Anita L. Ganesan

Rising atmospheric methane: 2007-2014 growth and isotopic shift

From 2007 to 2013, the globally averaged mole fraction of methane in the atmosphere increased by 5.7 ± 1.2 ppb yr−1. Simultaneously, δ13CCH4 (a measure of the 13C/12C isotope ratio in methane) has shifted to significantly more negative values since 2007. Growth was extreme in 2014, at 12.5 ± 0.4 ppb, with a further shift to more negative values being observed at most latitudes. The isotopic evidence presented here suggests that the methane rise was dominated by significant increases in biogenic methane emissions, particularly in the tropics, for example, from expansion of tropical wetlands in years with strongly positive rainfall anomalies or emissions from increased agricultural sources such as ruminants and rice paddies. Changes in the removal rate of methane by the OH radical have not been seen in other tracers of atmospheric chemistry and do not appear to explain short-term variations in methane. Fossil fuel emissions may also have grown, but the sustained shift to more 13C-depleted values and its significant interannual variability, and the tropical and Southern Hemisphere loci of post-2007 growth, both indicate that fossil fuel emissions have not been the dominant factor driving the increase. A major cause of increased tropical wetland and tropical agricultural methane emissions, the likely major contributors to growth, may be their responses to meteorological change.

Role of atmospheric oxidation in recent methane growth

Significance Methane, the second most important greenhouse gas, has varied markedly in its atmospheric growth rate. The cause of these fluctuations remains poorly understood. Recent efforts to determine the drivers of the pause in growth in 1999 and renewed growth from 2007 onward have focused primarily on changes in sources alone. Here, we show that changes in the major methane sink, the hydroxyl radical, have likely played a substantial role in the global methane growth rate. This work has significant implications for our understanding of the methane budget, which is important if we are to better predict future changes in this potent greenhouse gas and effectively mitigate enhanced radiative forcing caused by anthropogenic emissions. The growth in global methane (CH4) concentration, which had been ongoing since the industrial revolution, stalled around the year 2000 before resuming globally in 2007. We evaluate the role of the hydroxyl radical (OH), the major CH4 sink, in the recent CH4 growth. We also examine the influence of systematic uncertainties in OH concentrations on CH4 emissions inferred from atmospheric observations. We use observations of 1,1,1-trichloroethane (CH3CCl3), which is lost primarily through reaction with OH, to estimate OH levels as well as CH3CC3 emissions, which have uncertainty that previously limited the accuracy of OH estimates. We find a 64–70% probability that a decline in OH has contributed to the post-2007 methane rise. Our median solution suggests that CH4 emissions increased relatively steadily during the late 1990s and early 2000s, after which growth was more modest. This solution obviates the need for a sudden statistically significant change in total CH4 emissions around the year 2007 to explain the atmospheric observations and can explain some of the decline in the atmospheric 13CH4/12CH4 ratio and the recent growth in C2H6. Our approach indicates that significant OH-related uncertainties in the CH4 budget remain, and we find that it is not possible to implicate, with a high degree of confidence, rapid global CH4 emissions changes as the primary driver of recent trends when our inferred OH trends and these uncertainties are considered.

Reconciling reported and unreported HFC emissions with atmospheric observations

Significance Hydrofluorocarbons (HFCs) are among the atmosphere’s fastest growing, and most potent, greenhouse gases. Proposals have been made to phase down their use over the coming decades. Such initiatives may largely be informed by existing emissions inventories, which, we show, are the subject of significant uncertainty. In this work, we use atmospheric models and measurements to examine the accuracy of these inventories for five major HFCs. We show that, when aggregated together, reported emissions of these HFCs from developed countries are consistent with the atmospheric measurements, and almost half of global emissions now originate from nonreporting countries. However, the agreement between our results and the inventory breaks down for individual HFC emissions, suggesting inaccuracies in the reporting methods for individual compounds. We infer global and regional emissions of five of the most abundant hydrofluorocarbons (HFCs) using atmospheric measurements from the Advanced Global Atmospheric Gases Experiment and the National Institute for Environmental Studies, Japan, networks. We find that the total CO2-equivalent emissions of the five HFCs from countries that are required to provide detailed, annual reports to the United Nations Framework Convention on Climate Change (UNFCCC) increased from 198 (175–221) Tg-CO2-eq⋅y–1 in 2007 to 275 (246–304) Tg-CO2-eq⋅y–1 in 2012. These global warming potential-weighted aggregated emissions agree well with those reported to the UNFCCC throughout this period and indicate that the gap between reported emissions and global HFC emissions derived from atmospheric trends is almost entirely due to emissions from nonreporting countries. However, our measurement-based estimates of individual HFC species suggest that emissions, from reporting countries, of the most abundant HFC, HFC-134a, were only 79% (63–95%) of the UNFCCC inventory total, while other HFC emissions were significantly greater than the reported values. These results suggest that there are inaccuracies in the reporting methods for individual HFCs, which appear to cancel when aggregated together.

Quantifying aluminum and semiconductor industry perfluorocarbon emissions from atmospheric measurements

United States. National Aeronautics and Space Administration (Upper Atmospheric Research Program Grant NNX11AF17G)

Atmospheric observations show accurate reporting and little growth in India’s methane emissions

Changes in tropical wetland, ruminant or rice emissions are thought to have played a role in recent variations in atmospheric methane (CH4) concentrations. India has the world’s largest ruminant population and produces ~ 20% of the world’s rice. Therefore, changes in these sources could have significant implications for global warming. Here, we infer India’s CH4 emissions for the period 2010–2015 using a combination of satellite, surface and aircraft data. We apply a high-resolution atmospheric transport model to simulate data from these platforms to infer fluxes at sub-national scales and to quantify changes in rice emissions. We find that average emissions over this period are 22.0 (19.6–24.3) Tg yr−1, which is consistent with the emissions reported by India to the United Framework Convention on Climate Change. Annual emissions have not changed significantly (0.2 ± 0.7 Tg yr−1) between 2010 and 2015, suggesting that major CH4 sources did not change appreciably. These findings are in contrast to another major economy, China, which has shown significant growth in recent years due to increasing fossil fuel emissions. However, the trend in a global emission inventory has been overestimated for China due to incorrect rate of fossil fuel growth. Here, we find growth has been overestimated in India but likely due to ruminant and waste sectors.India’s methane emissions have been quantified using atmospheric measurements to provide an independent comparison with reported emissions. Here Ganesan et al. find that derived methane emissions are consistent with India’s reports and no significant trend has been observed between 2010–2015.

Spatio-temporal bivariate statistical models for atmospheric trace-gas inversion

Abstract Atmospheric trace-gas inversion refers to any technique used to predict spatial and temporal fluxes using mole-fraction measurements and atmospheric simulations obtained from computer models. Studies to date are most often of a data-assimilation flavour, which implicitly consider univariate statistical models with the flux as the variate of interest. This univariate approach typically assumes that the flux field is either a spatially correlated Gaussian process or a spatially uncorrelated non-Gaussian process with prior expectation fixed using flux inventories (e.g., NAEI or EDGAR). Here, we extend this approach in three ways. First, we develop a bivariate model for the mole-fraction field and the flux field. The bivariate approach allows optimal prediction of both the flux field and the mole-fraction field, and it leads to significant computational savings over the univariate approach. Second, we employ a lognormal spatial process for the flux field that captures both the lognormal characteristics of the flux field (when appropriate) and its spatial dependence. Third, we propose a new, geostatistical approach to incorporate the flux inventories in our updates, such that the posterior spatial distribution of the flux field is predominantly data-driven. The approach is illustrated on a case study of methane (CH4) emissions in the United Kingdom and Ireland.

Spatially Resolved Isotopic Source Signatures of Wetland Methane Emissions

We present the first spatially‐resolved wetland δ13C(CH4) source signature map based on data characterizing wetland ecosystems and demonstrate good agreement with wetland signatures derived from atmospheric observations. The source signature map resolves a latitudinal difference of ~10‰ between northern high‐latitude (mean ‐67.8‰) and tropical (mean ‐56.7‰) wetlands, and shows significant regional variations on top of the latitudinal gradient. We assess the errors in inverse modeling studies aiming to separate CH4 sources and sinks by comparing atmospheric δ13C(CH4) derived using our spatially‐resolved map against the common assumption of globally uniform wetland δ13C(CH4) signature. We find a larger interhemispheric gradient, a larger high‐latitude seasonal cycle and smaller trend over the period 2000‐2012. The implication is that erroneous CH4 fluxes would be derived to compensate for the biases imposed by not utilizing spatially‐resolved signatures for the largest source of CH4 emissions. These biases are significant when compared to the size of observed signals.

Continued Emissions of the Ozone-Depleting Substance Carbon Tetrachloride From Eastern Asia

Carbon tetrachloride (CCl4) is an ozone-depleting substance, accounting for about 10% of the chlorine in the troposphere. Under the terms of the Montreal Protocol, its production for dispersive uses was banned from 2010. In this work we show that, despite the controls on production being introduced, CCl4 emissions from the eastern part of China did not decline between 2009 and 2016. This finding is in contrast to a recent bottom-up estimate, which predicted a significant decrease in emissions after the introduction of production controls. We find eastern Asian emissions of CCl4 to be 16 (9–24) Gg/year on average between 2009 and 2016, with the primary source regions being in eastern China. The spatial distribution of emissions that we derive suggests that the source distribution of CCl4 in China changed during the 8-year study period, indicating a new source or sources of emissions from China’s Shandong province after 2012.

Quantifying the UK’s Carbon Dioxide Flux: An atmospheric inversemodelling approach using a regional measurement network

We present a method to derive atmosphericobservation-based estimates of carbon dioxide (CO2) fluxes at the national scale, demonstrated using data from a network of surface tall-tower sites across the UK and Ireland over the period 2013–2014. The inversion is carried out using simulations from a Lagrangian chemical transport model and an innovative hierarchical Bayesian Markov chain Monte Carlo (MCMC) framework, which addresses some of the traditional problems faced by inverse modelling studies, such as subjectivity in the specification of model and prior uncertainties. Biospheric fluxes related to gross primary productivity and terrestrial ecosystem respiration are solved separately in the inversion and then combined a posteriori to determine net ecosystem exchange of CO2. Two different models, Data Assimilation Linked Ecosystem Carbon (DALEC) and Joint UK Land Environment Simulator (JULES), provide prior estimates for these fluxes. We carry out separate inversions to assess the impact of these different priors on the posterior flux estimates and evaluate the differences between the prior and posterior estimates in terms of missing model components. The Numerical Atmospheric dispersion Modelling Environment (NAME) is used to relate fluxes to the measurements taken across the regional network. Posterior CO2 estimates from the two inversions agree within estimated uncertainties, despite large differences in the prior fluxes from the different models. With our method, averaging results from 2013 and 2014, we find a total annual net biospheric flux for the UK of 8± 79 Tg CO2 yr−1 (DALEC prior) and 64± 85 Tg CO2 yr−1 (JULES prior), where negative values represent an uptake of CO2. These biospheric CO2 estimates show that annual UK biospheric sources and sinks are roughly in balance. These annual mean estimates consistently indicate a greater net release of CO2 than the prior estimates, which show much more pronounced uptake in summer months. Published by Copernicus Publications on behalf of the European Geosciences Union. 4346 E. D. White et al.: Quantifying the UK’s carbon dioxide flux: an atmospheric inverse modelling approach