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@PHDTHESIS{Kaminski:151374,
      author       = {Kaminski, Martin},
      title        = {{U}ntersuchung des photochemischen {T}erpenoidabbaus in der
                      {A}tmosphärensimulationskammer {SAPHIR}},
      volume       = {218},
      school       = {Universität Köln},
      type         = {Dr.},
      address      = {Jülich},
      publisher    = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
      reportid     = {FZJ-2014-01343},
      isbn         = {987-3-89336-967-6},
      series       = {Schriften des Forschungszentrums Jülich Reihe Energie $\&$
                      Umwelt / Energy $\&$ Environment},
      pages        = {148 S.},
      year         = {2014},
      note         = {Universität Köln, Diss., 2014},
      abstract     = {The hydroxyl radical (OH) is the main oxidation agent in
                      the atmosphere during daytime. Recent field campaigns
                      studying the radical chemistry in forested areas showed
                      large discrepancies between measured and modeled OH
                      concentration at low NO$_{x}$ conditions and a VOC dominated
                      OH reactivity k(OH) (Hofzumahaus et al., 2009; Lelieveld et
                      al., 2008). These observations were only partially explained
                      by the evidence for new efficient hydroxyl radical
                      regeneration pathways in the isoprene oxidation mechanism
                      (Fuchs et al., 2013; Whalley et al., 2011). So it is likely
                      that other VOC species are also capable of additional OH
                      recycling. Beside isoprene monoterpenes and
                      2-methyl-3-buten-2-ol (MBO) belong to the volatile organic
                      compound (VOC) species with the highest global emission
                      rates. Due to their high reactivity towards OH, monoterpenes
                      and MBO can dominate the radical chemistry of the atmosphere
                      in forested areas under certain conditions (Kim et al.,
                      2013). In the present study the photochemical degradation
                      mechanism of $\alpha$-pinene, $\beta$-pinene, limonene,
                      myrcene and MBO was investigated in the atmosphere
                      simulation chamber SAPHIR. The focus of this study was in
                      particular on the investigation of the radical budget in the
                      degradation process. The photochemical degradation of the
                      five terpenoids was studied in a dedicated series of
                      experiments in the years 2012 and 2013. The SAPHIR chamber
                      was equipped with instrumentation to measure all important
                      OH precursors (O$_{3}$, HONO, HCHO), the parent VOC and its
                      main oxidation products, radicals (OH, HO$_{2}$, RO$_{2}$),
                      the total OH reactivity, and photolysis frequencies to
                      investigate the radical budget in the chamber. All
                      experiments were carried out under low NOx conditions (≤
                      2ppb) and atmospheric terpenoid concentrations (≤ 5ppb)
                      with and without the addition of ozone. The intercomparison
                      of the measured time series of the atmospheric trace gases
                      with simulations using the atmospheric box model Master
                      Chemical Mechanism (MCM) 3.2 showed that the MBO experiments
                      could be described well by the MCM. In contrast to MBO the
                      measured OH and HO$_{2}$ concentrations in the simulations
                      of the $\alpha$-pinene, $\beta$- pinene and limonene
                      experiments were systematically underestimated. In addition
                      the measured k(OH) was overestimated increasingly by the MCM
                      model after VOC injection in the atmosphere simulation
                      chamber. A sensitivity study showed that this overestimation
                      is related to the product spectrum assumed in the MCM model.
                      Despite adjusting the modelled k(OH) to the measured values
                      the measured OH and HO2 concentrations were still
                      underestimated by the model. Model sensitivity studies on
                      additional OH [...]},
      keywords     = {Dissertation (GND)},
      cin          = {IEK-8},
      cid          = {I:(DE-Juel1)IEK-8-20101013},
      pnm          = {233 - Trace gas and aerosol processes in the troposphere
                      (POF2-233)},
      pid          = {G:(DE-HGF)POF2-233},
      typ          = {PUB:(DE-HGF)11},
      url          = {https://juser.fz-juelich.de/record/151374},
}