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Abstract. Nitrous oxide (N2O) is a potent greenhouse gas emitted by oceanic and terrestrial sources, with its biogeochemical cycle influenced by both natural processes and anthropogenic activities. Current atmospheric N2O monitoring networks, including tall-tower and flask measurements, often overlook major marine hotspots, such as the eastern tropical Pacific Ocean. We present the first 15 months of high-frequency continuous measurements of N2O and carbon monoxide from the newly established Galapagos Emissions Monitoring Station (GEMS) in this region. Over this period, N2O mole fractions vary by approximately 5 ppb, influenced by seasonal trade winds, local anthropogenic emissions, and air masses transported from marine N2O hotspots. Notably, between February and April 2024, we observe high variability linked to the southward shift of the intertropical convergence zone and weakened trade winds over the Galapagos Islands. Increased variability during this period is driven by stagnant local winds, which accumulate emissions, and the mixing of air masses with different N2O content from the northern and southern hemispheres. The remaining variability is primarily due to differences in air mass transport and heterogeneity in surface fluxes from the eastern tropical Pacific. Air masses passing over the Peruvian and Chilean upwelling systems— key sources of oceanic N2O efflux — show markedly higher N2O mole fractions at the GEMS station. 

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. Nitrous oxide (N2O) is a long-lived potent greenhouse gas and stratospheric ozone-depleting substance that has been accumulating in the atmosphere since the preindustrial period. The mole fraction of atmospheric N2O has increased by nearly 25 % from 270 ppb (parts per billion) in 1750 to 336 ppb in 2022, with the fastest annual growth rate since 1980 of more than 1.3 ppb yr−1 in both 2020 and 2021. According to the Sixth Assessment Report of the Intergovernmental Panel on Climate Change (IPCC AR6), the relative contribution of N2O to the total enhanced effective radiative forcing of greenhouse gases was 6.4 % for 1750–2022. As a core component of our global greenhouse gas assessments coordinated by the Global Carbon Project (GCP), our global N2O budget incorporates both natural and anthropogenic sources and sinks and accounts for the interactions between nitrogen additions and the biogeochemical processes that control N2O emissions. We use bottom-up (BU: inventory, statistical extrapolation of flux measurements, and process-based land and ocean modeling) and top-down (TD: atmospheric measurement-based inversion) approaches. We provide a comprehensive quantification of global N2O sources and sinks in 21 natural and anthropogenic categories in 18 regions between 1980 and 2020. We estimate that total annual anthropogenic N2O emissions have increased 40 % (or 1.9 Tg N yr−1) in the past 4 decades (1980–2020). Direct agricultural emissions in 2020 (3.9 Tg N yr−1, best estimate) represent the large majority of anthropogenic emissions, followed by other direct anthropogenic sources, including fossil fuel and industry, waste and wastewater, and biomass burning (2.1 Tg N yr−1), and indirect anthropogenic sources (1.3 Tg N yr−1) . For the year 2020, our best estimate of total BU emissions for natural and anthropogenic sources was 18.5 (lower–upper bounds: 10.6–27.0) Tg N yr−1, close to our TD estimate of 17.0 (16.6–17.4) Tg N yr−1. For the 2010–2019 period, the annual BU decadal-average emissions for both natural and anthropogenic sources were 18.2 (10.6–25.9) Tg N yr−1 and TD emissions were 17.4 (15.8–19.20) Tg N yr−1. The once top emitter Europe has reduced its emissions by 31 % since the 1980s, while those of emerging economies have grown, making China the top emitter since the 2010s. The observed atmospheric N2O concentrations in recent years have exceeded projected levels under all scenarios in the Coupled Model Intercomparison Project Phase 6 (CMIP6), underscoring the importance of reducing anthropogenic N2O emissions. To evaluate mitigation efforts and contribute to the Global Stocktake of the United Nations Framework Convention on Climate Change, we propose the establishment of a global network for monitoring and modeling N2O from the surface through to the stratosphere. The data presented in this work can be downloaded from https://doi.org/10.18160/RQ8P-2Z4R (Tian et al., 2023). 

The Southern Ocean plays an important role in determining atmospheric carbon dioxide (CO 2 ), yet estimates of air-sea CO 2 flux for the region diverge widely. In this study, we constrained Southern Ocean air-sea CO 2 exchange by relating fluxes to horizontal and vertical CO 2 gradients in atmospheric transport models and applying atmospheric observations of these gradients to estimate fluxes. Aircraft-based measurements of the vertical atmospheric CO 2 gradient provide robust flux constraints. We found an annual mean flux of –0.53 ± 0.23 petagrams of carbon per year (net uptake) south of 45°S during the period 2009–2018. This is consistent with the mean of atmospheric inversion estimates and surface-ocean partial pressure of CO 2 ( P co 2 )–based products, but our data indicate stronger annual mean uptake than suggested by recent interpretations of profiling float observations. 

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.