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Saunois, M, Bousquet P, Poulter B, Peregon A, Ciais P, Canadell JG, Dlugokencky EJ, Etiope G, Bastviken D, Houweling S, Janssens-Maenhout G, Tubiello FN, Castaldi S, Jackson RB, Alexe M, Arora VK, Beerling DJ, Bergamaschi P, Blake DR, Brailsford G, Bruhwiler L, Crevoisier C, Crill P, Covey K, Frankenberg C, Gedney N, Hoglund-Isaksson L, Ishizawa M, Ito A, Joos F, Kim HS, Kleinen T, Krummel P, Lamarque JF, Langenfelds R, Locatelli R, Machida T, Maksyutov S, Melton JR, Morino I, Naik V, O'Doherty S, Parmentier FJ, Patra PK, Peng CH, Peng SS, Peters GP, Pison I, Prinn R, Ramonet M, Riley WJ, Saito M, Santini M, Schroeder R, Simpson IJ, Spahni R, Takizawa A, Thornton BF, Tian HQ, Tohjima Y, Viovy N, Voulgarakis A, Weiss R, Wilton DJ, Wiltshire A, Worthy D, Wunch D, Xu XY, Yoshida Y, Zhang BW, Zhang Z, Zhu QA.  2017.  Variability and quasi-decadal changes in the methane budget over the period 2000-2012. Atmospheric Chemistry and Physics. 17:11135-11161.   10.5194/acp-17-11135-2017   AbstractWebsite

Following the recent Global Carbon Project (GCP) synthesis of the decadal methane (CH4) budget over 2000-2012 (Saunois et al., 2016), we analyse here the same dataset with a focus on quasi-decadal and inter-annual variability in CH4 emissions. The GCP dataset integrates results from top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models (including process-based models for estimating land surface emissions and atmospheric chemistry), inventories of anthropogenic emissions, and data-driven approaches. The annual global methane emissions from top-down studies, which by construction match the observed methane growth rate within their uncertainties, all show an increase in total methane emissions over the period 2000-2012, but this increase is not linear over the 13 years. Despite differences between individual studies, the mean emission anomaly of the top-down ensemble shows no significant trend in total methane emissions over the period 2000-2006, during the plateau of atmospheric methane mole fractions, and also over the period 2008-2012, during the renewed atmospheric methane increase. However, the top-down ensemble mean produces an emission shift between 2006 and 2008, leading to 22 [16-32] Tg CH4 yr(-1) higher methane emissions over the period 2008-2012 compared to 2002-2006. This emission increase mostly originated from the tropics, with a smaller contribution from mid-latitudes and no significant change from boreal regions. The regional contributions remain uncertain in top-down studies. Tropical South America and South and East Asia seem to contribute the most to the emission increase in the tropics. However, these two regions have only limited atmospheric measurements and remain therefore poorly constrained. The sectorial partitioning of this emission increase between the periods 2002-2006 and 2008-2012 differs from one atmospheric inversion study to another. However, all top-down studies suggest smaller changes in fossil fuel emissions (from oil, gas, and coal industries) compared to the mean of the bottom-up inventories included in this study. This difference is partly driven by a smaller emission change in China from the top-down studies compared to the estimate in the Emission Database for Global Atmospheric Research (EDGARv4.2) inventory, which should be revised to smaller values in a near future. We apply isotopic signatures to the emission changes estimated for individual studies based on five emission sectors and find that for six individual top-down studies (out of eight) the average isotopic signature of the emission changes is not consistent with the observed change in atmospheric (CH4)-C-13. However, the partitioning in emission change derived from the ensemble mean is consistent with this isotopic constraint. At the global scale, the top-down ensemble mean suggests that the dominant contribution to the resumed atmospheric CH4 growth after 2006 comes from microbial sources (more from agriculture and waste sectors than from natural wetlands), with an uncertain but smaller contribution from fossil CH4 emissions. In addition, a decrease in biomass burning emissions (in agreement with the biomass burning emission databases) makes the balance of sources consistent with atmospheric (CH4)-C-13 observations. In most of the top-down studies included here, OH concentrations are considered constant over the years (seasonal variations but without any inter-annual variability). As a result, the methane loss (in particular through OH oxidation) varies mainly through the change in methane concentrations and not its oxidants. For these reasons, changes in the methane loss could not be properly investigated in this study, although it may play a significant role in the recent atmospheric methane changes as briefly discussed at the end of the paper.

Ganesan, AL, Chatterjee A, Prinn RG, Harth CM, Salameh PK, Manning AJ, Hall BD, Mühle J, Meredith LK, Weiss RF, O'Doherty S, Young D.  2013.  The variability of methane, nitrous oxide and sulfur hexafluoride in Northeast India. Atmos. Chem. Phys.. 13:10633-10644.: Copernicus Publications   10.5194/acp-13-10633-2013   AbstractWebsite

High-frequency atmospheric measurements of methane (CH4), nitrous oxide (N2O) and sulfur hexafluoride (SF6) from Darjeeling, India are presented from December 2011 (CH4)/March 2012 (N2O and SF6) through February 2013. These measurements were made on a gas chromatograph equipped with a flame ionization detector and electron capture detector, and were calibrated on the Tohoku University, the Scripps Institution of Oceanography (SIO)-98 and SIO-2005 scales for CH4, N2O and SF6, respectively. The observations show large variability and frequent pollution events in CH4 and N2O mole fractions, suggesting significant sources in the regions sampled by Darjeeling throughout the year. By contrast, SF6 mole fractions show little variability and only occasional pollution episodes, likely due to weak sources in the region. Simulations using the Numerical Atmospheric dispersion Modelling Environment (NAME) particle dispersion model suggest that many of the enhancements in the three gases result from the transport of pollutants from the densely populated Indo-Gangetic Plains of India to Darjeeling. The meteorology of the region varies considerably throughout the year from Himalayan flows in the winter to the strong south Asian summer monsoon. The model is consistent in simulating a diurnal cycle in CH4 and N2O mole fractions that is present during the winter but absent in the summer and suggests that the signals measured at Darjeeling are dominated by large-scale (~100 km) flows rather than local (<10 km) flows.

Murphy, PP, Harrison DE, Feely RA, Takahashi T, Weiss RF, Gammon RH.  1998.  Variability of Δ pCO2 in the subarctic North Pacific. A comparison of results from four expeditions. Tellus Series B-Chemical and Physical Meteorology. 50:185-204.   10.1034/j.1600-0889.1998.t01-1-00006.x   AbstractWebsite

Time-space variability of surface seawater pCO(2) is examined over the region (150 degrees W-180 degrees, 46 degrees N-50 degrees N) of the subarctic North Pacific where large meridional gradients of temperature and nutrient concentrations exist. The data were collected during four trans-Pacific expeditions in three different years (1985-1987), but within the same 30-day period of the year (August-September). Systematic measurement differences between the four data sets are estimated as <10 mu atm. The inter-expedition comparison suggests that surface seawater pCO(2) in the study area is quite variable, with mean differences of up to 25 mu atm and local differences up to 60 mu atm. Spatial and interannual variability of surface seawater pCO(2) were found to contribute significant uncertainty to estimates of the mean Delta pCO(2) for the study area. Fluxes were calculated using Delta pCO(2) values from the four expeditions combined with gas exchange coefficients calculated from four different wind fields giving a range of -0.94 to +4.1 mmol CO2 m(-2) d(-1). The range of fluxes from the study area is scaled to a larger area of the North Pacific to address how this variability can translate into uncertainties in basin-wide carbon air-sea exchange fluxes.

Vollmer, MK, Weiss RF, Bootsma HA.  2002.  Ventilation of Lake Malawi/Nyasa. The East African great lakes limnology, palaeolimnology, and biodiversity. ( Odada EO, Olago DO, Eds.).:209-233., Dordrecht; Boston, MA: Kluwer Academic Publishers Abstract
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Reverdin, G, Weiss RF, Jenkins WJ.  1993.  Ventilation of the Atlantic Ocean equatorial thermocline. Journal of Geophysical Research-Oceans. 98:16289-16310.   10.1029/93jc00976   AbstractWebsite

The ventilation of the lower equatorial Atlantic thermocline (100 m to 400 m) is investigated from the distributions of salinity, oxygen, the chlorofluoromethanes F-11 and F-12, tritium, and the excess helium 3; 1983 data suggest a correlation on isopycnal surfaces between oxygen, chlorofluoromethanes and to a lesser extent, with the apparent ages derived from F-11/F-12 and helium 3/tritium. The apparent ages increase with depth from 10 years on sigma(THETA)=26.5 to over 15 years near 400 m. The tracers are largely undersaturated with respect to the surface concentrations corresponding to the apparent ages. We investigate the ventilation processes responsible for these distributions with simple circulation models, where water from the subtropical gyres reaches isopycnally the equatorial thermocline. The few model parameters are determined by fitting the simulations to the chlorofluoromethane distributions in 1983. The sensitivity of these parameters to expected errors on the past surface concentrations and to vertical mixing is comparable and can result in an error of more than 20% in the model parameters. In 1983, model [H-3] and [He-3]* are too large, in particular when no diapycnal mixing is modeled, but the differences could have arisen from errors on past surface concentrations. During the 1980s, die model overestimates the increase in chlorofluoromethanes, in particular F-12. The fitted model inflow from the southern subtropical gyre between 110 m and 400 m is 14 x 10(6) m3 s-1, in the range of expected transports by the western boundary current near Brazil. The model oxygen utilization rate is on the order of 12 mmol kg-1 yr-1 at 100 m and 5 mmol kg-1 yr-1 at 400 m (below sigma(theta)=27.1).