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@ARTICLE{Rosanka:902281,
      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},
      volume       = {21},
      number       = {12},
      issn         = {1680-7324},
      address      = {Katlenburg-Lindau},
      publisher    = {EGU},
      reportid     = {FZJ-2021-04144},
      pages        = {9909 - 9930},
      year         = {2021},
      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 a
                      tropospheric O3 sink is sensitive to the abundance of
                      O−2(aq) and therefore to the production of its main
                      precursor, the 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 ECHAM/MESSy Atmospheric
                      Chemistry (EMAC) model, 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)
                      by 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 in predicted OVOC 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 yr−1 of O3 is scavenged, which
                      increases to 336 Tg yr−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},
      UT           = {WOS:000670319200004},
      doi          = {10.5194/acp-21-9909-2021},
      url          = {https://juser.fz-juelich.de/record/902281},
}