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    Terrestrial or marine – indications towards the origin of ice-nucleating particles during melt season in the European Arctic up to 83.7° N
    (Katlenburg-Lindau : European Geosciences Union, 2021) Hartmann, Markus; Gong, Xianda; Kecorius, Simonas; van Pinxteren, Manuela; Vogl, Teresa; Welti, André; Wex, Heike; Zeppenfeld, Sebastian; Herrmann, Hartmut; Wiedensohler, Alfred; Stratmann, Frank
    Ice-nucleating particles (INPs) initiate the primary ice formation in clouds at temperatures above ca. -38gC and have an impact on precipitation formation, cloud optical properties, and cloud persistence. Despite their roles in both weather and climate, INPs are not well characterized, especially in remote regions such as the Arctic. We present results from a ship-based campaign to the European Arctic during May to July 2017. We deployed a filter sampler and a continuous-flow diffusion chamber for offline and online INP analyses, respectively. We also investigated the ice nucleation properties of samples from different environmental compartments, i.e., the sea surface microlayer (SML), the bulk seawater (BSW), and fog water. Concentrations of INPs (NINP) in the air vary between 2 to 3 orders of magnitudes at any particular temperature and are, except for the temperatures above -10gC and below -32gC, lower than in midlatitudes. In these temperature ranges, INP concentrations are the same or even higher than in the midlatitudes. By heating of the filter samples to 95gC for 1ĝ€¯h, we found a significant reduction in ice nucleation activity, i.e., indications that the INPs active at warmer temperatures are biogenic. At colder temperatures the INP population was likely dominated by mineral dust. The SML was found to be enriched in INPs compared to the BSW in almost all samples. The enrichment factor (EF) varied mostly between 1 and 10, but EFs as high as 94.97 were also observed. Filtration of the seawater samples with 0.2ĝ€¯μm syringe filters led to a significant reduction in ice activity, indicating the INPs are larger and/or are associated with particles larger than 0.2ĝ€¯μm. A closure study showed that aerosolization of SML and/or seawater alone cannot explain the observed airborne NINP unless significant enrichment of INP by a factor of 105 takes place during the transfer from the ocean surface to the atmosphere. In the fog water samples with -3.47gC, we observed the highest freezing onset of any sample. A closure study connecting NINP in fog water and the ambient NINP derived from the filter samples shows good agreement of the concentrations in both compartments, which indicates that INPs in the air are likely all activated into fog droplets during fog events. In a case study, we considered a situation during which the ship was located in the marginal sea ice zone and NINP levels in air and the SML were highest in the temperature range above -10gC. Chlorophyll a measurements by satellite remote sensing point towards the waters in the investigated region being biologically active. Similar slopes in the temperature spectra suggested a connection between the INP populations in the SML and the air. Air mass history had no influence on the observed airborne INP population. Therefore, we conclude that during the case study collected airborne INPs originated from a local biogenic probably marine source. © Author(s) 2021.
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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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    Importance of size representation and morphology in modelling optical properties of black carbon: comparison between laboratory measurements and model simulations
    (Katlenburg-Lindau : Copernicus, 2022) Romshoo, Baseerat; Pöhlker, Mira; Wiedensohler, Alfred; Pfeifer, Sascha; Saturno, Jorge; Nowak, Andreas; Ciupek, Krzysztof; Quincey, Paul; Vasilatou, Konstantina; Ess, Michaela N.; Gini, Maria; Eleftheriadis, Konstantinos; Robins, Chris; Gaie-Levrel, François; Müller, Thomas
    Black carbon (BC) from incomplete combustion of biomass or fossil fuels is the strongest absorbing aerosol component in the atmosphere. Optical properties of BC are essential in climate models for quantification of their impact on radiative forcing. The global climate models, however, consider BC to be spherical particles, which causes uncertainties in their optical properties. Based on this, an increasing number of model-based studies provide databases and parameterization schemes for the optical properties of BC, using more realistic fractal aggregate morphologies. In this study, the reliability of the different modelling techniques of BC was investigated by comparing them to laboratory measurements. The modelling techniques were examined for bare BC particles in the first step and for BC particles with organic material in the second step. A total of six morphological representations of BC particles were compared, three each for spherical and fractal aggregate morphologies. In general, the aggregate representation performed well for modelling the particle light absorption coefficient σabs, single-scattering albedo SSA, and mass absorption cross-section MACBC for laboratory-generated BC particles with volume mean mobility diameters dp,V larger than 100nm. However, for modelling Ångström absorption exponent AAE, it was difficult to suggest a method due to size dependence, although the spherical assumption was in better agreement in some cases. The BC fractal aggregates are usually modelled using monodispersed particles, since their optical simulations are computationally expensive. In such studies, the modelled optical properties showed a 25% uncertainty in using the monodisperse size method. It is shown that using the polydisperse size distribution in combination with fractal aggregate morphology reduces the uncertainty in measured σabs to 10% for particles with dp,V between 60-160nm. Furthermore, the sensitivities of the BC optical properties to the various model input parameters such as the real and imaginary parts of the refractive index (mre and mim), the fractal dimension (Df), and the primary particle radius (app) of an aggregate were investigated. When the BC particle is small and rather fresh, the change in the Df had relatively little effect on the optical properties. There was, however, a significant relationship between app and the particle light scattering, which increased by a factor of up to 6 with increasing total particle size. The modelled optical properties of BC are well aligned with laboratory-measured values when the following assumptions are used in the fractal aggregate representation: mre between 1.6 and 2, mim between 0.50 and 1, Df from 1.7 to 1.9, and app between 10 and 14nm. Overall, this study provides experimental support for emphasizing the importance of an appropriate size representation (polydisperse size method) and an appropriate morphological representation for optical modelling and parameterization scheme development of BC.
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    The potential of elastic and polarization lidars to retrieve extinction profiles
    (Katlenburg-Lindau : Copernicus, 2020) Giannakaki, Elina; Kokkalis, Panos; Marinou, Eleni; Bartsotas, Nikolaos S.; Amiridis, Vassilis; Ansmann, Albert; Komppula, Mika
    A new method, called ElEx (elastic extinction), is proposed for the estimation of extinction coefficient lidar profiles using only the information provided by the elastic and polarization channels of a lidar system. The method is applicable to lidar measurements both during daytime and nighttime under well-defined aerosol mixtures. ElEx uses the particle backscatter profiles at 532 nm and the vertically resolved particle linear depolarization ratio measurements at the same wavelength. The particle linear depolarization ratio and the lidar ratio values of pure aerosol types are also taken from literature. The total extinction profile is then estimated and compared well with Raman retrievals. In this study, ElEx was applied in an aerosol mixture of marine and dust particles at Finokalia station during the CHARADMExp campaign. Any difference between ElEx and Raman extinction profiles indicates that the nondust component could be probably attributed to polluted marine or polluted continental aerosols. Comparison with sun photometer aerosol optical depth observations is performed as well during daytime. Differences in the total aerosol optical depth are varying between 1.2 % and 72 %, and these differences are attributed to the limited ability of the lidar to correctly represent the aerosol optical properties in the near range due to the overlap problem. © 2020 Author(s).
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    Application of the shipborne remote sensing supersite OCEANET for profiling of Arctic aerosols and clouds during Polarstern cruise PS106
    (Katlenburg-Lindau : Copernicus, 2020) Griesche, Hannes J.; Seifer, Patric; Ansmann, Albert; Baars, Holger; Velasco, Carola Barrientos; Bühl, Johannes; Engelmann, Ronny; Radenz, Martin; Zhenping, Yin; Macke, Andreas
    From 25 May to 21 July 2017, the research vessel Polarstern performed the cruise PS106 to the high Arctic in the region north and northeast of Svalbard. The mobile remote-sensing platform OCEANET was deployed aboard Polarstern. Within a single container, OCEANET houses state-of-the-art remote-sensing equipment, including a multiwavelength Raman polarization lidar PollyXT and a 14-channel microwave radiometer HATPRO (Humidity And Temperature PROfiler). For the cruise PS106, the measurements were supplemented by a motion-stabilized 35 GHz cloud radar Mira-35. This paper describes the treatment of technical challenges which were immanent during the deployment of OCEANET in the high Arctic. This includes the description of the motion stabilization of the cloud radar Mira-35 to ensure vertical-pointing observations aboard the moving Polarstern as well as the applied correction of the vessels heave rate to provide valid Doppler velocities. The correction ensured a leveling accuracy of ±0.5◦ during transits through the ice and an ice floe camp. The applied heave correction reduced the signal induced by the vertical movement of the cloud radar in the PSD of the Doppler velocity by a factor of 15. Low-level clouds, in addition, frequently prevented a continuous analysis of cloud conditions from synergies of lidar and radar within Cloudnet, because the technically determined lowest detection height of Mira-35 was 165 m above sea level. To overcome this obstacle, an approach for identification of the cloud presence solely based on data from the near-field receiver of PollyXT at heights from 50 m and 165 m above sea level is presented. We found low-level stratus clouds, which were below the lowest detection range of most automatic ground-based remote-sensing instruments during 25 % of the observation time. We present case studies of aerosol and cloud studies to introduce the capabilities of the data set. In addition, new approaches for ice crystal effective radius and eddy dissipation rates from cloud radar measurements and the retrieval of aerosol optical and microphysical properties from the observations of PollyXT are introduced. © Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License.
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    Is the near-spherical shape the "new black" for smoke?
    (Katlenburg-Lindau : EGU, 2020) Gialitaki, Anna; Tsekeri, Alexandra; Amiridis, Vassilis; Ceolato, Romain; Paulien, Lucas; Kampouri, Anna; Gkikas, Antonis; Solomos, Stavros; Marinou, Eleni; Haarig, Moritz; Baars, Holger; Ansmann, Albert; Lapyonok, Tatyana; Lopatin, Anton; Dubovik, Oleg; Groß, Silke; Wirth, Martin; Tsichla, Maria; Tsikoudi, Ioanna; Balis, Dimitris
    We examine the capability of near-sphericalshaped particles to reproduce the triple-wavelength particle linear depolarization ratio (PLDR) and lidar ratio (LR) values measured over Europe for stratospheric smoke originating from Canadian wildfires. The smoke layers were detected both in the troposphere and the stratosphere, though in the latter case the particles presented PLDR values of almost 18% at 532 nm as well as a strong spectral dependence from the UV to the near-IR wavelength. Although recent simulation studies of rather complicated smoke particle morphologies have shown that heavily coated smoke aggregates can produce large PLDR, herein we propose a much simpler model of compact near-spherical smoke particles. This assumption allows for the reproduction of the observed intensive optical properties of stratospheric smoke, as well as their spectral dependence. We further examine whether an extension of the current Aerosol Robotic Network (AERONET) scattering model to include the near-spherical shapes could be of benefit to the AERONET retrieval for stratospheric smoke cases associated with enhanced PLDR. Results of our study illustrate the fact that triple-wavelength PLDR and LR lidar measurements can provide us with additional insight when it comes to particle characterization. © 2020 Author(s).
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    Optical and geometrical aerosol particle properties over the United Arab Emirates
    (Katlenburg-Lindau : EGU, 2020) Filioglou, Maria; Giannakaki, Elina; Backman, John; Kesti, Jutta; Hirsikko, Anne; Engelmann, Ronny; O’Connor, Ewan; Leskinen, Jari T.T.; Shang, Xiaoxia; Korhonen, Hannele; Lihavainen, Heikki; Romakkaniemi, Sami; Komppula, Mika
    One year of ground-based night-time Raman lidar observations has been analysed under the Optimization of Aerosol Seeding In rain enhancement Strategies (OASIS) project, in order to characterize the aerosol particle properties over a rural site in the United Arab Emirates. In total, 1130 aerosol particle layers were detected during the 1-year measurement campaign which took place between March 2018 and February 2019. Several subsequent aerosol layers could be observed simultaneously in the atmosphere up to 11 km. The observations indicate that the measurement site is a receptor of frequent dust events, but predominantly the dust is mixed with aerosols of anthropogenic and/or marine origin. The mean aerosol optical depth over the measurement site ranged at 0.37±0.12 and 0.21±0.11 for 355 and 532 nm, respectively. Moreover, mean lidar ratios of 43±11 sr at a wavelength of 355 nm and 39±10 sr at 532 nm were found. The average linear particle depolarization ratio measured over the course of the campaign was 15±6% and 19±7% at the 355 and 532 nm wavelengths, respectively. Since the region is both a source and a receptor of mineral dust, we have also explored the properties of Arabian mineral dust of the greater area of the United Arab of Emirates and the Arabian Peninsula. The observed Arabian dust particle properties were 45±5 (42±5) sr at 355 (532) nm for the lidar ratio, 25±2% (31±2 %) for the linear particle depolarization ratio at 355 (532) nm, and 0.3±0.2 (0.2±0.2) for the extinction-related Angstrom exponent (backscatterrelated Angstrom exponent) between 355 and 532 nm. This study is the first to report comprehensive optical properties of the Arabian dust particles based on 1-year long observations, using to their fullest the capabilities of a multi-wavelength Raman lidar instrument. The results suggest that the mineral dust properties over the Middle East and western Asia, including the observation site, are comparable to those of African mineral dust with regard to the particle depolarization ratios, but not for lidar ratios. The smaller lidar ratio values in this study compared to the reference studies are attributed to the difference in the geochemical characteristics of the soil originating in the study region compared to northern Africa. © 2020 Royal Society of Chemistry. All rights reserved.
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    Multidecadal trend analysis of in situ aerosol radiative properties around the world
    (Katlenburg-Lindau : EGU, 2020) Collaud Coen, Martine; Andrews, Elisabeth; Alastuey, Andrés; Petkov Arsov, Todor; Backman, John; Brem, Benjamin T.; Bukowiecki, Nicolas; Couret, Cédric; Eleftheriadis, Konstantinos; Flentje, Harald; Fiebig, Markus; Gysel-Beer, Martin; Hand, Jenny L.; Hoffer, András; Hooda, Rakesh; Hueglin, Christoph; Joubert, Warren; Keywood, Melita; Eun Kim, Jeong; Kim, Sang-Woo; Labuschagne, Casper; Lin, Neng-Huei; Lin, Yong; Lund Myhre, Cathrine; Luoma, Krista; Lyamani, Hassan; Marinoni, Angela; Mayol-Bracero, Olga L.; Mihalopoulos, Nikos; Pandolfi, Marco; Prats, Natalia; Prenni, Anthony J.; Putaud, Jean-Philippe; Ries, Ludwig; Reisen, Fabienne; Sellegri, Karine; Sharma, Sangeeta; Sheridan, Patrick; Sherman, James Patrick; Sun, Junying; Titos, Gloria; Torres, Elvis; Tuch, Thomas; Weller, Rolf; Wiedensohler, Alfred; Zieger, Paul; Laj, Paolo
    In order to assess the evolution of aerosol parameters affecting climate change, a long-term trend analysis of aerosol optical properties was performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Ångström exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann-Kendall (MK) statistical test associated with several pre-whitening methods and with Sen's slope was used as the main trend analysis method. Comparisons with general least mean square associated with autoregressive bootstrap (GLS/ARB) and with standard least mean square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficient trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficient time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, eastern/northern Europe and the Arctic, 22 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 26 % of sites have trends which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10-year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10-year trends are primarily found for earlier periods (10-year trends ending in 2010-2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10-year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10-year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10-year trends of the scattering coefficient - there is a shift to statistically significant negative trends in 2009-2012 for all stations in the eastern and central USA. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage provides insight into potential aerosol effects on climate changes. © 2020 Royal Society of Chemistry. All rights reserved.