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@ARTICLE{Lauther:906264,
author = {Lauther, Valentin and Vogel, Bärbel and Wintel, Johannes
and Rau, Andrea and Hoor, Peter and Bense, Vera and Müller,
Rolf and Volk, C. Michael},
title = {{I}n situ observations of {CH}2{C}l2 and {CHC}l3 show
efficient transport pathways for very short-lived species
into the lower stratosphere via the {A}sian and the {N}orth
{A}merican summer monsoon},
journal = {Atmospheric chemistry and physics},
volume = {22},
number = {3},
issn = {1680-7316},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2022-01330},
pages = {2049 - 2077},
year = {2022},
abstract = {Efficient transport pathways for ozone-depleting very
short-lived substances (VSLSs) from their source regions
into the stratosphere are a matter of current scientific
debate; however they have yet to be fully identified on an
observational basis. Understanding the increasing impact of
chlorine-containing VSLSs (Cl-VSLSs) on stratospheric ozone
depletion is important in order to validate and improve
model simulations and future predictions. We report on a
transport study using airborne in situ measurements of the
Cl-VSLSs dichloromethane (CH2Cl2) and trichloromethane
(chloroform, CHCl3) to derive a detailed description of two
transport pathways from (sub)tropical source regions into
the extratropical upper troposphere and lower stratosphere
(Ex-UTLS) in the Northern Hemisphere (NH) late summer. The
Cl-VSLS measurements were obtained in the upper troposphere
and lower stratosphere (UTLS) above western Europe and the
midlatitude Atlantic Ocean in the frame of the WISE
(Wave-driven ISentropic Exchange) aircraft campaign in
autumn 2017 and are combined with the results from a
three-dimensional simulation of a Lagrangian transport model
as well as back-trajectory calculations. Compared to
background measurements of similar age we find up to
$150 \%$ enhanced CH2Cl2 and up to $100 \%$ enhanced
CHCl3 mixing ratios in the extratropical lower stratosphere
(Ex-LS). We link the measurements of enhanced CH2Cl2 and
CHCl3 mixing ratios to emissions in the region of southern
and eastern Asia. Transport from this area to the Ex-LS at
potential temperatures in the range of 370–400 K takes
about 6–11 weeks via the Asian summer monsoon anticyclone
(ASMA). Our measurements suggest anthropogenic sources to be
the cause of these strongly elevated Cl-VSLS concentrations
observed at the top of the lowermost stratosphere (LMS). A
faster transport pathway into the Ex-LS is derived from
particularly low CH2Cl2 and CHCl3 mixing ratios in the UTLS.
These low mixing ratios reflect weak emissions and a local
seasonal minimum of both species in the boundary layer of
Central America and the tropical Atlantic. We show that air
masses uplifted by hurricanes, the North American monsoon,
and general convection above Central America into the
tropical tropopause layer to potential temperatures of about
360–370 K are transported isentropically within 5–9
weeks from the boundary layer into the Ex-LS. This transport
pathway linked to the North American monsoon mainly impacts
the middle and lower part of the LMS with particularly low
CH2Cl2 and CHCl3 mixing ratios. In a case study, we
specifically analyze air samples directly linked to the
uplift by the Category 5 Hurricane Maria that occurred
during October 2017 above the Atlantic Ocean. CH2Cl2 and
CHCl3 have similar atmospheric sinks and lifetimes, but the
fraction of biogenic emissions is clearly higher for CHCl3
than for the mainly anthropogenically emitted CH2Cl2;
consequently lower CHCl3 : CH2Cl2 ratios are expected in
air parcels showing a higher impact of anthropogenic
emissions. The observed CHCl3 : CH2Cl2 ratio suggests
clearly stronger anthropogenic emissions in the region of
southern and eastern Asia compared to those in the region of
Central America and the tropical Atlantic. Overall, the
transport of strongly enhanced CH2Cl2 and CHCl3 mixing
ratios from southern and eastern Asia via the ASMA is the
main factor in increasing the chlorine loading from the
analyzed VSLSs in the Ex-LS during the NH late summer. Thus,
further increases in Asian CH2Cl2 and CHCl3 emissions, as
frequently reported in recent years, will further increase
the impact of Cl-VSLSs on stratospheric ozone depletion.},
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:000759289700001},
doi = {10.5194/acp-22-2049-2022},
url = {https://juser.fz-juelich.de/record/906264},
}