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@ARTICLE{Robrecht:862870,
author = {Robrecht, Sabine and Vogel, Bärbel and Grooss, Jens-Uwe
and Rosenlof, K. and Thornberry, T. and Rollins, A. and
Krämer, Martina and Christensen, L. and Müller, Rolf},
title = {{M}echanism of ozone loss under enhanced water vapour
conditions in the mid-latitude lower stratosphere in summer},
journal = {Atmospheric chemistry and physics},
volume = {19},
issn = {1680-7316},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2019-03057},
pages = {5805-5833},
year = {2019},
abstract = {Water vapour convectively injected into the mid-latitude
lowermost stratosphere could affect stratospheric ozone. The
associated potential ozone loss process requires low
temperatures together with elevated water vapour mixing
ratios. Since this ozone loss is initiated by heterogeneous
chlorine activation on liquid aerosols, an increase in
sulfate aerosol surface area due to a volcanic eruption or
geoengineering could increase the likelihood of its
occurrence. However, the chemical mechanism of this ozone
loss process has not yet been analysed in sufficient detail
and its sensitivity to various conditions is not yet clear.
Under conditions of climate change associated with an
increase in greenhouse gases, both a stratospheric cooling
and an increase in water vapour convectively injected into
the stratosphere are expected. Understanding the influence
of low temperatures, elevated water vapour and enhanced
sulfate particles on this ozone loss mechanism is a key step
in estimating the impact of climate change and potential
sulfate geoengineering on mid-latitude ozone.Here, we
analyse the ozone loss mechanism and its sensitivity to
various stratospheric conditions in detail. By conducting a
box-model study with the Chemical Lagrangian Model of the
Stratosphere (CLaMS), chemistry was simulated along a 7 d
backward trajectory. This trajectory was calculated
neglecting mixing of neighbouring air masses. Chemical
simulations were initialized using measurements taken during
the Studies of Emissions and Atmospheric Composition, Clouds
and Climate Coupling by Regional Surveys (SEAC4RS) aircraft
campaign (2013, Texas), which encountered an elevated water
vapour mixing ratio of 10.6 ppmv at a pressure level
around 100 hPa. We present a detailed analysis of the
ozone loss mechanism, including the chlorine activation,
chlorine-catalysed ozone loss cycles, maintenance of
activated chlorine and the role of active nitrogen oxide
radicals (NOx). Focussing on a realistic trajectory in a
temperature range from 197 to 202 K, a threshold in water
vapour of 10.6 ppmv has to be exceeded and maintained for
stratospheric ozone loss to occur. We investigated the
sensitivity of the water vapour threshold to temperature,
sulfate content, inorganic chlorine (Cly), inorganic
nitrogen (NOy) and inorganic bromine (Bry). The water vapour
threshold is mainly determined by the temperature and
sulfate content. However, the amount of ozone loss depends
on Cly, Bry and the duration of the time period over which
chlorine activation can be maintained. NOy affects both the
potential of ozone formation and the balance between
reactions yielding chlorine activation and deactivation,
which determines the water vapour threshold. Our results
show that in order to deplete ozone, a chlorine activation
time of 24 to 36 h for conditions of the water vapour
threshold with low temperatures must be maintained. A
maximum ozone loss of $9 \%$ was found for a 20 ppmv
water vapour mixing ratio using North American Monsoon (NAM)
tropopause standard conditions with a chemical box-model
simulation along a realistic trajectory. For the same
trajectory, using observed conditions (of 10.6 ppmv H2O),
the occurrence of simulated ozone loss was dependent on the
sulfate amount assumed. Detailed analysis of current and
future possibilities is needed to assess whether enhanced
water vapour conditions in the summertime mid-latitude lower
stratosphere lead to significant ozone loss},
cin = {IEK-7},
ddc = {550},
cid = {I:(DE-Juel1)IEK-7-20101013},
pnm = {244 - Composition and dynamics of the upper troposphere and
middle atmosphere (POF3-244)},
pid = {G:(DE-HGF)POF3-244},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000466855400003},
doi = {10.5194/acp-19-5805-2019},
url = {https://juser.fz-juelich.de/record/862870},
}