Preprints
https://doi.org/10.5194/acp-2021-950
https://doi.org/10.5194/acp-2021-950
 
02 Dec 2021
02 Dec 2021
Status: a revised version of this preprint is currently under review for the journal ACP.

How do Cl concentrations matter for simulating CH4, δ13C(CH4) and estimating CH4 budget through atmospheric inversions?

Joël Thanwerdas1, Marielle Saunois1, Isabelle Pison1, Didier Hauglustaine1, Antoine Berchet1, Bianca Baier2,3, Colm Sweeney3, and Philippe Bousquet1 Joël Thanwerdas et al.
  • 1Laboratoire des Sciences du Climat et de l’Environnement, LSCE-IPSL (CEA-CNRS-UVSQ), Université Paris-Saclay 91191 Gif-sur-Yvette, France
  • 2Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado-Boulder, Boulder, CO, USA 80305
  • 3NOAA Earth System Research Laboratory Global Monitoring Division, Boulder, CO, USA 80305

Abstract. Atmospheric methane (CH4) concentrations have been rising since 2007, resulting from an imbalance between CH4 sources and sinks. The CH4 budget is generally estimated through top-down approaches using CH4 observations as constraints. The atmospheric isotopic CH4 signal, δ13C(CH4), can also provide additional constraints and helps to discriminate between emission categories. The oxidation by chlorine (Cl) likely contributes less than 5 % to the total oxidation of atmospheric CH4. However, the Cl sink is highly fractionating, and thus strongly influences δ13C(CH4). As inversion studies do not prescribe the same Cl fields to constrain CH4 budget, it can lead to discrepancies between estimates. To quantify the influence of the Cl concentrations on CH4, δ13C(CH4) and CH4 budget estimates, we perform multiple sensitivity simulations using three Cl fields with concentrations that are realistic with regard to recent literature and one Cl field with concentrations that are very likely to be overestimated. We also test removing the tropospheric and the entire Cl sink in other sensitivity simulations. We find that the realistic Cl fields tested here are responsible for between 0.3 % and 1.8 % of the total chemical CH4 sink in the troposphere and between 1.0 % and 1.2 % in the stratosphere. Prescribing these different Cl amounts in surface-based inversions can lead to differences in global CH4 source adjustments of up to 12.3 TgCH4.yr−1. We also find that the globally-averaged isotopic signature of the CH4 sources inferred by a surface-based inversion assimilating δ13C(CH4) observations would decrease by 0.53 ‰ for each additional percent of contribution from the tropospheric Cl sink to the total sink. Finally, our study shows that CH4 seasonal cycle amplitude is modified by less than 1–2 % but δ13(CH4) seasonal cycle amplitude can be modified by up to 10–20 %, depending on the latitude.

Joël Thanwerdas et al.

Status: final response (author comments only)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-950', Anonymous Referee #1, 22 Dec 2021
  • RC2: 'Comment on acp-2021-950', Anonymous Referee #2, 02 Jan 2022
    • RC3: 'Corrections to RC2', Anonymous Referee #2, 02 Jan 2022
  • RC4: 'Comment on acp-2021-950', Anonymous Referee #3, 03 Jan 2022
  • AC1: 'Author final response', Joel Thanwerdas, 06 Jun 2022

Joël Thanwerdas et al.

Joël Thanwerdas et al.

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Short summary
Atmospheric methane (CH4) concentrations have been rising since 2007, resulting from an imbalance between CH4 sources and sinks. The CH4 budget is generally estimated through top-down approaches using CH4 and δ13C(CH4) observations as constraints. The oxidation by chlorine (Cl) contributes little to the total oxidation of CH4 but strongly influences δ13C(CH4). Here, we compare multiple recent Cl fields and quantify the influence of Cl concentrations on CH4, δ13C(CH4) and CH4 budget estimates.
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