Hydroxyl (OH) is the atmosphere's main oxidant removing most pollutants including methane. Its short lifetime prevents large-scale direct observational quantification. Abundances inferred using anthropogenic trace gas measurements and models yield conflicting trend estimates. By contrast, radiocarbon monoxide (14CO), produced naturally by cosmic rays and almost exclusively removed by OH, is a tracer with a well-understood source. Here we show that Southern-Hemisphere 14CO measurements indicate increasing OH. New Zealand 14CO data exhibit an annual-mean decrease of 12 ± 2% since 1997, whereas Antarctic measurements show a December-January decrease of 43 ± 24%. Both imply similar OH increases, corroborating our own and other model results suggesting that OH has been globally increasing during recent decades. Model sensitivity simulations illustrate the roles of methane, nitrogen oxides, stratospheric ozone depletion, and global warming driving these trends. They have substantial implications for the budgets of pollutants removed by OH, and especially imply larger than documented methane emission increases.

The growth rate of the atmospheric abundance of methane (CH4) reached a record high of 15.4 ppb yr-1 between 2020 and 2022, but the mechanisms driving the accelerated CH4 growth have so far been unclear. In this work, we use measurements of the 13C:12C ratio of CH4 (expressed as δ13CCH4) from NOAA's Global Greenhouse Gas Reference Network and a box model to investigate potential drivers for the rapid CH4 growth. These measurements show that the record-high CH4 growth in 2020-2022 was accompanied by a sharp decline in δ13CCH4, indicating that the increase in CH4 abundance was mainly driven by increased emissions from microbial sources such as wetlands, waste, and agriculture. We use our box model to reject increasing fossil fuel emissions or decreasing hydroxyl radical sink as the dominant driver for increasing global methane abundance.

The rapidly expanding and energy-intensive production from the Canadian oil sands, one of the largest oil reserves globally, accounts for almost 12 % of Canada's greenhouse gas emissions according to inventories. Developing approaches for evaluating reported methane (CH4) emission is crucial for developing effective mitigation policies, but only one study has characterized CH4 sources in the Athabasca oil sands region (AOSR). We tested the use of 14C and 13C carbon isotope measurements in ambient CH4 from the AOSR to estimate source contributions from key regional CH4 sources: (1) tailings ponds, (2) surface mines and processing facilities, and (3) wetlands. The isotopic signatures of ambient CH4 indicate that the CH4 enrichments measured at the site were mainly influenced by fossil CH4 emissions from surface mining and processing facilities (56 ± 18 %), followed by fossil CH4 emissions from tailings ponds (34 ± 18 %) and to a lesser extent modern CH4 emissions from wetlands (10 ± <1 %). Our results confirm the importance of tailings ponds in regional CH4 emissions and show that this method can successfully distinguish wetland CH4 emissions. In the future, the isotopic characterization of CH4 sources and measurements from different seasons and wind directions are needed to provide a better source attribution in the AOSR.

To investigate which processes cause the current increase in atmospheric methane in the context of future interactions between climate change, the methane cycle and policy decisions. There is evidence for various contributors to emission increases or reduced removal of atmospheric methane. No single process can explain the methane rise and remain consistent with available data. Reconstructions of recent changes in the methane budget do not converge as to the dominant contributor to the rise. A plausible scenario includes increasing emissions from agriculture and fossil fuels while biomass burning is reduced, with possible contributions from wetlands and a weakened sink. Further studies are needed to identify contributors to the methane rise for targeted emission reductions and adaptation to changes in natural methane sources and sinks. Mitigation plans must address the methane rise and possible consequences from a climate-methane feedback.

The amount of the greenhouse gas methane in Earth's atmosphere is rising rapidly

The El Niño–Southern Oscillation (ENSO) has been suggested as a strong forcing in the methane cycle and as a driver of recent trends in global atmospheric methane mole fractions [CH4]. Such a sensitivity of the global CH4 budget to climate events would have important repercussions for climate change mitigation strategies and the accuracy of projections for future greenhouse forcing. Here, we test the impact of ENSO on atmospheric CH4 in a correlation analysis. We use local and global records of [CH4], as well as stable carbon isotopic records of atmospheric CH4 (δ13CH4), which are particularly sensitive to the combined ENSO effects on CH4 production from wetlands and biomass burning. We use a variety of nominal, smoothed, and detrended time series including growth rate records. We find that at most 36 % of the variability in [CH4] and δ13CH4 is attributable to ENSO, but only for detrended records in the southern tropics. Trend-bearing records from the southern tropics, as well as all studied hemispheric and global records, show a minor impact of ENSO, i.e. < 24 % of variability explained. Additional analyses using hydrogen cyanide (HCN) records show a detectable ENSO influence on biomass burning (up to 51 %–55 %), suggesting that it is wetland CH4 production that responds less to ENSO than previously suggested. Dynamics of the removal by hydroxyl likely counteract the variation in emissions, but the expected isotope signal is not evident. It is possible that other processes obscure the ENSO signal, which itself indicates a minor influence of the latter on global CH4 emissions. Trends like the recent rise in atmospheric [CH4] can therefore not be attributed to ENSO. This leaves anthropogenic methane sources as the likely driver, which must be mitigated to reduce anthropogenic climate change.

1.I didn't see a discussion of significance level for the correlation

Abstract. The El Niño – Southern Oscillation (ENSO) has been suggested as a strong forcing in the methane cycle and as a driver of recent trends in global atmospheric methane levels. Such a sensitivity of the global CH4 budget to climate events would have important repercussions for climate change mitigation strategies and the accuracy of projections for future greenhouse forcing. Here, we test the impact of ENSO on the CH4 cycle in a correlation analysis. We use local and global records of methane mixing ratio [CH4], as well as stable carbon isotopic records of atmospheric CH4 (δ13CH4), which are particularly sensitive to the combined ENSO effects on CH4 production from wetlands and biomass burning. We use a variety of nominal, smoothed and detrended time series including growth rate records. We find that at most 38 % of the variability in [CH4] and δ13CH4 is attributable to ENSO, but only for detrended records in the Southern tropics. Trend-bearing records from the Southern tropics, as well as all studied hemispheric and global records show a minor impact of ENSO, i.e.

We report results from a worldwide interlaboratory comparison of samples among laboratories that measure (or measured) stable carbon and hydrogen isotope ratios of atmospheric CH4 (δ13C-CH4 and δD-CH4). The offsets among the laboratories are larger than the measurement reproducibility of individual laboratories. To disentangle plausible measurement offsets, we evaluated and critically assessed a large number of intercomparison results, some of which have been documented previously in the literature. The results indicate significant offsets of δ13C-CH4 and δD-CH4 measurements among data sets reported from different laboratories; the differences among laboratories at modern atmospheric CH4 level spread over ranges of 0.5 ‰ for δ13C-CH4 and 13 ‰ for δD-CH4. The intercomparison results summarized in this study may be of help in future attempts to harmonize δ13C-CH4 and δD-CH4 data sets from different laboratories in order to jointly incorporate them into modelling studies. However, establishing a merged data set, which includes δ13C-CH4 and δD-CH4 data from multiple laboratories with desirable compatibility, is still challenging due to differences among laboratories in instrument settings, correction methods, traceability to reference materials and long-term data management. Further efforts are needed to identify causes of the interlaboratory measurement offsets and to decrease those to move towards the best use of available δ13C-CH4 and δD-CH4 data sets.

Methane (CH4) is a powerful greenhouse gas and plays a key part in global atmospheric chemistry. Natural geological emissions (fossil methane vented naturally from marine and terrestrial seeps and mud volcanoes) are thought to contribute around 52 teragrams of methane per year to the global methane source, about 10 per cent of the total, but both bottom-up methods (measuring emissions) and top-down approaches (measuring atmospheric mole fractions and isotopes) for constraining these geological emissions have been associated with large uncertainties. Here we use ice core measurements to quantify the absolute amount of radiocarbon-containing methane (14CH4) in the past atmosphere and show that geological methane emissions were no higher than 15.4 teragrams per year (95 per cent confidence), averaged over the abrupt warming event that occurred between the Younger Dryas and Preboreal intervals, approximately 11,600 years ago. Assuming that past geological methane emissions were no lower than today, our results indicate that current estimates of today's natural geological methane emissions (about 52 teragrams per year) are too high and, by extension, that current estimates of anthropogenic fossil methane emissions are too low. Our results also improve on and confirm earlier findings that the rapid increase of about 50 per cent in mole fraction of atmospheric methane at the Younger Dryas-Preboreal event was driven by contemporaneous methane from sources such as wetlands; our findings constrain the contribution from old carbon reservoirs (marine methane hydrates, permafrost and methane trapped under ice) to 19 per cent or less (95 per cent confidence). To the extent that the characteristics of the most recent deglaciation and the Younger Dryas-Preboreal warming are comparable to those of the current anthropogenic warming, our measurements suggest that large future atmospheric releases of methane from old carbon sources are unlikely to occur.

We report results from intercomparison exercises between laboratories that conduct measurements of stable carbon and hydrogen isotope ratios of atmospheric CH4 (δ13C-CH4 and δD-CH4). The offsets between the laboratories are larger than the measurement reproducibility of individual laboratories. To disentangle plausible offsets between worldwide laboratories, we evaluated and critically assessed a large number of intercomparison results documented previously in the literature. The results indicate significant offsets of δ13C-CH4 and δD-CH4 measurements among datasets reported from different laboratories; the data spread over ranges of 0.5 ‰ for δ13C-CH4 and 13 ‰ for δD-CH4. The intercomparison results summarized in this study may be of help when combining isotope datasets from different laboratories in future studies.