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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. Atmospheric non-methane hydrocarbons (NMHCs) play an important role in theformation of secondary organic aerosols and ozone. After a multidecadalglobal decline in atmospheric mole fractions of ethane and propane – themost abundant atmospheric NMHCs – previous work has shown a reversal ofthis trend with increasing atmospheric abundances from 2009 to 2015 in theNorthern Hemisphere. These concentration increases were attributed to theunprecedented growth in oil and natural gas (O&NG) production in NorthAmerica. Here, we supplement this trend analysis building on the long-term(2008–2010; 2012–2020) high-resolution (∼3 h) record ofambient air C2–C7 NMHCs from in situ measurements at the GreenlandEnvironmental Observatory at Summit station (GEOSummit, 72.58 ∘ N,38.48 ∘ W; 3210 m above sea level). We confirm previous findingsthat the ethane mole fraction significantly increased by +69.0 [+47.4,+73.2; 95 % confidence interval] ppt yr−1 from January 2010 toDecember 2014. Subsequent measurements, however, reveal a significantdecrease by −58.4 [−64.1, −48.9] ppt yr−1 from January 2015 to December2018. A similar reversal is found for propane. The upturn observed after2019 suggests, however, that the pause in the growth of atmospheric ethaneand propane might only have been temporary. Discrete samples collected atother northern hemispheric baseline sites under the umbrella of the NOAAcooperative global air sampling network show a similar decrease in 2015–2018and suggest a hemispheric pattern. Here, we further discuss the potentialcontribution of biomass burning and O&NG emissions (the main sources ofethane and propane) and conclude that O&NG activities likely played arole in these recent changes. This study highlights the crucial need forbetter constrained emission inventories.