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Can the carbon isotopic composition of methane be reconstructed from multi-site firn air measurements?

Authors: J. Sapart, C.; Martinerie, P.; Witrant, Emmanuel; Chappellaz, J.; S. W. van de Wal, R.; Sperlich, P.; van Der Veen, C.; +6 Authors

Can the carbon isotopic composition of methane be reconstructed from multi-site firn air measurements?

Abstract

Abstract. Methane is a strong greenhouse gas and large uncertainties exist concerning the future evolution of its atmospheric abundance. Analyzing methane atmospheric mixing and stable isotope ratios in air trapped in polar ice sheets helps in reconstructing the evolution of its sources and sinks in the past. This is important to improve predictions of atmospheric CH4 mixing ratios in the future under the influence of a changing climate. The aim of this study is to assess whether past atmospheric δ13C(CH4) variations can be reliably reconstructed from firn air measurements. Isotope reconstructions obtained with a state of the art firn model from different individual sites show unexpectedly large discrepancies and are mutually inconsistent. We show that small changes in the diffusivity profiles at individual sites lead to strong differences in the firn fractionation, which can explain a large part of these discrepancies. Using slightly modified diffusivities for some sites, and neglecting samples for which the firn fractionation signals are strongest, a combined multi-site inversion can be performed, which returns an isotope reconstruction that is consistent with firn data. However, the isotope trends are lower than what has been concluded from Southern Hemisphere (SH) archived air samples and high-accumulation ice core data. We conclude that with the current datasets and understanding of firn air transport, a high precision reconstruction of δ13C of CH4 from firn air samples is not possible, because reconstructed atmospheric trends over the last 50 yr of 0.3–1.5 ‰ are of the same magnitude as inherent uncertainties in the method, which are the firn fractionation correction (up to ~2 ‰ at individual sites), the Kr isobaric interference (up to ~0.8 ‰, system dependent), inter-laboratory calibration offsets (~0.2 ‰) and uncertainties in past CH4 levels (~0.5 ‰).

Countries
France, Netherlands, Denmark, Switzerland, France, Belgium, France, Switzerland, United Kingdom, France, France
Keywords

[ SDU.OCEAN ] Sciences of the Universe [physics]/Ocean, Atmosphere, atmospheric chemistry, 550, carbon isotope, 530 Physics, QC1-999, [ SDU.STU.GL ] Sciences of the Universe [physics]/Earth Sciences/Glaciology, isotopic composition, 551, mixing ratio, [SDU.STU.GL] Sciences of the Universe/Earth Sciences/Glaciology, [SDU.OCEAN] Sciences of the Universe/Ocean, Atmosphere, SDG 13 - Climate Action, [SDU.STU.GL]Sciences of the Universe [physics]/Earth Sciences/Glaciology, QD1-999, [SDU.STU.GL] Sciences of the Universe [physics]/Earth Sciences/Glaciology, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, [SDU.OCEAN] Sciences of the Universe [physics]/Ocean, Atmosphere, methane, Physics, 500, Chemistry, greenhouse gas, isotopic ratio, Southern Hemisphere, ice core, Sciences exactes et naturelles

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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!
19
Top 10%
Average
Top 10%
Green
gold