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@ARTICLE{Groo:849790,
author = {Grooß, Jens-Uwe and Müller, Rolf and Spang, Reinhold and
Tritscher, Ines and Wegner, Tobias and Chipperfield, Martyn
P. and Feng, Wuhu and Kinnison, Douglas E. and Madronich,
Sasha},
title = {{O}n the discrepancy of {HC}l processing in the core of the
wintertime polar vortices},
journal = {Atmospheric chemistry and physics},
volume = {18},
number = {12},
issn = {1680-7324},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2018-03902},
pages = {8647 - 8666},
year = {2018},
abstract = {More than 3 decades after the discovery of the ozone hole,
the processes involved in its formation are believed to be
understood in great detail. Current state-of-the-art models
can reproduce the observed chemical composition in the
springtime polar stratosphere, especially regarding the
quantification of halogen-catalysed ozone loss. However, we
report here on a discrepancy between simulations and
observations during the less-well-studied period of the
onset of chlorine activation. During this period, which in
the Antarctic is between May and July, model simulations
significantly overestimate HCl, one of the key chemical
species, inside the polar vortex during polar night. This
HCl discrepancy is also observed in the Arctic. The
discrepancy exists in different models to varying extents;
here, we discuss three independent ones, the Chemical
Lagrangian Model of the Stratosphere (CLaMS) as well as the
Eulerian models SD-WACCM (the specified dynamics version of
the Whole Atmosphere Community Climate Model) and
TOMCAT/SLIMCAT. The HCl discrepancy points to some unknown
process in the formulation of stratospheric chemistry that
is currently not represented in the models.We characterise
the HCl discrepancy in space and time for the Lagrangian
chemistry–transport model CLaMS, in which HCl in the polar
vortex core stays about constant from June to August in the
Antarctic, while the observations indicate a continuous HCl
decrease over this period. The somewhat smaller
discrepancies in the Eulerian models SD-WACCM and
TOMCAT/SLIMCAT are also presented. Numerical diffusion in
the transport scheme of the Eulerian models is identified to
be a likely cause for the inter-model differences. Although
the missing process has not yet been identified, we
investigate different hypotheses on the basis of the
characteristics of the discrepancy. An underestimated HCl
uptake into the polar stratospheric cloud (PSC) particles
that consist mainly of H2O and HNO3 cannot explain it due to
the temperature correlation of the discrepancy. Also, a
direct photolysis of particulate HNO3 does not resolve the
discrepancy since it would also cause changes in chlorine
chemistry in late winter which are not observed. The
ionisation caused by galactic cosmic rays provides an
additional NOx and HOx source that can explain only about
$20\%$ of the discrepancy. However, the model simulations
show that a hypothetical decomposition of particulate HNO3
by some other process not dependent on the solar elevation,
e.g. involving galactic cosmic rays, may be a possible
mechanism to resolve the HCl discrepancy. Since the
discrepancy reported here occurs during the beginning of the
chlorine activation period, where the ozone loss rates are
small, there is only a minor impact of about $2\%$ on the
overall ozone column loss over the course of Antarctic
winter and spring.},
cin = {IEK-7 / JARA-HPC},
ddc = {550},
cid = {I:(DE-Juel1)IEK-7-20101013 / $I:(DE-82)080012_20140620$},
pnm = {244 - Composition and dynamics of the upper troposphere and
middle atmosphere (POF3-244) / Chemisches Lagrangesches
Modell der Stratosphäre (CLaMS) $(jicg11_20090701)$},
pid = {G:(DE-HGF)POF3-244 / $G:(DE-Juel1)jicg11_20090701$},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000435651200002},
doi = {10.5194/acp-18-8647-2018},
url = {https://juser.fz-juelich.de/record/849790},
}