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@ARTICLE{Pullinen:885396,
author = {Pullinen, Iida and Schmitt, Sebastian and Kang, Sungah and
Sarrafzadeh, Mehrnaz and Schlag, Patrick and Andres,
Stefanie and Kleist, Einhard and Mentel, Thomas F. and
Rohrer, Franz and Springer, Monika and Tillmann, Ralf and
Wildt, Jürgen and Wu, Cheng and Zhao, Defeng and Wahner,
Andreas and Kiendler-Scharr, Astrid},
title = {{I}mpact of {NO}x on secondary organic aerosol ({SOA})
formation from α-pinene and β-pinene photooxidation: the
role of highly oxygenated organic nitrates},
journal = {Atmospheric chemistry and physics},
volume = {20},
number = {17},
issn = {1680-7324},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2020-03793},
pages = {10125 - 10147},
year = {2020},
abstract = {The formation of organic nitrates (ONs) in the gas phase
and their impact on mass formation of secondary organic
aerosol (SOA) was investigated in a laboratory study for
α-pinene and β-pinene photooxidation. Focus was the
elucidation of those mechanisms that cause the often
observed suppression of SOA mass formation by NOx, and
therein the role of highly oxygenated multifunctional
molecules (HOMs). We observed that with increasing NOx
concentration (a) the portion of HOM organic nitrates
(HOM-ONs) increased, (b) the fraction of accretion products
(HOM-ACCs) decreased, and (c) HOM-ACCs contained on average
smaller carbon numbers.Specifically, we investigated HOM
organic nitrates (HOM-ONs), arising from the termination
reactions of HOM peroxy radicals with NOx, and HOM
permutation products (HOM-PPs), such as ketones, alcohols,
or hydroperoxides, formed by other termination reactions.
Effective uptake coefficients γeff of HOMs on particles
were determined. HOMs with more than six O atoms efficiently
condensed on particles (γeff>0.5 on average), and for HOMs
containing more than eight O atoms, every collision led to
loss. There was no systematic difference in γeff for
HOM-ONs and HOM-PPs arising from the same HOM peroxy
radicals. This similarity is attributed to the
multifunctional character of the HOMs: as functional groups
in HOMs arising from the same precursor HOM peroxy radical
are identical, vapor pressures should not strongly depend on
the character of the final termination group. As a
consequence, the suppressing effect of NOx on SOA formation
cannot be simply explained by replacement of terminal
functional groups by organic nitrate groups.According to
their γeff all HOM-ONs with more than six O atoms will
contribute to organic bound nitrate (OrgNO3) in the
particulate phase. However, the fraction of OrgNO3 stored in
condensable HOMs with molecular masses > 230 Da
appeared to be substantially higher than the fraction of
particulate OrgNO3 observed by aerosol mass spectrometry.
This result suggests losses of OrgNO3 for organic nitrates
in particles, probably due to hydrolysis of OrgNO3 that
releases HNO3 into the gas phase but leaves behind the
organic rest in the particulate phase. However, the loss of
HNO3 alone could not explain the observed suppressing effect
of NOx on particle mass formation from α-pinene and
β-pinene.Instead we can attribute most of the reduction in
SOA mass yields with increasing NOx to the significant
suppression of gas phase HOM-ACCs, which have high molecular
mass and are potentially important for SOA mass formation at
low-NOx conditions.},
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:000567769500001},
doi = {10.5194/acp-20-10125-2020},
url = {https://juser.fz-juelich.de/record/885396},
}