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    Tropospheric and stratospheric wildfire smoke profiling with lidar: mass, surface area, CCN, and INP retrieval
    (Katlenburg-Lindau : European Geosciences Union, 2021) Ansmann, Albert; Ohneiser, Kevin; Mamouri, Rodanthi-Elisavet; Knopf, Daniel A.; Veselovskii, Igor; Baars, Holger; Engelmann, Ronny; Foth, Andreas; Jimenez, Cristofer; Seifert, Patric; Barja, Boris
    We present retrievals of tropospheric and stratospheric height profiles of particle mass, volume, surface area, and number concentrations in the case of wildfire smoke layers as well as estimates of smoke-related cloud condensation nuclei (CCN) and ice-nucleating particle (INP) concentrations from backscatter lidar measurements on the ground and in space. Conversion factors used to convert the optical measurements into microphysical properties play a central role in the data analysis, in addition to estimates of the smoke extinction-to-backscatter ratios required to obtain smoke extinction coefficients. The set of needed conversion parameters for wildfire smoke is derived from AERONET observations of major smoke events, e.g., in western Canada in August 2017, California in September 2020, and southeastern Australia in January-February 2020 as well as from AERONET long-term observations of smoke in the Amazon region, southern Africa, and Southeast Asia. The new smoke analysis scheme is applied to CALIPSO observations of tropospheric smoke plumes over the United States in September 2020 and to ground-based lidar observation in Punta Arenas, in southern Chile, in aged Australian smoke layers in the stratosphere in January 2020. These case studies show the potential of spaceborne and ground-based lidars to document large-scale and long-lasting wildfire smoke events in detail and thus to provide valuable information for climate, cloud, and air chemistry modeling efforts performed to investigate the role of wildfire smoke in the atmospheric system. © 2021 Albert Ansmann et al.
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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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    The dual-field-of-view polarization lidar technique: a new concept in monitoring aerosol effects in liquid-water clouds – theoretical framework
    (Katlenburg-Lindau : EGU, 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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    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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    Experimental assessment of a micro-pulse lidar system in comparison with reference lidar measurements for aerosol optical properties retrieval
    (Katlenburg-Lindau : European Geosciences Union, 2021) Córdoba-Jabonero, Carmen; Ansmann, Albert; Jiménez, Cristofer; Baars, Holger; López-Cayuela, María-Ángeles; Engelmann, Ronny
    Simultaneous observations of a polarized micro-pulse lidar (P-MPL) system and two reference European Aerosol Research Lidar Network lidars running at the Leipzig site Germany, 51.4g gN, 12.4g gE; 125gmga.s.l.) were performed during a comprehensive 2-month field intercomparison campaign in summer 2019. An experimental assessment regarding both the overlap (OVP) correction of the P-MPL signal profiles and the volume linear depolarization ratio (VLDR) analysis, together with its impact on the retrieval of the aerosol optical properties, is achieved; the experimental procedure used is also described. The optimal lidar-specific OVP function is experimentally determined, highlighting that the one delivered by the P-MPL manufacturer cannot be used long. Among the OVP functions examined, the averaged function between those obtained from the comparison of the P-MPL observations with those of the other two reference lidars seems to be the best proxy at both near- and far-field ranges. In addition, the impact of the OVP function on the accuracy of the retrieved profiles of the total particle backscatter coefficient (PBC) and the particle linear depolarization ratio (PLDR) is examined. The VLDR profile is obtained and compared with that derived from the reference lidar, showing that it needs to be corrected by a small offset value with good accuracy. Once P-MPL measurements are optimally (OVP, VLDR) corrected, both the PBC and PLDR profiles can be accurately derived and are in good agreement with reference aerosol retrievals. Overall, as a systematic requirement for lidar systems, an adequate OVP function determination and VLDR testing analysis needs to be performed on a regular basis to correct the P-MPL measurements in order to derive suitable aerosol products. A dust event observed in Leipzig in June 2019 is used for illustration.
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    Contrasting ice formation in Arctic clouds: surface-coupled vs. surface-decoupled clouds
    (Katlenburg-Lindau : European Geosciences Union, 2021) Griesche, Hannes J.; Ohneiser, Kevin; Seifert, Patric; Radenz, Martin; Engelmann, Ronny; Ansmann, Albert
    In the Arctic summer of 2017 (1 June to 16 July) measurements with the OCEANET-Atmosphere facility were performed during the Polarstern cruise PS106. OCEANET comprises amongst other instruments the multiwavelength polarization lidar PollyXT_OCEANET and for PS106 was complemented with a vertically pointed 35 GHz cloud radar. In the scope of the presented study, the influence of cloud height and surface coupling on the probability of clouds to contain and form ice is investigated. Polarimetric lidar data were used for the detection of the cloud base and the identification of the thermodynamic phase. Both radar and lidar were used to detect cloud top. Radiosonde data were used to derive the thermodynamic structure of the atmosphere and the clouds. The analyzed data set shows a significant impact of the surface-coupling state on the probability of ice formation. Surface-coupled clouds were identified by a quasi-constant potential temperature profile from the surface up to liquid layer base. Within the same minimum cloud temperature range, ice-containing clouds have been observed more frequently than surface-decoupled clouds by a factor of up to 6 (temperature intervals between -7.5 and -5 C, 164 vs. 27 analyzed intervals of 30 min). The frequency of occurrence of surface-coupled ice-containing clouds was found to be 2-3 times higher (e.g., 82% vs. 35% between -7.5 and -5 C). These findings provide evidence that above -10 C heterogeneous ice formation in Arctic mixed-phase clouds occurs by a factor of 2-6 more often when the cloud layer is coupled to the surface. In turn, for minimum cloud temperatures below -15 C, the frequency of ice-containing clouds for coupled and decoupled conditions approached the respective curve for the central European site of Leipzig, Germany (51 N, 12 E). This corroborates the hypothesis that the free-tropospheric ice nucleating particle (INP) reservoir over the Arctic is controlled by continental aerosol. Two sensitivity studies, also using the cloud radar for detection of ice particles and applying a modified coupling state detection, both confirmed the findings, albeit with a lower magnitude. Possible explanations for the observations are discussed by considering recent in situ measurements of INP in the Arctic, of which much higher concentrations were found in the surface-coupled atmosphere in close vicinity to the ice shore.
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    First triple-wavelength lidar observations of depolarization and extinction-to-backscatter ratios of Saharan dus
    (Katlenburg-Lindau : EGU, 2022) Haarig, Moritz; Ansmann, Albert; Engelmann, Ronny; Baars, Holger; Toledano, Carlos; Torres, Benjamin; Althausen, Dietrich; Radenz, Martin; Wandinger, Ulla
    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 1064gnm). The pure-dust conditions during the first event exhibit lidar ratios of 47g±g8, 50g±g5 and 69g±g14gsr and particle linear depolarization ratios of 0.242g±g0.024, 0.299g±g0.018 and 0.206g±g0.010 at wavelengths of 355, 532 and 1064gnm, 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 49g±g4, 46g±g5 and 57g±g9gsr and the depolarization ratio of 0.174g±g0.041, 0.298g±g0.016 and 0.242g±g0.007 at 355, 532 and 1064gnm, 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 1064gnm 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.
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    Significant continental source of ice-nucleating particles at the tip of Chile's southernmost Patagonia region
    (Katlenburg-Lindau : EGU, 2022) Gong, Xianda; Radenz, Martin; Wex, Heike; Seifert, Patric; Ataei, Farnoush; Henning, Silvia; Baars, Holger; Barja, Boris; Ansmann, Albert; Stratmann, Frank
    The sources and abundance of ice-nucleating particles (INPs) that initiate cloud ice formation remain understudied, especially in the Southern Hemisphere. In this study, we present INP measurements taken close to Punta Arenas, Chile, at the southernmost tip of South America from May 2019 to March 2020, during the Dynamics, Aerosol, Cloud, And Precipitation Observations in the Pristine Environment of the Southern Ocean (DACAPO-PESO) campaign. The highest ice nucleation temperature was observed at −3◦C, and from this temperature down to ∼ −10◦C, a sharp increase of INP number concentration (NINP) was observed. Heating of the samples revealed that roughly 90 % and 80 % of INPs are proteinaceous-based biogenic particles at > −10 and −15◦C, respectively. The NINP at Punta Arenas is much higher than that in the Southern Ocean, but it is comparable with an agricultural area in Argentina and forestry environment in the US. Ice active surface site density (ns) is much higher than that for marine aerosol in the Southern Ocean, but comparable to English fertile soil dust. Parameterization based on particle number concentration in the size range larger than 500 nm (N>500 nm) from the global average (DeMott et al., 2010) overestimates the measured INP, but the parameterization representing biological particles from a forestry environment (Tobo et al., 2013) yields NINP comparable to this study. No clear seasonal variation of NINP was observed. High precipitation is one of the most important meteorological parameters to enhance the NINP in both cold and warm seasons. A comparison of data from in situ and lidar measurements showed good agreement for concentrations of large aerosol particles (> 500 nm) when assuming continental conditions for retrieval of the lidar data, suggesting that these particles were well mixed within the planetary boundary layer (PBL). This corroborates the continental origin of these particles, consistent with the results from our INP source analysis. Overall, we suggest that a high NINP of biogenic INPs originated from terrestrial sources and were added to the marine air masses during the overflow of a maximum of roughly 150 km of land before arriving at the measurement station.
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    A review of coarse mineral dust in the Earth system
    (Amsterdam [u.a.] : Elsevier, 2022) Adebiyi, Adeyemi; Kok, Jasper F.; Murray, Benjamin J.; Ryder, Claire L.; Stuut, Jan-Berend W.; Kahn, Ralph A.; Knippertz, Peter; Formenti, Paola; Mahowald, Natalie M.; Pérez García-Pando, Carlos; Klose, Martina; Ansmann, Albert; Samset, Bjørn H.; Ito, Akinori; Balkanski, Yves; Di Biagio, Claudia; Romanias, Manolis N.; Huang, Yue; Meng, Jun
    Mineral dust particles suspended in the atmosphere span more than three orders of magnitude in diameter, from <0.1 µm to more than 100 µm. This wide size range makes dust a unique aerosol species with the ability to interact with many aspects of the Earth system, including radiation, clouds, hydrology, atmospheric chemistry, and biogeochemistry. This review focuses on coarse and super-coarse dust aerosols, which we respectively define as dust particles with a diameter of 2.5–10 µm and 10–62.5 µm. We review several lines of observational evidence indicating that coarse and super-coarse dust particles are transported farther than previously expected and that the abundance of these particles is substantially underestimated in current global models. We synthesize previous studies that used observations, theories, and model simulations to highlight the impacts of coarse and super-coarse dust aerosols on the Earth system, including their effects on dust-radiation interactions, dust-cloud interactions, atmospheric chemistry, and biogeochemistry. Specifically, coarse and super-coarse dust aerosols produce a net positive direct radiative effect (warming) at the top of the atmosphere and can modify temperature and water vapor profiles, influencing the distribution of clouds and precipitation. In addition, coarse and super-coarse dust aerosols contribute a substantial fraction of ice-nucleating particles, especially at temperatures above –23 °C. They also contribute a substantial fraction to the available reactive surfaces for atmospheric processing and the dust deposition flux that impacts land and ocean biogeochemistry by supplying important nutrients such as iron and phosphorus. Furthermore, we examine several limitations in the representation of coarse and super-coarse dust aerosols in current model simulations and remote-sensing retrievals. Because these limitations substantially contribute to the uncertainties in simulating the abundance and impacts of coarse and super-coarse dust aerosols, we offer some recommendations to facilitate future studies. Overall, we conclude that an accurate representation of coarse and super-coarse properties is critical in understanding the impacts of dust aerosols on the Earth system.
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    Californian Wildfire Smoke Over Europe: A First Example of the Aerosol Observing Capabilities of Aeolus Compared to Ground‐Based Lidar
    (Hoboken, NJ : Wiley, 2021) Baars, Holger; Radenz, Martin; Floutsi, Athena Augusta; Engelmann, Ronny; Althausen, Dietrich; Heese, Birgit; Ansmann, Albert; Flament, Thomas; Dabas, Alain; Trapon, Dimitri; Reitebuch, Oliver; Bley, Sebastian; Wandinger, Ulla
    In September 2020, extremely strong wildfires in the western United States of America (i.e., mainly in California) produced large amounts of smoke, which was lifted into the free troposphere. These biomass-burning-aerosol (BBA) layers were transported from the US west coast toward central Europe within 3–4 days turning the sky milky and receiving high media attention. The present study characterizes this pronounced smoke plume above Leipzig, Germany, using a ground-based multiwavelength-Raman-polarization lidar and the aerosol/cloud product of ESA’s wind lidar mission Aeolus. An exceptional high smoke-AOT >0.4 was measured, yielding to a mean mass concentration of 8 μg m−3. The 355 nm lidar ratio was moderate at around 40–50 sr. The Aeolus-derived backscatter, extinction and lidar ratio profiles agree well with the observations of the ground-based lidar PollyXT considering the fact that Aeolus’ aerosol and cloud products are still preliminary and subject to ongoing algorithm improvements.