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@ARTICLE{Thomas:892382,
author = {Thomas, Max and Laube, Johannes C. and Kaiser, Jan and
Allin, Samuel and Martinerie, Patricia and Mulvaney, Robert
and Ridley, Anna and Röckmann, Thomas and Sturges, William
T. and Witrant, Emmanuel},
title = {{S}tratospheric carbon isotope fractionation and
tropospheric histories of {CFC}-11, {CFC}-12 and {CFC}-113
isotopologues},
journal = {Atmospheric chemistry and physics / Discussions},
volume = {2020},
issn = {1680-7367},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2021-02043},
pages = {843},
year = {2020},
abstract = {We present novel measurements of the carbon isotope
composition of CFC-11 (CCl3F), CFC-12 (CCl2F2), and CFC-113
(CF2ClCFCl2), three atmospheric trace gases that are
important for both stratospheric ozone depletion and global
warming. These measurements were carried out on air samples
collected in the stratosphere – the main sink region for
these gases – and on air extracted from deep polar firn
snow. We quantify, for the first time, the apparent isotopic
fractionation, εapp(13C), for these gases as they are
destroyed in the high- and mid-latitude stratosphere:
εapp(CFC-12, high-lat) = (−20.2 ± 4.4) ‰ and
εapp(CFC-113, high-lat) = (−9.4 ± 4.4) ‰,
εapp(CFC-12, mid-lat) = (−30.3 ± 10.7) ‰, and
εapp(CFC-113, mid-lat) = (−34.4 ± 9.8) ‰. Our CFC-11
measurements were not sufficient to calculate εapp(CFC-11)
so we instead used previously reported photolytic
fractionation for CFC-11 and CFC-12 to scale our
εapp(CFC-12), resulting in εapp(CFC-11, high-lat) =
(−7.8 ± 1.7) ‰ and εapp(CFC-11, mid-lat) = (−11.7 ±
4.2) ‰. Measurements of firn air were used to construct
histories of the tropospheric isotopic composition,
δT(13C), for CFC-11 (1950s to 2009), CFC-12 (1950s to
2009), and CFC-113 (1970s to 2009) – with δT(13C)
increasing for each gas. We used εapp(high-lat), which were
derived from more data, and a constant isotopic composition
of emissions, δE(13C), to model δT(13C, CFC-11), δT(13C,
CFC-12), and δT(13C, CFC-113). For CFC-11 and CFC-12,
modelled δT(13C) was consistent with measured δT(13C) for
the entire period covered by the measurements, suggesting no
dramatic change in δE(13C, CFC-11) or δE(13C, CFC-12) has
occurred since the 1950s. For CFC-113, our modelled δT(13C,
CFC-113) did not agree with our measurements earlier than
1980. While this discrepancy may be indicative of a change
in δE(13C, CFC-113), it is premature to assign one. Our
modelling predicts increasing δT(13C, CFC-11), δT(13C,
CFC-12), and δT(13C, CFC-113) into the future. We
investigated the effect of recently reported new CFC-11
emissions on background δT(13C, CFC-11) by fixing model
emissions after 2012, and comparing δT(13C, CFC-11) in this
scenario to the model base case. The difference in δT(13C,
CFC-11) between these scenarios was 1.4 ‰ in 2050. This
difference is smaller than our model uncertainty envelope
and would therefore require improved modelling and
measurement precision, as well as better quantified isotopic
source compositions, to detect.},
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) / EXC3ITE - EXploring
Chemistry, Composition and Circulation in the stratosphere
with InnovativeTEchnologies (678904)},
pid = {G:(DE-HGF)POF3-244 / G:(EU-Grant)678904},
typ = {PUB:(DE-HGF)16},
doi = {https://doi.org/10.5194/acp-2020-843},
url = {https://juser.fz-juelich.de/record/892382},
}