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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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    Comparative study between ground-based observations and NAVGEM-HA analysis data in the mesosphere and lower thermosphere region
    (Katlenburg-Lindau : EGU, 2020) Stober, Gunter; Baumgarten, Kathrin; McCormack, John P.; Brown, Peter; Czarnecki, Jerry
    Recent studies have shown that day-to-day variability of the migrating semidiurnal solar (SW2) tide within the mesosphere and lower thermosphere (MLT) is a key driver of anomalies in the thermosphere-ionosphere system. Here, we study the variability in both the amplitude and phase of SW2 using meteor radar wind and lidar temperature observations at altitudes of 75-110 km as well as wind and temperature output from the Navy Global Environmental Model-High Altitude (NAVGEM-HA), a high-altitude meteorological analysis system. Application of a new adaptive spectral filter technique to both local radar wind observations and global NAVGEM-HA analyses offers an important cross-validation of both data sets and makes it possible to distinguish between migrating and non-migrating tidal components, which is difficult using local measurements alone. Comparisons of NAVGEM-HA, meteor radar and lidar observations over a 12-month period show that the meteorological analyses consistently reproduce the seasonal as well as day-to-day variability in mean winds, mean temperatures and SW2 features from the ground-based observations. This study also examines in detail the day-to-day variability in SW2 during two sudden stratospheric warming, events that have been implicated in producing ionospheric anomalies. During this period, both meteor radar and NAVGEM-HA winds show a significant phase shift and amplitude modulation, but no signs of coupling to the lunar tide as previous studies have suggested. Overall, these findings demonstrate the benefit of combining global high-altitude meteorological analyses with ground-based observations of the MLT region to better understand the tidal variability in the atmosphere. © 2020 Author(s).
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    Aerosol pollution maps and trends over Germany with hourly data at four rural background stations from 2009 to 2018
    (Katlenburg-Lindau : EGU, 2020) Heintzenberg, Jost; Birmili, Wolfram; Hellack, Bryan; Spindler, Gerald; Tuch, Thomas; Wiedensohler, Alfred
    A total of 10 years of hourly aerosol and gas data at four rural German stations have been combined with hourly back trajectories to the stations and inventories of the European Emissions Database for Global Atmospheric Research (EDGAR), yielding pollution maps over Germany of PM10, particle number concentrations, and equivalent black carbon (eBC). The maps reflect aerosol emissions modified with atmospheric processes during transport between sources and receptor sites. Compared to emission maps, strong western European emission centers do not dominate the downwind concentrations because their emissions are reduced by atmospheric processes on the way to the receptor area. PM10, eBC, and to some extent also particle number concentrations are rather controlled by emissions from southeastern Europe from which pollution transport often occurs under drier conditions. Newly formed particles are found in air masses from a broad sector reaching from southern Germany to western Europe, which we explain with gaseous particle precursors coming with little wet scavenging from this region. Annual emissions for 2009 of PM10, BC, SO2, and NOx were accumulated along each trajectory and compared with the corresponding measured time series. The agreement of each pair of time series was optimized by varying monthly factors and annual factors on the 2009 emissions. This approach yielded broader summer emission minima than published values that were partly displaced from the midsummer positions. The validity of connecting the ambient concentration and emission of particulate pollution was tested by calculating temporal changes in eBC for subsets of back trajectories passing over two separate prominent emission regions, region A to the northwest and B to the southeast of the measuring stations. Consistent with reported emission data the calculated emission decreases over region A are significantly stronger than over region B.
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    Long-term profiling of aerosol light extinction, particle mass, cloud condensation nuclei, and ice-nucleating particle concentration over Dushanbe, Tajikistan, in Central Asia
    (Katlenburg-Lindau : EGU, 2020) Hofer, Julian; Ansmann, Albert; Althausen, Dietrich; Engelmann, Ronny; Baars, Holger; Abdullaev, Sabur F.; Makhmudov, Abduvosit N.
    For the first time, continuous, vertically resolved long-term aerosol measurements were conducted with a state-of-the-art multiwavelength lidar over a Central Asian site. Such observations are urgently required in efforts to predict future climate and environmental conditions and to support spaceborne remote sensing (ground truth activities). The lidar observations were performed in the framework of the Central Asian Dust Experiment (CADEX) at Dushanbe, Tajikistan, from March 2015 to August 2016. An AERONET (AErosol RObotic NETwork) sun photometer was operated at the lidar field site. During the 18-month campaign, mixtures of continental aerosol pollution and mineral dust were frequently detected from ground to cirrus height level. Regional sources of dust and pollution as well as long-range transport of mineral dust mainly from Middle Eastern and the Saharan deserts determine the aerosol conditions over Tajikistan. In this study, we summarize our findings and present seasonally resolved statistics regarding aerosol layering (main aerosol layer depth, lofted layer occurrence); optical properties (aerosol and dust optical thicknesses at 500–532 nm, vertically resolved light-extinction coefficient at 532 nm); profiles of dust and non-dust mass concentrations and dust fraction; and profiles of particle parameters relevant for liquid water, mixed-phase cloud, and cirrus formation such as cloud condensation nuclei (CCN) and ice-nucleating particle (INP) concentrations. The main aerosol layer over Dushanbe typically reaches 4–5 km height in spring to autumn. Frequently lofted dust-containing aerosol layers were observed at heights from 5 to 10 km, indicating a sensitive potential of dust to influence cloud ice formation. Typical dust mass fractions were of the order of 60 %–80 %. A considerable fraction is thus anthropogenic pollution and biomass burning smoke. The highest aerosol pollution levels (in the relatively shallow winter boundary layer) occur during the winter months. The seasonal mean 500 nm AOT (aerosol optical thickness) ranges from 0.15 in winter to 0.36 in summer during the CADEX period (March 2015 to August 2016); DOTs (dust optical thicknesses) were usually below 0.2; seasonally mean particle extinction coefficients were of the order of 100–500 Mm−1 in the main aerosol layer during the summer half year and about 100–150 Mm−1 in winter but were mainly caused by anthropogenic haze. Accordingly, the highest dust mass concentrations occurred in the summer season (200–600 µg m−3) and the lowest during the winter months (20–50 µg m−3) in the main aerosol layer. In winter, the aerosol pollution mass concentrations were 20–50 µg m−3, while during the summer half year (spring to autumn), the mass concentration caused by urban haze and biomass burning smoke decreases to 10–20 µg m−3 in the lower troposphere. The CCN concentration levels are always controlled by aerosol pollution. The INP concentrations were found to be high enough in the middle and upper troposphere to significantly influence ice formation in mixed-phase and ice clouds during spring and summer seasons.
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    High number concentrations of transparent exopolymer particles in ambient aerosol particles and cloud water – a case study at the tropical Atlantic Ocean
    (Katlenburg-Lindau : EGU, 2022) van Pinxteren, Manuela; Robinson, Tiera-Brandy; Zeppenfeld, Sebastian; Gong, Xianda; Bahlmann, Enno; Fomba, Khanneh Wadinga; Triesch, Nadja; Stratmann, Frank; Wurl, Oliver; Engel, Anja; Wex, Heike; Herrmann, Hartmut
    Transparent exopolymer particles (TEPs) exhibit the properties of gels and are ubiquitously found in the world oceans. TEPs may enter the atmosphere as part of sea-spray aerosol. Here, we report number concentrations of TEPs with a diameter >4.5 μm, hence covering a part of the supermicron particle range, in ambient aerosol and cloud water samples from the tropical Atlantic Ocean as well as in generated aerosol particles using a plunging waterfall tank that was filled with the ambient seawater. The ambient TEP concentrations ranged between 7×102 and 3×104 #TEP m-3 in the aerosol particles and correlations with sodium (Na+) and calcium (Ca2+) (R2=0.5) suggested some contribution via bubble bursting. Cloud water TEP concentrations were between 4×106 and 9×106 #TEP L-1 and, according to the measured cloud liquid water content, corresponding to equivalent air concentrations of 2-4 × 103 #TEP m-3. Based on Na+ concentrations in seawater and in the atmosphere, the enrichment factors for TEPs in the atmosphere were calculated. The tank-generated TEPs were enriched by a factor of 50 compared with seawater and, therefore, in-line with published enrichment factors for supermicron organic matter in general and TEPs specifically. TEP enrichment in the ambient atmosphere was on average 1×103 in cloud water and 9×103 in ambient aerosol particles and therefore about two orders of magnitude higher than the corresponding enrichment from the tank study. Such high enrichment of supermicron particulate organic constituents in the atmosphere is uncommon and we propose that atmospheric TEP concentrations resulted from a combination of enrichment during bubble bursting transfer from the ocean and a secondary TEP in-situ formation in atmospheric phases. Abiotic in-situ formation might have occurred from aqueous reactions of dissolved organic precursors that were present in particle and cloud water samples, whereas biotic formation involves bacteria, which were abundant in the cloud water samples. The ambient TEP number concentrations were two orders of magnitude higher than recently reported ice nucleating particle (INP) concentrations measured at the same location. As TEPs likely possess good properties to act as INPs, in future experiments it is worth studying if a certain part of TEPs contributes a fraction of the biogenic INP population.
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    Source apportionment and impact of long-range transport on carbonaceous aerosol particles in central Germany during HCCT-2010
    (Katlenburg-Lindau : EGU, 2021) Poulain, Laurent; Fahlbusch, Benjamin; Spindler, Gerald; Mueller, Konrad; van Pinxteren, Dominik; Wu, Zhijun; Iinuma, Yoshiteru; Birmili, Wolfram; Wiedensohler, Alfred; Herrmann, Hartmut
    The identification of different sources of the carbonaceous aerosol (organics and black carbon) was investigated at a mountain forest site located in central Germany from September to October 2010 to characterize incoming air masses during the Hill Cap Cloud Thuringia 2010 (HCCT-2010) experiment. The near-PM1 chemical composition, as measured by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), was dominated by organic aerosol (OA; 41 %) followed by sulfate (19 %) and nitrate (18 %). Source apportionment of the OA fraction was performed using the multilinear engine (ME-2) approach, resulting in the identification of the following five factors: hydrocarbon-like OA (HOA; 3 % of OA mass), biomass burning OA (BBOA; 13 %), semi-volatile-like OA (SV-OOA; 19 %), and two oxygenated OA (OOA) factors. The more oxidized OOA (MO-OOA, 28 %) was interpreted as being influenced by aged, polluted continental air masses, whereas the less oxidized OOA (LO-OOA, 37 %) was found to be more linked to aged biogenic sources. Equivalent black carbon (eBC), measured by a multi-angle absorption photometer (MAAP) represented 10 % of the total particulate matter (PM). The eBC was clearly associated with HOA, BBOA, and MO-OOA factors (all together R2=0.83). Therefore, eBC's contribution to each factor was achieved using a multi-linear regression model. More than half of the eBC (52 %) was associated with long-range transport (i.e., MO-OOA), whereas liquid fuel eBC (35 %) and biomass burning eBC (13 %) were associated with local emissions, leading to a complete apportionment of the carbonaceous aerosol. The separation between local and transported eBC was well supported by the mass size distribution of elemental carbon (EC) from Berner impactor samples. Air masses with the strongest marine influence, based on back trajectory analysis, corresponded with a low particle mass concentration (6.4–7.5 µg m−3) and organic fraction (≈30 %). However, they also had the largest contribution of primary OA (HOA ≈ 4 % and BBOA 15 %–20 %), which was associated with local emissions. Continental air masses had the highest mass concentration (11.4–12.6 µg m−3), and a larger fraction of oxygenated OA (≈45 %) indicated highly processed OA. The present results emphasize the key role played by long-range transport processes not only in the OA fraction but also in the eBC mass concentration and the importance of improving our knowledge on the identification of eBC sources.
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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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    Optical properties of Central Asian aerosol relevant for spaceborne lidar applications and aerosol typing at 355 and 532nm
    (Katlenburg-Lindau : EGU, 2020) Hofer, Julian; Ansmann, Albert; Althausen, Dietrich; Engelmann, Ronny; Baars, Holger; Fomba, Khanneh Wadinga; Wandinger, Ulla; Abdullaev, Sabur F.; Makhmudov, Abduvosit N.
    For the first time, a dense data set of particle extinction-to-backscatter ratios (lidar ratios), linear depolarization ratios, and backscatter- and extinction-related Ångström exponents for a Central Asian site are presented. The observations were performed with a continuously running multiwavelength polarization Raman lidar at Dushanbe, Tajikistan, during an 18-month campaign (March 2015 to August 2016). The presented seasonally resolved observations fill an important gap in the database of aerosol optical properties used in aerosol typing efforts with spaceborne lidars and ground-based lidar networks. Lidar ratios and depolarization ratios are also basic input parameters in spaceborne lidar data analyses and in efforts to harmonize long-term observations with different space lidar systems operated at either 355 or 532 nm. As a general result, the found optical properties reflect the large range of occurring aerosol mixtures consisting of long-range-transported dust (from the Middle East and the Sahara), regional desert, soil, and salt dust, and anthropogenic pollution. The full range from highly polluted to pure dust situations could be observed. Typical dust depolarization ratios of 0.23–0.29 (355 nm) and 0.30–0.35 (532 nm) were observed. In contrast, comparably low lidar ratios were found. Dust lidar ratios at 532 nm accumulated around 35–40 sr and were even lower for regional background dust conditions (20–30 sr). Detailed correlation studies (e.g., lidar ratio vs. depolarization ratios, Ångström exponent vs. lidar ratio and vs. depolarization ratio) are presented to illuminate the complex relationships between the observed optical properties and to identify the contributions of anthropogenic haze, dust, and background aerosol to the overall aerosol mixtures found within the 18-month campaign. The observation of 532 nm lidar ratios (<25 sr) and depolarization ratios (around 15 %–20 %) in layers with very low particle extinction coefficient (<30 sr) suggests that direct emission and emission of resuspended salt dust (initially originated from numerous desiccating lakes and the Aralkum desert) have a sensitive impact on the aerosol background optical properties over Dushanbe.
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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
    (Katlenburg-Lindau : EGU, 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.
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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
    (Katlenburg-Lindau : EGU, 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.