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@ARTICLE{Bonn:202039,
author = {Bonn, B. and Bourtsoukidis, E. and Sun, T. S. and Bingemer,
H. and Rondo, L. and Javed, U. and Li, J. and Axinte, R. and
Li, Xin and Brauers, T. and Sonderfeld, H. and Koppmann, R.
and Sogachev, A. and Jacobi, S. and Spracklen, D. V.},
title = {{T}he link between atmospheric radicals and newly formed
particles at a spruce forest site in {G}ermany},
journal = {Atmospheric chemistry and physics},
volume = {14},
number = {19},
issn = {1680-7324},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2015-04328},
pages = {10823 - 10843},
year = {2014},
abstract = {It has been claimed for more than a century that
atmospheric new particle formation is primarily influenced
by the presence of sulfuric acid. However, the activation
process of sulfuric acid related clusters into detectable
particles is still an unresolved topic. In this study we
focus on the PARADE campaign measurements conducted during
August/September 2011 at Mt Kleiner Feldberg in central
Germany. During this campaign a set of radicals, organic and
inorganic compounds and oxidants and aerosol properties were
measured or calculated. We compared a range of organic and
inorganic nucleation theories, evaluating their ability to
simulate measured particle formation rates at 3 nm in
diameter (J3) for a variety of different conditions.
Nucleation mechanisms involving only sulfuric acid
tentatively captured the observed noon-time daily maximum in
J3, but displayed an increasing difference to J3
measurements during the rest of the diurnal cycle. Including
large organic radicals, i.e. organic peroxy radicals (RO2)
deriving from monoterpenes and their oxidation products, in
the nucleation mechanism improved the correlation between
observed and simulated J3. This supports a recently proposed
empirical relationship for new particle formation that has
been used in global models. However, the best match between
theory and measurements for the site of interest was found
for an activation process based on large organic peroxy
radicals and stabilised Criegee intermediates (sCI). This
novel laboratory-derived algorithm simulated the daily
pattern and intensity of J3 observed in the ambient data. In
this algorithm organic derived radicals are involved in
activation and growth and link the formation rate of
smallest aerosol particles with OH during daytime and NO3
during night-time. Because the RO2 lifetime is controlled by
HO2 and NO we conclude that peroxy radicals and NO seem to
play an important role for ambient radical chemistry not
only with respect to oxidation capacity but also for the
activation process of new particle formation. This is
supposed to have significant impact of atmospheric radical
species on aerosol chemistry and should be taken into
account when studying the impact of new particles in climate
feedback cycles.},
cin = {IEK-8},
ddc = {550},
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)16},
UT = {WOS:000344164800027},
doi = {10.5194/acp-14-10823-2014},
url = {https://juser.fz-juelich.de/record/202039},
}