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Stratospheric carbon isotope fractionation and tropospheric histories of CFC-11, CFC-12, and CFC-113 isotopologues

Authors: Thomas, Max; Laube, Johannes C.; Kaiser, Jan; Allin, Samuel; Martinerie, Patricia; Mulvaney, Robert; Ridley, Anna; +5 Authors

Stratospheric carbon isotope fractionation and tropospheric histories of CFC-11, CFC-12, and CFC-113 isotopologues

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-latitude) =(-20.2±4.4) ‰, and ϵapp(CFC-113, high-latitude) =(-9.4±4.4) ‰, ϵapp(CFC-12, mid-latitude) =(-30.3±10.7) ‰, and ϵapp(CFC-113, mid-latitude) =(-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-latitude) =(-7.8±1.7) ‰ and ϵapp(CFC-11, mid-latitude) =(-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-latitude), which was 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 that 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. This discrepancy may be indicative of a change in δE(13C, CFC-113). However, this conclusion is based largely on a single sample and only just significant outside the 95 % confidence interval. Therefore more work is needed to independently verify this temporal trend in the global tropospheric 13C isotopic composition of CFC-113. 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.

Country
Netherlands
Keywords

Atmospheric Science, Chemistry, Physics, QC1-999, QD1-999

50 references, page 1 of 5

Supplement. The supplement related to this article is available online at: https://doi.org/10.5194/acp-21-6857-2021-supplement.

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    Average
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citations
This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Citations provided by BIP!
popularity
This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
BIP!Popularity provided by BIP!
influence
This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Influence provided by BIP!
impulse
This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.
BIP!Impulse provided by BIP!
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EC| EUROCHAMP-2020
Project
EUROCHAMP-2020
Integration of European Simulation Chambers for Investigating Atmospheric Processes – Towards 2020 and beyond
  • Funder: European Commission (EC)
  • Project Code: 730997
  • Funding stream: H2020 | RIA
,
EC| EXC3ITE
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EXC3ITE
EXploring Chemistry, Composition and Circulation in the stratosphere with Innovative TEchnologies
  • Funder: European Commission (EC)
  • Project Code: 678904
  • Funding stream: H2020 | ERC | ERC-STG
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