The growth in global methane (CH 4 ) 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 CH 4 sink, in the recent CH 4 growth. We also examine the influence of systematic uncertainties in OH concentrations on CH 4 emissions inferred from atmospheric observations. We use observations of 1,1,1-trichloroethane (CH 3 CCl 3 ), which is lost primarily through reaction with OH, to estimate OH levels as well as CH 3 CCl 3 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 CH 4 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 CH 4 emissions around the year 2007 to explain the atmospheric observations and can explain some of the decline in the atmospheric 13 CH 4 / 12 CH 4 ratio and the recent growth in C 2 H 6 . Our approach indicates that significant OH-related uncertainties in the CH 4 budget remain, and we find that it is not possible to implicate, with a high degree of confidence, rapid global CH 4 emissions changes as the primary driver of recent trends when our inferred OH trends and these uncertainties are considered., the second most important partially anthropogenic greenhouse gas, is observed to vary markedly in its year to year growth rate (Fig. 1). The causes of these variations have been the subject of much controversy and uncertainty, primarily because there is a wide range of poorly quantified sources and because its sinks are ill-constrained (1). Of particular recent interest are the cause of the "pause" in CH4 growth between 1999 and 2007 and the renewed growth from 2007 onward (2-7). It is important that we understand these changes if we are to better project future CH4 changes and effectively mitigate enhanced radiative forcing caused by anthropogenic methane emissions.The major sources of CH4 include wetlands (natural and agricultural), fossil fuel extraction and distribution, enteric fermentation in ruminant animals, and solid and liquid waste. Our understanding of the sources of CH4 comes from two approaches: "bottom up," in which inventories or process models are used to predict fluxes, or "top down," in which fluxes are inferred from observations assimilated into atmospheric chemical transport models. Bottom-up methods suffer from uncertainties and potential biases in the available activity data or emissions factors or the extrapolation to large scales of a relatively small number of observations. Furthermore, there is no constraint on the global total emissions from bottom-up techniques. The topdown approach is limited by incomplete or imperfect observations and our understanding of atmospheric transport and chemical sinks. For CH4, these di...

The recovery of the stratospheric ozone layer relies on the continued decline in the atmospheric concentrations of ozone-depleting gases such as the chlorofluorocarbons 1. The atmospheric concentration of trichlorofluoromethane (CFC-11), the second most abundant chlorofluorocarbon, has declined substantially since the mid-1990s 2. A recently reported slowdown in the decline of the atmospheric concentration of CFC-11 after 2012, however, implies that global emissions have increased 3,4. A concurrent increase in CFC-11 emissions from eastern Asia contributes to the global emission increase, but the location and magnitude of this regional source remain uncertain 3. Here we use high-frequency atmospheric observations from Gosan, Republic of Korea and Hateruma, Japan, together with global monitoring data and atmospheric chemical transport model simulations to investigate regional CFC-11 emissions from eastern Asia. We find that emissions from eastern mainland China are 7.0 ± 3.0 Gg yr-1 higher in 2014-2017 compared to 2008-2012, and the emissions increase arises primarily around the northeastern provinces of Shandong and Hebei. This increase accounts for a substantial fraction (about 40-60%, or more) of the global CFC-11 emission rise. We find no evidence for a significant increase in emissions from any other eastern Asian countries or other regions of the world where available data allow for the detection of regional emissions. Attribution of any remaining fraction of the global CFC-11 emission rise to other regions is limited by the sparsity of long-term measurements of sufficient frequency near potentially emissive regions. Multiple considerations suggest that the increase in CFC-11 emissions from eastern mainland China is likely the result of new Energy & Industrial Strategy (BEIS, UK, formerly the Department of Energy and Climate Change (DECC)) contract 1028/06/2015 to the University of Bristol and the UK Meteorological Office. Ragged Point, Barbados is supported by the National Oceanic and Atmospheric Administration (NOAA, USA), contract RA-133-R15-CN-0008 to the University of Bristol. L.W., M.L.

Abstract. Emissions of methane (CH4) from tropical ecosystems, and how they respond to changes in climate, represent one of the biggest uncertainties associated with the global CH4 budget. Historically, this has been due to the dearth of pan-tropical in situ measurements, which is particularly acute in Africa. By virtue of their superior spatial coverage, satellite observations of atmospheric CH4 columns can help to narrow down some of the uncertainties in the tropical CH4 emission budget. We use proxy column retrievals of atmospheric CH4 (XCH4) from the Japanese Greenhouse gases Observing Satellite (GOSAT) and the nested version of the GEOS-Chem atmospheric chemistry and transport model (0.5∘×0.625∘) to infer emissions from tropical Africa between 2010 and 2016. Proxy retrievals of XCH4 are less sensitive to scattering due to clouds and aerosol than full physics retrievals, but the method assumes that the global distribution of carbon dioxide (CO2) is known. We explore the sensitivity of inferred a posteriori emissions to this source of systematic error by using two different XCH4 data products that are determined using different model CO2 fields. We infer monthly emissions from GOSAT XCH4 data using a hierarchical Bayesian framework, allowing us to report seasonal cycles and trends in annual mean values. We find mean tropical African emissions between 2010 and 2016 range from 76 (74–78) to 80 (78–82) Tg yr−1, depending on the proxy XCH4 data used, with larger differences in Northern Hemisphere Africa than Southern Hemisphere Africa. We find a robust positive linear trend in tropical African CH4 emissions for our 7-year study period, with values of 1.5 (1.1–1.9) Tg yr−1 or 2.1 (1.7–2.5) Tg yr−1, depending on the CO2 data product used in the proxy retrieval. This linear emissions trend accounts for around a third of the global emissions growth rate during this period. A substantial portion of this increase is due to a short-term increase in emissions of 3 Tg yr−1 between 2011 and 2015 from the Sudd in South Sudan. Using satellite land surface temperature anomalies and altimetry data, we find this increase in CH4 emissions is consistent with an increase in wetland extent due to increased inflow from the White Nile, although the data indicate that the Sudd was anomalously dry at the start of our inversion period. We find a strong seasonality in emissions across Northern Hemisphere Africa, with the timing of the seasonal emissions peak coincident with the seasonal peak in ground water storage. In contrast, we find that a posteriori CH4 emissions from the wetland area of the Congo Basin are approximately constant throughout the year, consistent with less temporal variability in wetland extent, and significantly smaller than a priori estimates.

Chloroform (CHCl3) contributes to the depletion of the stratospheric ozone layer. However, due to its short lifetime and predominantly natural sources, it is not included in the Montreal Protocol that regulates the production and uses of ozone depleting substances. Atmospheric chloroform mole fractions were relatively stable or slowly decreased during 1990-2010. Here, we show that global chloroform mole fractions increased after 2010, based on in situ chloroform measurements at seven stations around the world. We estimate that the global chloroform emissions grew at the rate of 3.5% yr-1 between 2010 and 2015 based on atmospheric model simulations. We use two regional inverse modelling approaches, combined with observations from East Asia, to show that emissions from eastern China grew by 49 (41-59) Gg between 2010 and 2015, a change that could explain the entire increase in global emissions. We suggest that if chloroform emissions continuously grow at the current rate, the recovery of the stratospheric ozone layer above Antarctica could be delayed by several years. 22. Hossaini, R., et al. A multi-model intercomparison of halogenated very short-lived substances (TransCom-VSLS): linking oceanic emissions and tropospheric transport for a reconciled estimate of the stratospheric source gas injection of bromine. Atmos. Chem. Phys. 16, 9163-9187 (2016). 23. Yu, P., et al. Efficient transport of tropospheric aerosol into the stratosphere via the Asian summer monsoon anticyclone.

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 CO 2 -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-CO 2 -eq·y -1 in 2007 to 275 (246-304) Tg-CO 2 -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 measurementbased 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.halocarbons | radiative forcing | climate change