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@ARTICLE{Crowley:857862,
      author       = {Crowley, John N. and Pouvesle, Nicolas and Phillips, Gavin
                      J. and Axinte, Raoul and Fischer, Horst and Petäjä, Tuukka
                      and Nölscher, Anke and Williams, Jonathan and Hens,
                      Korbinian and Harder, Hartwig and Martinez-Harder, Monica
                      and Novelli, Anna and Kubistin, Dagmar and Bohn, Birger and
                      Lelieveld, Jos},
      title        = {{I}nsights into {HO}x and {RO}x chemistry in the boreal
                      forest via measurement of peroxyacetic acid, peroxyacetic
                      nitric anhydride ({PAN}) and hydrogen peroxide},
      journal      = {Atmospheric chemistry and physics},
      volume       = {18},
      number       = {18},
      issn         = {1680-7324},
      address      = {Katlenburg-Lindau},
      publisher    = {EGU},
      reportid     = {FZJ-2018-06825},
      pages        = {13457 - 13479},
      year         = {2018},
      abstract     = {Unlike many oxidised atmospheric trace gases, which have
                      numerous production pathways, peroxyacetic acid (PAA) and
                      PAN are formed almost exclusively in gas-phase reactions
                      involving the hydroperoxy radical (HO2), the acetyl peroxy
                      radical (CH3C(O)O2) and NO2 and are not believed to be
                      directly emitted in significant amounts by vegetation. As
                      the self-reaction of HO2 is the main photochemical route to
                      hydrogen peroxide (H2O2), simultaneous observation of PAA,
                      PAN and H2O2 can provide insight into the HO2 budget. We
                      present an analysis of observations taken during a
                      summertime campaign in a boreal forest that, in addition to
                      natural conditions, was temporarily impacted by two
                      biomass-burning plumes. The observations were analysed using
                      an expression based on a steady-state assumption using
                      relative PAA-to-PAN mixing ratios to derive HO2
                      concentrations. The steady-state approach generated HO2
                      concentrations that were generally in reasonable agreement
                      with measurements but sometimes overestimated those observed
                      by factors of 2 or more. We also used a chemically simple,
                      constrained box model to analyse the formation and reaction
                      of radicals that define the observed mixing ratios of PAA
                      and H2O2. After nudging the simulation towards observations
                      by adding extra, photochemical sources of HO2 and CH3C(O)O2,
                      the box model replicated the observations of PAA, H2O2, ROOH
                      and OH throughout the campaign, including the
                      biomass-burning-influenced episodes during which
                      significantly higher levels of many oxidized trace gases
                      were observed. A dominant fraction of CH3O2 radical
                      generation was found to arise via reactions of the CH3C(O)O2
                      radical. The model indicates that organic peroxy radicals
                      were present at night in high concentrations that sometimes
                      exceeded those predicted for daytime, and initially
                      divergent measured and modelled HO2 concentrations and daily
                      concentration profiles are reconciled when organic peroxy
                      radicals are detected (as HO2) at an efficiency of $35\%.$
                      Organic peroxy radicals are found to play an important role
                      in the recycling of OH radicals subsequent to their loss via
                      reactions with volatile organic compounds.},
      cin          = {IEK-8},
      ddc          = {550},
      cid          = {I:(DE-Juel1)IEK-8-20101013},
      pnm          = {243 - Tropospheric trace substances and their
                      transformation processes (POF3-243)},
      pid          = {G:(DE-HGF)POF3-243},
      typ          = {PUB:(DE-HGF)16},
      UT           = {WOS:000445271300003},
      doi          = {10.5194/acp-18-13457-2018},
      url          = {https://juser.fz-juelich.de/record/857862},
}