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Abstract. Since 1999, Environment and Climate Change Canada (ECCC) has been coordinating a multi-laboratory comparison of measurements of long-lived greenhouse gases in whole air samples collected at the Global Atmosphere Watch (GAW) Alert Observatory located in the Canadian High Arctic (82∘28′ N, 62∘30′ W). In this paper, we evaluate the measurement agreement of atmospheric CO2, CH4, N2O, SF6, and stable isotopes of CO2 (δ13C, δ18O) between leading laboratories from seven independent international institutions. The measure of success is linked to target goals for network compatibility outlined by the World Meteorological Organization's (WMO) GAW greenhouse gas measurement community. Overall, based on ∼ 8000 discrete flask samples, we find that the co-located atmospheric CO2 and CH4 measurement records from Alert by CSIRO, MPI-BGC, SIO, UHEI-IUP, and ECCC versus NOAA (the designated reference laboratory) are generally consistent with the WMO compatibility goals of ± 0.1 ppm CO2 and ± 2 ppb CH4 over the 17-year period (1999–2016), although there are periods where differences exceed target levels and persist as systematic bias for months or years. Consistency with the WMO goals for N2O, SF6, and stable isotopes of CO2 (δ13C, δ18O) has not been demonstrated. Additional analysis of co-located comparison measurements between CSIRO and SIO versus NOAA or INSTAAR (for the isotopes of CO2) at other geographical sites suggests that the findings at Alert for CO2, CH4, N2O, and δ13C–CO2 could be extended across the CSIRO, SIO, and NOAA observing networks. The primary approach to estimate an overall measurement agreement level was carried out by pooling the differences of all individual laboratories versus the designated reference laboratory and determining the 95th percentile range of these data points. Using this approach over the entire data record, our best estimate of the measurement agreement range is −0.51 to +0.53 ppm for CO2, −0.09 ‰ to +0.07 ‰ for δ13C, −0.50 ‰ to +0.58 ‰ for δ18O, −4.86 to +6.16 ppb for CH4, −0.75 to +1.20 ppb for N2O, and −0.14 to +0.09 ppt for SF6. A secondary approach of using the average of 2 standard deviations of the means for all flask samples taken in each individual sampling episode provided similar results. These upper and lower limits represent our best estimate of the measurement agreement at the 95 % confidence level for these individual laboratories, providing more confidence for using these datasets in various scientific applications (e.g., long-term trend analysis). 

The atmospheric history of molecular hydrogen (H 2 ) from 1852 to 2003 was reconstructed from measurements of firn air collected at Megadunes, Antarctica. The reconstruction shows that H 2 levels in the southern hemisphere were roughly constant near 330 parts per billion (ppb; nmol H 2 mol −1 air) during the mid to late 1800s. Over the twentieth century, H 2 levels rose by about 70% to 550 ppb. The reconstruction shows good agreement with the H 2 atmospheric history based on firn air measurements from the South Pole. The broad trends in atmospheric H 2 over the twentieth century can be explained by increased methane oxidation and anthropogenic emissions. The H 2 rise shows no evidence of deceleration during the last quarter of the twentieth century despite an expected reduction in automotive emissions following more stringent regulations. During the late twentieth century, atmospheric CO levels decreased due to a reduction in automotive emissions. It is surprising that atmospheric H 2 did not respond similarly as automotive exhaust is thought to be the dominant source of anthropogenic H 2. The monotonic late twentieth century rise in H 2 levels is consistent with late twentieth-century flask air measurements from high southern latitudes. An additional unknown source of H 2 is needed to explain twentieth-century trends in atmospheric H 2 and to resolve the discrepancy between bottom-up and top-down estimates of the anthropogenic source term. The firn air–based atmospheric history of H 2 provides a baseline from which to assess human impact on the H 2 cycle over the last 150 y and validate models that will be used to project future trends in atmospheric composition as H 2 becomes a more common energy source. 

Abstract. Understanding and quantifying the global methane (CH4) budgetis important for assessing realistic pathways to mitigate climate change.Atmospheric emissions and concentrations of CH4 continue to increase,making CH4 the second most important human-influenced greenhouse gas interms of climate forcing, after carbon dioxide (CO2). The relativeimportance of CH4 compared to CO2 depends on its shorteratmospheric lifetime, stronger warming potential, and variations inatmospheric growth rate over the past decade, the causes of which are stilldebated. Two major challenges in reducing uncertainties in the atmosphericgrowth rate arise from the variety of geographically overlapping CH4sources and from the destruction of CH4 by short-lived hydroxylradicals (OH). To address these challenges, we have established aconsortium of multidisciplinary scientists under the umbrella of the GlobalCarbon Project to synthesize and stimulate new research aimed at improvingand regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paperdedicated to the decadal methane budget, integrating results of top-downstudies (atmospheric observations within an atmospheric inverse-modellingframework) and bottom-up estimates (including process-based models forestimating land surface emissions and atmospheric chemistry, inventories ofanthropogenic emissions, and data-driven extrapolations). For the 2008–2017 decade, global methane emissions are estimated byatmospheric inversions (a top-down approach) to be 576 Tg CH4 yr−1 (range 550–594, corresponding to the minimum and maximumestimates of the model ensemble). Of this total, 359 Tg CH4 yr−1 or∼ 60 % is attributed to anthropogenic sources, that isemissions caused by direct human activity (i.e. anthropogenic emissions; range 336–376 Tg CH4 yr−1 or 50 %–65 %). The mean annual total emission for the new decade (2008–2017) is29 Tg CH4 yr−1 larger than our estimate for the previous decade (2000–2009),and 24 Tg CH4 yr−1 larger than the one reported in the previousbudget for 2003–2012 (Saunois et al., 2016). Since 2012, global CH4emissions have been tracking the warmest scenarios assessed by theIntergovernmental Panel on Climate Change. Bottom-up methods suggest almost30 % larger global emissions (737 Tg CH4 yr−1, range 594–881)than top-down inversion methods. Indeed, bottom-up estimates for naturalsources such as natural wetlands, other inland water systems, and geologicalsources are higher than top-down estimates. The atmospheric constraints onthe top-down budget suggest that at least some of these bottom-up emissionsare overestimated. The latitudinal distribution of atmosphericobservation-based emissions indicates a predominance of tropical emissions(∼ 65 % of the global budget, < 30∘ N)compared to mid-latitudes (∼ 30 %, 30–60∘ N)and high northern latitudes (∼ 4 %, 60–90∘ N). The most important source of uncertainty in the methanebudget is attributable to natural emissions, especially those from wetlandsand other inland waters. Some of our global source estimates are smaller than those in previouslypublished budgets (Saunois et al., 2016; Kirschke et al., 2013). In particular wetland emissions are about 35 Tg CH4 yr−1 lower due toimproved partition wetlands and other inland waters. Emissions fromgeological sources and wild animals are also found to be smaller by 7 Tg CH4 yr−1 by 8 Tg CH4 yr−1, respectively. However, the overalldiscrepancy between bottom-up and top-down estimates has been reduced byonly 5 % compared to Saunois et al. (2016), due to a higher estimate of emissions from inland waters, highlighting the need for more detailed research on emissions factors. Priorities for improving the methanebudget include (i) a global, high-resolution map of water-saturated soilsand inundated areas emitting methane based on a robust classification ofdifferent types of emitting habitats; (ii) further development ofprocess-based models for inland-water emissions; (iii) intensification ofmethane observations at local scales (e.g., FLUXNET-CH4 measurements)and urban-scale monitoring to constrain bottom-up land surface models, andat regional scales (surface networks and satellites) to constrainatmospheric inversions; (iv) improvements of transport models and therepresentation of photochemical sinks in top-down inversions; and (v) development of a 3D variational inversion system using isotopic and/orco-emitted species such as ethane to improve source partitioning. The data presented here can be downloaded fromhttps://doi.org/10.18160/GCP-CH4-2019 (Saunois et al., 2020) and from theGlobal Carbon Project.