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@ARTICLE{Jesswein:911910,
author = {Jesswein, Markus and Fernandez, Rafael P. and Berná, Lucas
and Saiz-Lopez, Alfonso and Grooß, Jens-Uwe and Hossaini,
Ryan and Apel, Eric C. and Hornbrook, Rebecca S. and Atlas,
Elliot L. and Blake, Donald R. and Montzka, Stephen and
Keber, Timo and Schuck, Tanja and Wagenhäuser, Thomas and
Engel, Andreas},
title = {{G}lobal seasonal distribution of {CH}2{B}r2 and {CHB}r3 in
the upper troposphere and lower stratosphere},
journal = {Atmospheric chemistry and physics},
volume = {22},
number = {22},
issn = {1680-7316},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2022-05157},
pages = {15049 - 15070},
year = {2022},
abstract = {Bromine released from the decomposition of short-lived
brominated source gases contributes as a sink of ozone in
the lower stratosphere. The two major contributors are
CH2Br2 and CHBr3. In this study, we investigate the global
seasonal distribution of these two substances, based on four
High Altitude and Long Range Research Aircraft (HALO)
missions, the HIAPER Pole-to-Pole Observations (HIPPO)
mission, and the Atmospheric Tomography (ATom) mission.
Observations of CH2Br2 in the free and upper troposphere
indicate a pronounced seasonality in both hemispheres, with
slightly larger mixing ratios in the Northern Hemisphere
(NH). Compared to CH2Br2, CHBr3 in these regions shows
larger variability and less clear seasonality, presenting
larger mixing ratios in winter and autumn in NH midlatitudes
to high latitudes. The lowermost stratosphere of SH and NH
shows a very similar distribution of CH2Br2 in hemispheric
spring with differences well below 0.1 ppt, while the
differences in hemispheric autumn are much larger with
substantially smaller values in the SH than in the NH. This
suggests that transport processes may be different in both
hemispheric autumn seasons, which implies that the influx of
tropospheric air (“flushing”) into the NH lowermost
stratosphere is more efficient than in the SH. The
observations of CHBr3 support the suggestion, with a steeper
vertical gradient in the upper troposphere and lower
stratosphere in SH autumn than in NH autumn. However, the SH
database is insufficient to quantify this difference. We
further compare the observations to model estimates of
TOMCAT (Toulouse Off-line Model of Chemistry And Transport)
and CAM-Chem (Community Atmosphere Model with Chemistry,
version 4), both using the same emission inventory of
Ordóñez et al. (2012). The pronounced tropospheric
seasonality of CH2Br2 in the SH is not reproduced by the
models, presumably due to erroneous seasonal emissions or
atmospheric photochemical decomposition efficiencies. In
contrast, model simulations of CHBr3 show a pronounced
seasonality in both hemispheres, which is not confirmed by
observations. The distributions of both species in the
lowermost stratosphere of the Northern and Southern
hemispheres are overall well captured by the models with the
exception of southern hemispheric autumn, where both models
present a bias that maximizes in the lowest 40 K above the
tropopause, with considerably lower mixing ratios in the
observations. Thus, both models reproduce equivalent
flushing in both hemispheres, which is not confirmed by the
limited available observations. Our study emphasizes the
need for more extensive observations in the SH to fully
understand the impact of CH2Br2 and CHBr3 on
lowermost-stratospheric ozone loss and to help constrain
emissions.},
cin = {IEK-7},
ddc = {550},
cid = {I:(DE-Juel1)IEK-7-20101013},
pnm = {2112 - Climate Feedbacks (POF4-211)},
pid = {G:(DE-HGF)POF4-2112},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000890899200001},
doi = {10.5194/acp-22-15049-2022},
url = {https://juser.fz-juelich.de/record/911910},
}