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@PHDTHESIS{Gkatzelis:845400,
author = {Gkatzelis, Georgios},
title = {{G}as-to-{P}article {P}artitioning of {M}ajor {O}xidation
{P}roducts from {M}onoterpenes and {R}eal {P}lant
{E}missions},
volume = {417},
school = {Universität Köln},
type = {Dissertation},
address = {Jülich},
publisher = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
reportid = {FZJ-2018-02671},
isbn = {978-3-95806-314-3},
series = {Schriften des Forschungszentrums Jülich Reihe Energie $\&$
Umwelt / Energy $\&$ Environment},
pages = {xii, 128 S.},
year = {2018},
note = {Universität Köln, Diss., 2017},
abstract = {Secondary organic aerosol (SOA), formed through the
oxidation of volatile organic compounds (VOCs) in the
atmosphere, play a key role in climate change and air
quality. Due to thousands of individual compounds involved
in SOA formation, the chemical characterization of organic
aerosols (OA) remains a huge analytical challenge. Defining
the fundamental parameters that distribute these organic
molecules between the gas and particle phases is essential,
as atmospheric lifetime and their impacts change drastically
depending on their phase state. In this work, an instrument
called aerosol collection module (ACM) was redeveloped and
automated to allow a better characterization of SOA
originating from the oxidation of biogenic precursors. An
inter-comparison of the ACM to different aerosol chemical
characterization techniques was performed with a focus on
the partitioning of major biogenic oxidation products
between the gas- and particle-phase. In particular, the ACM,
the collection thermal desorption unit (TD) and the chemical
analysis of aerosol on-line (CHARON) are different aerosol
sampling inlets utilizing a Proton-Transfer-Reaction Timeof-
Flight Mass Spectrometer (PTR-ToF-MS). These techniques were
deployed at the atmosphere simulation chamber SAPHIR to
study SOA formation and aging from different monoterpenes
(β-pinene, limonene) and real plant emissions
($\textit{Pinus sylvestris L.}$). The capabilities of the
PTR-based techniques were compared among each other and to
results from an Aerodyne Aerosol Mass Spectrometer (AMS) and
a Scanning Mobility Particle Sizer (SMPS). Gas-to-particle
partitioning values were determined based on the saturation
mass concentration (C*) of individual ions by performing
simultaneous measurement of their signal in the gas- and
particle-phase. Despite significant differences in the
aerosol collection and desorption methods of the PTR based
techniques, the determined chemical composition was
comparable, i.e. the same major contributing ions were found
by all instruments for the different chemical systems
studied. These ions could be attributed to known products
expected from the oxidation of the examined monoterpenes.
Averaged over all experiments, the total aerosol mass
recovery compared to an SMPS was 80 ± 10\%, 51 ± 5\% and
27 ± 3\% for CHARON, ACM and TD, respectively. Comparison
to the oxygen to carbon ratios (O:C) obtained by AMS showed
that all PTR based techniques observed lower O:C ratios
indicating a loss of molecular oxygen either during aerosol
sampling or detection. Differences in total mass recovery
and O:C between the three instruments was found to result
predominately from differences in the electric field
strength (V cm$^{-1}$) to buffer gas density (molecules
cm$^{-3}$) (E/N) ratio in the drifttube reaction ionization
chambers of the PTR-ToF-MS instruments and from
dissimilarities in the collection/desorption of aerosols. A
method to identify and exclude ions affected by thermal
dissociation during desorption and ionic dissociation in the
ionization chamber of the PTRMS was developed and tested.
Determined species were mapped onto the two dimensional
volatility basis set (2D-VBS) and results showed a decrease
of the C* with increasing oxidation state. For compounds
measured [...]},
cin = {IEK-8},
cid = {I:(DE-Juel1)IEK-8-20101013},
pnm = {899 - ohne Topic (POF3-899)},
pid = {G:(DE-HGF)POF3-899},
typ = {PUB:(DE-HGF)3 / PUB:(DE-HGF)11},
urn = {urn:nbn:de:0001-2018050951},
url = {https://juser.fz-juelich.de/record/845400},
}