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@ARTICLE{Zhao:187521,
      author       = {Zhao, Defeng and Kaminski, Martin and Schlag, P. and Fuchs,
                      H. and Acir, I.-H. and Bohn, B. and Häseler, R. and
                      Kiendler-Scharr, A. and Rohrer, F. and Tillmann, R. and
                      Wang, Mingjin and Wegener, R. and Wildt, J. and Wahner, A.
                      and Mentel, Th. F.},
      title        = {{S}econdary organic aerosol formation from hydroxyl radical
                      oxidation and ozonolysis of monoterpenes},
      journal      = {Atmospheric chemistry and physics},
      volume       = {15},
      number       = {2},
      issn         = {1680-7324},
      address      = {Katlenburg-Lindau},
      publisher    = {EGU},
      reportid     = {FZJ-2015-01150},
      pages        = {991 - 1012},
      year         = {2015},
      abstract     = {Oxidation by hydroxyl radical (OH) and ozonolysis are the
                      two major pathways of daytime biogenic volatile organic
                      compound (BVOC) oxidation and secondary organic aerosol
                      (SOA) formation. In this study, we investigated the particle
                      formation of several common monoterpenes (α-pinene,
                      β-pinene and limonene) by OH-dominated oxidation, which has
                      seldom been investigated. OH oxidation experiments were
                      carried out in the SAPHIR (Simulation of Atmospheric
                      PHotochemistry In a large Reaction) chamber in Jülich,
                      Germany, at low NOx (0.01 ~ 1 ppbV) and low ozone (O3)
                      concentration (< 20 ppbV). OH concentration and total OH
                      reactivity (kOH) were measured directly, and through this
                      the overall reaction rate of total organics with OH in each
                      reaction system was quantified. Multi-generation reaction
                      process, particle growth, new particle formation (NPF),
                      particle yield and chemical composition were analyzed and
                      compared with that of monoterpene ozonolysis.
                      Multi-generation products were found to be important in
                      OH-dominated SOA formation. The relative role of
                      functionalization and fragmentation in the reaction process
                      of OH oxidation was analyzed by examining the particle mass
                      and the particle size as a function of OH dose. We developed
                      a novel method which quantitatively links particle growth to
                      the reaction rate of OH with total organics in a reaction
                      system. This method was also used to analyze the evolution
                      of functionalization and fragmentation of organics in the
                      particle formation by OH oxidation. It shows that
                      functionalization of organics was dominant in the beginning
                      of the reaction (within two lifetimes of the monoterpene)
                      and fragmentation started to play an important role after
                      that. We compared particle formation from OH oxidation with
                      that from pure ozonolysis. In individual experiments, growth
                      rates of the particle size did not necessarily correlate
                      with the reaction rate of monoterpene with OH and O3.
                      Comparing the size growth rates at the similar reaction
                      rates of monoterpene with OH or O3 indicates that,
                      generally, OH oxidation and ozonolysis had similar
                      efficiency in particle growth. The SOA yield of α-pinene
                      and limonene by ozonolysis was higher than that of OH
                      oxidation. Aerosol mass spectrometry (AMS) shows SOA
                      elemental composition from OH oxidation follows a slope
                      shallower than −1 in the O / C vs. H / C diagram, also
                      known as Van Krevelen diagram, indicating that oxidation
                      proceeds without significant loss of hydrogen. SOA from OH
                      oxidation had higher H / C ratios than SOA from ozonolysis.
                      In ozonolysis, a process with significant hydrogen loss
                      seemed to play an important role in SOA formation.},
      cin          = {IEK-8 / IBG-2},
      ddc          = {550},
      cid          = {I:(DE-Juel1)IEK-8-20101013 / I:(DE-Juel1)IBG-2-20101118},
      pnm          = {243 - Tropospheric trace substances and their
                      transformation processes (POF3-243) / HITEC - Helmholtz
                      Interdisciplinary Doctoral Training in Energy and Climate
                      Research (HITEC) (HITEC-20170406)},
      pid          = {G:(DE-HGF)POF3-243 / G:(DE-Juel1)HITEC-20170406},
      typ          = {PUB:(DE-HGF)16},
      UT           = {WOS:000351170000016},
      doi          = {10.5194/acp-15-991-2015},
      url          = {https://juser.fz-juelich.de/record/187521},
}