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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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    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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    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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    Measurement report: Balloon-borne in situ profiling of Saharan dust over Cyprus with the UCASS optical particle counter
    (Katlenburg-Lindau : European Geosciences Union, 2021) Kezoudi, Maria; Tesche, Matthias; Smith, Helen; Tsekeri, Alexandra; Baars, Holger; Dollner, Maximilian; Estellés, Víctor; Bühl, Johannes; Weinzierl, Bernadett; Ulanowski, Zbigniew; Müller, Detlef; Amiridis, Vassilis
    This paper presents measurements of mineral dust concentration in the diameter range from 0.4 to 14.0 µm with a novel balloon-borne optical particle counter, the Universal Cloud and Aerosol Sounding System (UCASS). The balloon launches were coordinated with ground-based active and passive remote-sensing observations and airborne in situ measurements with a research aircraft during a Saharan dust outbreak over Cyprus from 20 to 23 April 2017. The aerosol optical depth at 500 nm reached values up to 0.5 during that event over Cyprus, and particle number concentrations were as high as 50 cm−3 for the diameter range between 0.8 and 13.9 µm. Comparisons of the total particle number concentration and the particle size distribution from two cases of balloon-borne measurements with aircraft observations show reasonable agreement in magnitude and shape despite slight mismatches in time and space. While column-integrated size distributions from balloon-borne measurements and ground-based remote sensing show similar coarse-mode peak concentrations and diameters, they illustrate the ambiguity related to the missing vertical information in passive sun photometer observations. Extinction coefficient inferred from the balloon-borne measurements agrees with those derived from coinciding Raman lidar observations at height levels with particle number concentrations smaller than 10 cm−3 for the diameter range from 0.8 to 13.9 µm. An overestimation of the UCASS-derived extinction coefficient of a factor of 2 compared to the lidar measurement was found for layers with particle number concentrations that exceed 25 cm−3, i.e. in the centre of the dust plume where particle concentrations were highest. This is likely the result of a variation in the refractive index and the shape and size dependency of the extinction efficiency of dust particles along the UCASS measurements. In the future, profile measurements of the particle number concentration and particle size distribution with the UCASS could provide a valuable addition to the measurement capabilities generally used in field experiments that are focussed on the observation of coarse aerosols and clouds.
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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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    Important role of stratospheric injection height for the distribution and radiative forcing of smoke aerosol from the 2019–2020 Australian wildfires
    (Katlenburg-Lindau : EGU, 2022) Heinold, Bernd; Baars, Holger; Barja, Boris; Christensen, Matthew; Kubin, Anne; Ohneiser, Kevin; Schepanski, Kerstin; Schutgens, Nick; Senf, Fabian; Schrödner, Roland; Villanueva, Diego; Tegen, Ina
    More than 1 Tg smoke aerosol was emitted into the atmosphere by the exceptional 2019–2020 southeastern Australian wildfires. Triggered by the extreme fire heat, several deep pyroconvective events carried the smoke directly into the stratosphere. Once there, smoke aerosol remained airborne considerably longer than in lower atmospheric layers. The thick plumes traveled eastward, thereby being distributed across the high and mid-latitudes in the Southern Hemisphere, enhancing the atmospheric opacity. Due to the increased atmospheric lifetime of the smoke plume, its radiative effect increased compared to smoke that remains in lower altitudes. Global models describing aerosol-climate impacts lack adequate descriptions of the emission height of aerosols from intense wildfires. Here, we demonstrate, by a combination of aerosol-climate modeling and lidar observations, the importance of the representation of those high-altitude fire smoke layers for estimating the atmospheric energy budget. Through observation-based input into the simulations, the Australian wildfire emissions by pyroconvection are explicitly prescribed to the lower stratosphere in different scenarios. Based on our simulations, the 2019–2020 Australian fires caused a significant top-of-atmosphere (TOA) hemispheric instantaneous direct radiative forcing signal that reached a magnitude comparable to the radiative forcing induced by anthropogenic absorbing aerosol. Up to +0.50 W m−2 instantaneous direct radiative forcing was modeled at TOA, averaged for the Southern Hemisphere (+0.25 W m−2 globally) from January to March 2020 under all-sky conditions. At the surface, on the other hand, an instantaneous solar radiative forcing of up to −0.81 W m−2 was found for clear-sky conditions, with the respective estimates depending on the model configuration and subject to the model uncertainties in the smoke optical properties. Since extreme wildfires are expected to occur more frequently in the rapidly changing climate, our findings suggest that high-altitude wildfire plumes must be adequately considered in climate projections in order to obtain reasonable estimates of atmospheric energy budget changes.
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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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    Automated time–height-resolved air mass source attribution for profiling remote sensing applications
    (Katlenburg-Lindau : EGU, 2021) Radenz, Martin; Seifert, Patric; Baars, Holger; Floutsi, Athena Augusta; Yin, Zhenping; Bühl, Johannes
    Height-resolved air mass source attribution is crucial for the evaluation of profiling ground-based remote sensing observations, especially when using lidar (light detection and ranging) to investigate different aerosol types throughout the atmosphere. Lidar networks, such as EARLINET (European Aerosol Research Lidar Network) in the frame of ACTRIS (Aerosol, Clouds and Trace Gases), observe profiles of optical aerosol properties almost continuously, but usually, additional information is needed to support the characterization of the observed particles. This work presents an approach explaining how backward trajectories or particle positions from a dispersion model can be combined with geographical information (a land cover classification and manually defined areas) to obtain a continuous and vertically resolved estimate of an air mass source above a certain location. Ideally, such an estimate depends on as few as possible a priori information and auxiliary data. An automated framework for the computation of such an air mass source is presented, and two applications are described. First, the air mass source information is used for the interpretation of air mass sources for three case studies with lidar observations from Limassol (Cyprus), Punta Arenas (Chile) and ship-borne off Cabo Verde. Second, air mass source statistics are calculated for two multi-week campaigns to assess potential observation biases of lidar-based aerosol statistics. Such an automated approach is a valuable tool for the analysis of short-term campaigns but also for long-term data sets, for example, acquired by EARLINET.