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    The Importance of the Representation of DMS Oxidation in Global Chemistry‐Climate Simulations
    (Hoboken, NJ : Wiley, 2021) Hoffmann, Erik Hans; Heinold, Bernd; Kubin, Anne; Tegen, Ina; Herrmann, Hartmut
    The oxidation of dimethyl sulfide (DMS) is key for the natural sulfate aerosol formation and its climate impact. Multiphase chemistry is an important oxidation pathway but neglected in current chemistry-climate models. Here, the DMS chemistry in the aerosol-chemistry-climate model ECHAM-HAMMOZ is extended to include multiphase methane sulfonic acid (MSA) formation in deliquesced aerosol particles, parameterized by reactive uptake. First simulations agree well with observed gas-phase MSA concentrations. The implemented formation pathways are quantified to contribute up to 60% to the sulfate aerosol burden over the Southern Ocean and Arctic/Antarctic regions. While globally the impact on the aerosol radiative forcing almost levels off, a significantly more positive solar radiative forcing of up to +0.1 W m−2 is computed in the Arctic (>60°N). The findings imply the need of both further laboratory and model studies on the atmospheric multiphase oxidation of DMS.
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    Combining atmospheric and snow radiative transfer models to assess the solar radiative effects of black carbon in the Arctic
    (Katlenburg-Lindau : EGU, 2020) Donth, Tobias; Jäkel, Evelyn; Ehrlich, André; Heinold, Bernd; Schacht, Jacob; Herber, Andreas; Zanatta, Marco; Wendisch, Manfred
    The magnitude of solar radiative effects (cooling or warming) of black carbon (BC) particles embedded in the Arctic atmosphere and surface snow layer was explored on the basis of case studies. For this purpose, combined atmospheric and snow radiative transfer simulations were performed for cloudless and cloudy conditions on the basis of BC mass concentrations measured in pristine early summer and more polluted early spring conditions. The area of interest is the remote sea-ice-covered Arctic Ocean in the vicinity of Spitsbergen, northern Greenland, and northern Alaska typically not affected by local pollution. To account for the radiative interactions between the black-carbon-containing snow surface layer and the atmosphere, an atmospheric and snow radiative transfer model were coupled iteratively. For pristine summer conditions (no atmospheric BC, minimum solar zenith angles of 55 ) and a representative BC particle mass concentration of 5 ng g-1 in the surface snow layer, a positive daily mean solar radiative forcing of +0.2 W m-2 was calculated for the surface radiative budget. A higher load of atmospheric BC representing early springtime conditions results in a slightly negative mean radiative forcing at the surface of about -0.05 W m-2, even when the low BC mass concentration measured in the pristine early summer conditions was embedded in the surface snow layer. The total net surface radiative forcing combining the effects of BC embedded in the atmosphere and in the snow layer strongly depends on the snow optical properties (snow specific surface area and snow density). For the conditions over the Arctic Ocean analyzed in the simulations, it was found that the atmospheric heating rate by water vapor or clouds is 1 to 2 orders of magnitude larger than that by atmospheric BC. Similarly, the daily mean total heating rate (6 K d-1) within a snowpack due to absorption by the ice was more than 1 order of magnitude larger than that of atmospheric BC (0.2 K d-1). Also, it was shown that the cooling by atmospheric BC of the near-surface air and the warming effect by BC embedded in snow are reduced in the presence of clouds. © 2020 Copernicus GmbH. All rights reserved.