky, Anatoli P., Dubovik, Oleg

The Generalized Aerosol Retrieval from Radiometer and Lidar Combined data algorithm (GARRLiC) and the LIdar-Radiometer Inversion Code (LIRIC) provide the opportunity to study the aerosol vertical distribution by combining ground-based lidar and sun-photometric measurements. Here, we utilize the capabilities of both algorithms for the characterization of Saharan dust and marine particles, along with their mixtures, in the south-eastern Mediterranean during the CHARacterization of Aerosol mixtures of Dust and Marine origin Experiment (CHARADMExp). Three case studies are presented, focusing on dust-dominated, marinedominated and dust-marine mixing conditions. GARRLiC and LIRIC achieve a satisfactory characterization for the dust-dominated case in terms of particle microphysical properties and concentration profiles. The marine-dominated and the mixture cases are more challenging for both algorithms, although GARRLiC manages to provide more detailed microphysical retrievals compared to AERONET, while LIRIC effectively discriminates dust and marine particles in its concentration profile retrievals. The results are also compared with modelled dust and marine concentration profiles and surface in situ measurements.

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Validation of Aeolus wind products above the Atlantic Ocean

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

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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The dual-field-of-view polarization lidar technique: a new concept in monitoring aerosol effects in liquid-water clouds – theoretical framework

2021, Jimenez, Cristofer, Ansmann, Albert, Engelmann, Ronny, Donovan, David, Malinka, Aleksey, Schmidt, Jörg, Seifert, Patric, Wandinger, Ulla

In a series of two articles, a novel, robust, and practicable lidar approach is presented that allows us to derive microphysical properties of liquid-water clouds (cloud extinction coefficient, droplet effective radius, liquid-water content, cloud droplet number concentration) at a height of 50–100 m above the cloud base. The temporal resolution of the observations is on the order of 30–120 s. Together with the aerosol information (aerosol extinction coefficients, cloud condensation nucleus concentration) below the cloud layer, obtained with the same lidar, in-depth aerosol–cloud interaction studies can be performed. The theoretical background and the methodology of the new cloud lidar technique is outlined in this article (Part 1), and measurement applications are presented in a companion publication (Part 2) (Jimenez et al., 2020a). The novel cloud retrieval technique is based on lidar observations of the volume linear depolarization ratio at two different receiver fields of view (FOVs). Extensive simulations of lidar returns in the multiple scattering regime were conducted to investigate the capabilities of a dual-FOV polarization lidar to measure cloud properties and to quantify the information content in the measured depolarization features regarding the basic retrieval parameters (cloud extinction coefficient, droplet effective radius). Key simulation results and the overall data analysis scheme developed to obtain the aerosol and cloud products are presented.

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Target categorization of aerosol and clouds by continuous multiwavelength-polarization lidar measurements

2017, Baars, Holger, Seifert, Patric, Engelmann, Ronny, Wandinger, Ulla

Absolute calibrated signals at 532 and 1064 nm and the depolarization ratio from a multiwavelength lidar are used to categorize primary aerosol but also clouds in high temporal and spatial resolution. Automatically derived particle backscatter coefficient profiles in low temporal resolution (30 min) are applied to calibrate the lidar signals. From these calibrated lidar signals, new atmospheric parameters in temporally high resolution (quasi-particle-backscatter coefficients) are derived. By using thresholds obtained from multiyear, multisite EARLINET (European Aerosol Research Lidar Network) measurements, four aerosol classes (small; large, spherical; large, non-spherical; mixed, partly nonspherical) and several cloud classes (liquid, ice) are defined. Thus, particles are classified by their physical features (shape and size) instead of by source. The methodology is applied to 2 months of continuous observations (24 h a day, 7 days a week) with the multiwavelength-Raman-polarization lidar PollyXT during the High-Definition Clouds and Precipitation for advancing Climate Prediction (HD(CP)2) Observational Prototype Experiment (HOPE) in spring 2013. Cloudnet equipment was operated continuously directly next to the lidar and is used for comparison. By discussing three 24 h case studies, it is shown that the aerosol discrimination is very feasible and informative and gives a good complement to the Cloudnet target categorization. Performing the categorization for the 2-month data set of the entire HOPE campaign, almost 1 million pixel (5 min×30 m) could be analysed with the newly developed tool. We find that the majority of the aerosol trapped in the planetary boundary layer (PBL) was composed of small particles as expected for a heavily populated and industrialized area. Large, spherical aerosol was observed mostly at the top of the PBL and close to the identified cloud bases, indicating the importance of hygroscopic growth of the particles at high relative humidity. Interestingly, it is found that on several days non-spherical particles were dispersed from the ground into the atmosphere.

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Smoke of extreme Australian bushfires observed in the stratosphere over Punta Arenas, Chile, in January 2020 : optical thickness, lidar ratios, and depolarization ratios at 355 and 532nm

2020, Ohneiser, Kevin, Ansmann, Albert, Baars, Holger, Seifert, Patric, Barja, Boris, Jimenez, Cristofer, Radenz, Martin, Teisseire, Audrey, Floutsi, Athina, Haarig, Moritz, Foth, Andreas, Chudnovsky, Alexandra, Engelmann, Ronny, Zamorano, Félix, Bühl, Johannes, Wandinger, Ulla

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.

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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

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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Polarization lidar: An extended three-signal calibration approach

2019, Jimenez, Cristofer, Ansmann, Albert, Engelmann, Ronny, Haarig, Moritz, Schmidt, Jörg, Wandinger, Ulla

We present a new formalism to calibrate a threesignal polarization lidar and to measure highly accurate height profiles of the volume linear depolarization ratios under realistic experimental conditions. The methodology considers elliptically polarized laser light, angular misalignment of the receiver unit with respect to the main polarization plane of the laser pulses, and cross talk among the receiver channels. A case study of a liquid-water cloud observation demonstrates the potential of the new technique. Long-term observations of the calibration parameters corroborate the robustness of the method and the long-term stability of the three-signal polarization lidar. A comparison with a second polarization lidar shows excellent agreement regarding the derived volume linear polarization ratios in different scenarios: A biomass burning smoke event throughout the troposphere and the lower stratosphere up to 16 km in height, a dust case, and also a cirrus cloud case. © Author(s) 2019.

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The dual-field-of-view polarization lidar technique: A new concept in monitoring aerosol effects in liquid-water clouds - Case studies

2020, Jimenez, Cristofer, Ansmann, Albert, Engelmann, Ronny, Donovan, David, Malinka, Aleksey, Seifert, Patric, Wiesen, Robert, Radenz, Martin, Yin, Zhenping, Bühl, Johannes, Schmidt, Jörg, Barja, Boris, Wandinger, Ulla

In a companion article (Jimenez et al., 2020), we introduced a new lidar method to derive microphysical properties of liquid-water clouds (cloud extinction coefficient, droplet effective radius, liquid-water content, cloud droplet number concentration Nd) at a height of 50-100m above the cloud base together with aerosol information (aerosol extinction coefficients, cloud condensation nuclei concentration NCCN) below the cloud layer so that detailed studies of the influence of given aerosol conditions on the evolution of liquid-water cloud layers with high temporal resolution solely based on lidar observations have become possible now. The novel cloud retrieval technique makes use of lidar observations of the volume linear depolarization ratio at two different receiver field of views (FOVs). In this article, Part 2, the new dual-FOV polarization lidar technique is applied to cloud measurements in pristine marine conditions at Punta Arenas in southern Chile. A multiwavelength polarization Raman lidar, upgraded by integrating a second polarization-sensitive channel to permit depolarization ratio observations at two FOVs, was used for these measurements at the southernmost tip of South America. Two case studies are presented to demonstrate the potential of the new lidar technique. Successful aerosol-cloud-interaction (ACI) studies based on measurements with the upgraded aerosol-cloud lidar in combination with a Doppler lidar of the vertical wind component could be carried out with 1 min temporal resolution at these pristine conditions. In a stratocumulus layer at the top of the convective boundary layer, we found values of Nd and NCCN (for 0.2% water supersaturation) ranging from 15-100 and 75-200 cm-3, respectively, during updraft periods. The studies of the aerosol impact on cloud properties yielded ACI values close to 1. The impact of aerosol water uptake on the ACI studies was analyzed with the result that the highest ACI values were obtained when considering aerosol proxies (light-extinction coefficient par or NCCN) measured at heights about 500m below the cloud base (and thus for dry aerosol conditions). © 2020 BMJ Publishing Group. All rights reserved.