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@ARTICLE{Rosanka:902278,
      author       = {Rosanka, Simon and Sander, Rolf and Franco, Bruno and
                      Wespes, Catherine and Wahner, Andreas and Taraborrelli,
                      Domenico},
      title        = {{O}xidation of low-molecular weight organic compounds in
                      cloud droplets: global impact on tropospheric oxidants},
      journal      = {Atmospheric chemistry and physics / Discussions},
      volume       = {},
      issn         = {1680-7367},
      address      = {Katlenburg-Lindau},
      publisher    = {EGU},
      reportid     = {FZJ-2021-04141},
      pages        = {},
      year         = {2020},
      abstract     = {In liquid cloud droplets, superoxide anion (O−2(aq)) is
                      known to quickly consume ozone (O3(aq)), which is relatively
                      insoluble. The significance of this reaction as tropospheric
                      O3 sink is sensitive to the abundance of O−2(aq) and
                      therefore to the production of its main precursor,
                      hydroperoxyl radical (HO2(aq)). The aqueous-phase oxidation
                      of oxygenated volatile organic compounds (OVOCs) is the
                      major source of HO2(aq) in cloud droplets. Hence, the lack
                      of explicit aqueous-phase chemical kinetics in global
                      atmospheric models leads to a general underestimation of
                      clouds as O3 sinks. In this study, the importance of
                      in-cloud OVOC oxidation for tropospheric composition is
                      assessed by using the Chemistry As A Boxmodel Application
                      (CAABA) and the global atmospheric model ECHAM/MESSy (EMAC),
                      which are both capable of explicitly representing the
                      relevant chemical transformations. For this analysis, three
                      different in-cloud oxidation mechanisms are employed: (1)
                      one including the basic oxidation of SO2(aq) via O3(aq) and
                      H2O2(aq), which thus represents the capabilities of most
                      global models, (2) the more advanced standard EMAC
                      mechanism, which includes inorganic chemistry and simplified
                      degradation of methane oxidation products, and (3) the
                      detailed in-cloud OVOC oxidation scheme Jülich
                      Aqueous-phase Mechanism of Organic Chemistry (JAMOC). By
                      using EMAC, the global impact of each mechanism is assessed
                      focusing mainly on tropospheric volatile organic compounds
                      (VOCs), HOx (HOx = OH+HO2), and O3. This is achieved by
                      performing a detailed HOx and O3 budget analysis in the gas-
                      and aqueous-phase. The resulting changes are evaluated
                      against O3 and methanol (CH3OH) satellite observations from
                      the Infrared Atmospheric Sounding Interferometer (IASI) for
                      2015. In general, the explicit in-cloud oxidation leads to
                      an overall reduction of predicted OVOCs levels, and reduces
                      EMAC's overestimation of some OVOCs in the tropics. The
                      in-cloud OVOC oxidation shifts the HO2 production from the
                      gas- to the aqueous-phase. As a result, the O3 budget is
                      perturbed with scavenging being enhanced and the gas-phase
                      chemical losses being reduced. With the simplified in-cloud
                      chemistry, about 13 Tg a−1 of O3 are scavenged, which
                      increases to 336 Tg a−1 when JAMOC is used. The highest O3
                      reduction of 12 $\%$ is predicted in the upper
                      troposphere/lower stratosphere (UTLS). These changes in the
                      free troposphere significantly reduce the modelled
                      tropospheric ozone columns, which are known to be generally
                      overestimated by EMAC and other global atmospheric models.},
      cin          = {IEK-8},
      ddc          = {550},
      cid          = {I:(DE-Juel1)IEK-8-20101013},
      pnm          = {2111 - Air Quality (POF4-211)},
      pid          = {G:(DE-HGF)POF4-2111},
      typ          = {PUB:(DE-HGF)16},
      doi          = {10.5194/acp-2020-1041},
      url          = {https://juser.fz-juelich.de/record/902278},
}