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    Detection and attribution of aerosol-cloud interactions in large-domain large-eddy simulations with the ICOsahedral Non-hydrostatic model
    (Katlenburg-Lindau : EGU, 2020) Costa-Surós, Montserrat; Sourdeval, Odran; Acquistapace, Claudia; Baars, Holger; Carbajal Henken, Cintia; Genz, Christa; Hesemann, Jonas; Jimenez, Cristofer; König, Marcel; Kretzschmar, Jan; Madenach, Nils; Meyer, Catrin I.; Schrödner, Roland; Seifert, Patric; Senf, Fabian; Brueck, Matthias; Cioni, Guido; Engels, Jan Frederik; Fieg, Kerstin; Gorges, Ksenia; Heinze, Rieke; Kumar Siligam, Pavan; Burkhardt, Ulrike; Crewell, Susanne; Hoose, Corinna; Seifert, Axel; Tegen, Ina; Quaas, Johannes
    Clouds and aerosols contribute the largest uncertainty to current estimates and interpretations of the Earth's changing energy budget. Here we use a new-generation large-domain large-eddy model, ICON-LEM (ICOsahedral Non-hydrostatic Large Eddy Model), to simulate the response of clouds to realistic anthropogenic perturbations in aerosols serving as cloud condensation nuclei (CCN). The novelty compared to previous studies is that (i) the LEM is run in weather prediction mode and with fully interactive land surface over a large domain and (ii) a large range of data from various sources are used for the detection and attribution. The aerosol perturbation was chosen as peak-aerosol conditions over Europe in 1985, with more than fivefold more sulfate than in 2013. Observational data from various satellite and ground-based remote sensing instruments are used, aiming at the detection and attribution of this response. The simulation was run for a selected day (2 May 2013) in which a large variety of cloud regimes was present over the selected domain of central Europe. It is first demonstrated that the aerosol fields used in the model are consistent with corresponding satellite aerosol optical depth retrievals for both 1985 (perturbed) and 2013 (reference) conditions. In comparison to retrievals from groundbased lidar for 2013, CCN profiles for the reference conditions were consistent with the observations, while the ones for the 1985 conditions were not. Similarly, the detection and attribution process was successful for droplet number concentrations: the ones simulated for the 2013 conditions were consistent with satellite as well as new ground-based lidar retrievals, while the ones for the 1985 conditions were outside the observational range. For other cloud quantities, including cloud fraction, liquid water path, cloud base altitude and cloud lifetime, the aerosol response was small compared to their natural vari ability. Also, large uncertainties in satellite and ground-based observations make the detection and attribution difficult for these quantities. An exception to this is the fact that at a large liquid water path value (LWP > 200 g m-2), the control simulation matches the observations, while the perturbed one shows an LWP which is too large. The model simulations allowed for quantifying the radiative forcing due to aerosol-cloud interactions, as well as the adjustments to this forcing. The latter were small compared to the variability and showed overall a small positive radiative effect. The overall effective radiative forcing (ERF) due to aerosol-cloud interactions (ERFaci) in the simulation was dominated thus by the Twomey effect and yielded for this day, region and aerosol perturbation-2:6 W m-2. Using general circulation models to scale this to a global-mean present-day vs. pre-industrial ERFaci yields a global ERFaci of-0:8 W m-2 © 2020 Author(s).
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    Marine organic matter in the remote environment of the Cape Verde islands-an introduction and overview to the MarParCloud campaign
    (Katlenburg-Lindau : EGU, 2020) van Pinxteren, Manuela; Fomba, KhannehWadinga; Triesch, Nadja; Stolle, Christian; Wurl, Oliver; Bahlmann, Enno; Gong, Xianda; Voigtländer, Jens; Wex, Heike; Robinson, Tiera-Brandy; Barthel, Stefan; Zeppenfeld, Sebastian; Hoffmann, Erik Hans; Roveretto, Marie; Li, Chunlin; Grosselin, Benoit; Daële, Veronique; Senf, Fabian; van Pinxteren, Dominik; Manzi, Malena; Zabalegui, Nicolás; Frka, Sanja; Gašparović, Blaženka; Pereira, Ryan; Li, Tao; Wen, Liang; Li, Jiarong; Zhu, Chao; Chen, Hui; Chen, Jianmin; Fiedler, Björn; von Tümpling, Wolf; Read, Katie Alana; Punjabi, Shalini; Lewis, Alastair Charles; Hopkins, James Roland; Carpenter, Lucy Jane; Peeken, Ilka; Rixen, Tim; Schulz-Bull, Detlef; Mong, María Eugenia; Mellouki, Abdelwahid; George, Christian; Stratmann, Frank; Herrmann, Hartmut
    The project MarParCloud (Marine biological production, organic aerosol Particles and marine Clouds: a process chain) aims to improve our understanding of the genesis, modification and impact of marine organic matter (OM) from its biological production, to its export to marine aerosol particles and, finally, to its ability to act as ice-nucleating particles (INPs) and cloud condensation nuclei (CCN). A field campaign at the Cape Verde Atmospheric Observatory (CVAO) in the tropics in September-October 2017 formed the core of this project that was jointly performed with the project MARSU (MARine atmospheric Science Unravelled). A suite of chemical, physical, biological and meteorological techniques was applied, and comprehensive measurements of bulk water, the sea surface microlayer (SML), cloud water and ambient aerosol particles collected at a ground-based and a mountain station took place. Key variables comprised the chemical characterization of the atmospherically relevant OM components in the ocean and the atmosphere as well as measurements of INPs and CCN. Moreover, bacterial cell counts, mercury species and trace gases were analyzed. To interpret the results, the measurements were accompanied by various auxiliary parameters such as air mass back-trajectory analysis, vertical atmospheric profile analysis, cloud observations and pigment measurements in seawater. Additional modeling studies supported the experimental analysis. During the campaign, the CVAO exhibited marine air masses with low and partly moderate dust influences. The marine boundary layer was well mixed as indicated by an almost uniform particle number size distribution within the boundary layer. Lipid biomarkers were present in the aerosol particles in typical concentrations of marine background conditions. Accumulation-and coarse-mode particles served as CCN and were efficiently transferred to the cloud water. The ascent of ocean-derived compounds, such as sea salt and sugar-like compounds, to the cloud level, as derived from chemical analysis and atmospheric transfer modeling results, denotes an influence of marine emissions on cloud formation. Organic nitrogen compounds (free amino acids) were enriched by several orders of magnitude in submicron aerosol particles and in cloud water compared to seawater. However, INP measurements also indicated a significant contribution of other non-marine sources to the local INP concentration, as (biologically active) INPs were mainly present in supermicron aerosol particles that are not suggested to undergo strong enrichment during ocean-atmosphere transfer. In addition, the number of CCN at the supersaturation of 0.30 % was about 2.5 times higher during dust periods compared to marine periods. Lipids, sugar-like compounds, UV-absorbing (UV: ultraviolet) humic-like substances and low-molecularweight neutral components were important organic compounds in the seawater, and highly surface-active lipids were enriched within the SML. The selective enrichment of specific organic compounds in the SML needs to be studied in further detail and implemented in an OM source function for emission modeling to better understand transfer patterns, the mechanisms of marine OM transformation in the atmosphere and the role of additional sources. In summary, when looking at particulate mass, we see oceanic compounds transferred to the atmospheric aerosol and to the cloud level, while from a perspective of particle number concentrations, sea spray aerosol (i.e., primary marine aerosol) contributions to both CCN and INPs are rather limited. © Author(s) 2020.