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@ARTICLE{Gkatzelis:856151,
author = {Gkatzelis, Georgios and Hohaus, Thorsten and Tillmann, Ralf
and Gensch, Iulia and Müller, Markus and Eichler, Philipp
and Xu, Kang-Ming and Schlag, Patrick and Schmitt, Sebastian
H. and Yu, Zhujun and Wegener, Robert and Kaminski, Martin
and Holzinger, Rupert and Wisthaler, Armin and
Kiendler-Scharr, Astrid},
title = {{G}as-to-particle partitioning of major biogenic oxidation
products: a study on freshly formed and aged biogenic {SOA}},
journal = {Atmospheric chemistry and physics},
volume = {18},
number = {17},
issn = {1680-7324},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2018-05787},
pages = {12969 - 12989},
year = {2018},
abstract = {Secondary organic aerosols (SOAs) play a key role in
climate change and air quality. Determining the fundamental
parameters that distribute organic compounds between the
phases is essential, as atmospheric lifetime and impacts
change drastically between the gas and particle phase. In
this work, gas-to-particle partitioning of major biogenic
oxidation products was investigated using three different
aerosol chemical characterization techniques. The aerosol
collection module, the collection thermal desorption unit,
and the chemical analysis of aerosols online are different
aerosol sampling inlets connected to a proton-transfer
reaction time-of-flight mass spectrometer (ACM-PTR-ToF-MS,
TD-PTR-ToF-MS, and CHARON-PTR-ToF-MS, respectively, referred
to hereafter as ACM, TD, and CHARON). These techniques were
deployed at the atmosphere simulation chamber SAPHIR to
perform experiments on the SOA formation and aging from
different monoterpenes (β-pinene, limonene) and real plant
emissions (Pinus sylvestris L.). The saturation mass
concentration C* and thus the volatility of the individual
ions was determined based on the simultaneous measurement of
their signal in the gas and particle phase.A method to
identify and exclude ions affected by thermal dissociation
during desorption and ionic dissociation in the ionization
chamber of the proton-transfer reaction mass spectrometer
(PTR-MS) was developed and tested for each technique. Narrow
volatility distributions with organic compounds in the
semi-volatile (SVOCs – semi-volatile organic compounds) to
intermediate-volatility (IVOCs – intermediate-volatility
organic compounds) regime were found for all systems
studied. Despite significant differences in the aerosol
collection and desorption methods of the
proton-transfer-reaction (PTR)-based techniques, a
comparison of the C* values obtained with different
techniques was found to be in good agreement (within 1 order
of magnitude) with deviations explained by the different
operating conditions of the PTR-MS.The C* of the identified
organic compounds were mapped onto the two-dimensional
volatility basis set (2D-VBS), and results showed a decrease
in C* with increasing oxidation state. For all experiments
conducted in this study, identified partitioning organic
compounds accounted for $20–30\%$ of the total organic
mass measured from an aerosol mass spectrometer (AMS).
Further comparison between observations and theoretical
calculations was performed for species found in our
experiments that were also identified in previous
publications. Theoretical calculations based on the
molecular structure of the compounds showed, within the
uncertainties ranges, good agreement with the experimental
C* for most SVOCs, while IVOCs deviated by up to a factor of
300. These latter differences are discussed in relation to
two main processes affecting these systems: (i) possible
interferences by thermal and ionic fragmentation of higher
molecular-weight compounds, produced by accretion and
oligomerization reactions, that fragment in the m∕z range
detected by the PTR-MS and (ii) kinetic influences in the
distribution between the gas and particle phase with
gas-phase condensation, diffusion in the particle phase, and
irreversible uptake.},
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:000444187300002},
doi = {10.5194/acp-18-12969-2018},
url = {https://juser.fz-juelich.de/record/856151},
}