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Miller, BR, Rigby M, Kuijpers LJM, Krummel PB, Steele LP, Leist M, Fraser PJ, McCulloch A, Harth C, Salameh P, Muhle J, Weiss RF, Prinn RG, Wang RHJ, O'Doherty S, Greally BR, Simmonds PG.  2010.  HFC-23 (CHF3) emission trend response to HCFC-22 (CHClF2) production and recent HFC-23 emission abatement measures. Atmospheric Chemistry and Physics. 10:7875-7890.   10.5194/acp-10-7875-2010   AbstractWebsite

HFC-23 (also known as CHF(3), fluoroform or trifluoromethane) is a potent greenhouse gas (GHG), with a global warming potential (GWP) of 14 800 for a 100-year time horizon. It is an unavoidable by-product of HCFC-22 (CHClF(2), chlorodifluoromethane) production. HCFC-22, an ozone depleting substance (ODS), is used extensively in commercial refrigeration and air conditioning, in the extruded polystyrene (XPS) foam industries (dispersive applications) and also as a feedstock in fluoropolymer manufacture (a non-dispersive use). Aside from small markets in specialty uses, HFC-23 has historically been considered a waste gas that was, and often still is, simply vented to the atmosphere. Efforts have been made in the past two decades to reduce HFC-23 emissions, including destruction (incineration) in facilities in developing countries under the United Nations Framework Convention on Climate Change's (UNFCCC) Clean Development Mechanism (CDM), and by process optimization and/or voluntary incineration by most producers in developed countries. We present observations of lower-tropospheric mole fractions of HFC-23 measured by 'Medusa' GC/MSD instruments from ambient air sampled in situ at the Advanced Global Atmospheric Gases Experiment (AGAGE) network of five remote sites (2007-2009) and in Cape Grim air archive (CGAA) samples (1978-2009) from Tasmania, Australia. These observations are used with the AGAGE 2-D atmospheric 12-box model and an inverse method to produce model mole fractions and a 'top-down' HFC-23 emission history. The model 2009 annual mean global lower-tropospheric background abundance is 22.6 (+/- 0.2) pmol mol(-1). The derived HFC-23 emissions show a 'plateau' during 1997-2003, followed by a rapid similar to 50% increase to a peak of 15.0 (+1.3/-1.2) Gg/yr in 2006. Following this peak, emissions of HFC-23 declined rapidly to 8.6 (+0.9/-1.0) Gg/yr in 2009, the lowest annual emission of the past 15 years. We derive a 1990-2008 'bottom-up' HFC-23 emission history using data from the United Nations Environment Programme and the UNFCCC. Comparison with the top-down HFC-23 emission history shows agreement within the stated uncertainties. In the 1990s, HFC-23 emissions from developed countries dominated all other sources, then began to decline and eventually became fairly constant during 2003-2008. By this point, with developed countries' emissions essentially at a plateau, the major factor controlling the annual dynamics of global HFC-23 emissions became the historical rise of developing countries' HCFC-22 dispersive use production, which peaked in 2007. Thereafter in 2007-2009, incineration through CDM projects became a larger factor, reducing global HFC-23 emissions despite rapidly rising HCFC-22 feedstock production in developing countries.

Rigby, M, Muhle J, Miller BR, Prinn RG, Krummel PB, Steele LP, Fraser PJ, Salameh PK, Harth CM, Weiss RF, Greally BR, O'Doherty S, Simmonds PG, Vollmer MK, Reimann S, Kim J, Kim KR, Wang HJ, Olivier JGJ, Dlugokencky EJ, Dutton GS, Hall BD, Elkins JW.  2010.  History of atmospheric SF6 from 1973 to 2008. Atmospheric Chemistry and Physics. 10:10305-10320.   10.5194/acp-10-10305-2010   AbstractWebsite

We present atmospheric sulfur hexafluoride (SF(6)) mole fractions and emissions estimates from the 1970s to 2008. Measurements were made of archived air samples starting from 1973 in the Northern Hemisphere and from 1978 in the Southern Hemisphere, using the Advanced Global Atmospheric Gases Experiment (AGAGE) gas chromatographic-mass spectrometric (GC-MS) systems. These measurements were combined with modern high-frequency GC-MS and GC-electron capture detection (ECD) data from AGAGE monitoring sites, to produce a unique 35-year atmospheric record of this potent greenhouse gas. Atmospheric mole fractions were found to have increased by more than an order of magnitude between 1973 and 2008. The 2008 growth rate was the highest recorded, at 0.29 +/- 0.02 pmol mol(-1) yr(-1). A three-dimensional chemical transport model and a minimum variance Bayesian inverse method was used to estimate annual emission rates using the measurements, with a priori estimates from the Emissions Database for Global Atmospheric Research (EDGAR, version 4). Consistent with the mole fraction growth rate maximum, global emissions during 2008 were also the highest in the 1973-2008 period, reaching 7.4 +/- 0.6 Gg yr(-1) (1-sigma uncertainties) and surpassing the previous maximum in 1995. The 2008 values follow an increase in emissions of 48 +/- 20% since 2001. A second global inversion which also incorporated National Oceanic and Atmospheric Administration (NOAA) flask measurements and in situ monitoring site data agreed well with the emissions derived using AGAGE measurements alone. By estimating continent-scale emissions using all available AGAGE and NOAA surface measurements covering the period 2004-2008, with no pollution filtering, we find that it is likely that much of the global emissions rise during this five-year period originated primarily from Asian developing countries that do not report detailed, annual emissions to the United Nations Framework Convention on Climate Change (UNFCCC). We also find it likely that SF(6) emissions reported to the UNFCCC were underestimated between at least 2004 and 2005.

Stohl, A, Kim J, Li S, O'Doherty S, Muhle J, Salameh PK, Saito T, Vollmer MK, Wan D, Weiss RF, Yao B, Yokouchi Y, Zhou LX.  2010.  Hydrochlorofluorocarbon and hydrofluorocarbon emissions in East Asia determined by inverse modeling. Atmospheric Chemistry and Physics. 10:3545-3560.   10.5194/acp-10-3545-2010   AbstractWebsite

The emissions of three hydrochlorofluorocarbons, HCFC-22 (CHClF(2)), HCFC-141b (CH(3)CCl(2)F) and HCFC-142b (CH(3)CClF(2)) and three hydrofluorocarbons, HFC-23 (CHF(3)), HFC-134a (CH(2)FCF(3)) and HFC-152a (CH(3)CHF(2)) from four East Asian countries and the Taiwan region for the year 2008 are determined by inverse modeling. The inverse modeling is based on in-situ measurements of these halocarbons at the Japanese stations Cape Ochi-ishi and Hateruma, the Chinese station Shangdianzi and the South Korean station Gosan. For every station and every 3 h, 20-day backward calculations were made with the Lagrangian particle dispersion model FLEXPART. The model output, the measurement data, bottom-up emission information and corresponding uncertainties were fed into an inversion algorithm to determine the regional emission fluxes. The model captures the observed variation of halocarbon mixing ratios very well for the two Japanese stations but has difficulties explaining the large observed variability at Shangdianzi, which is partly caused by small-scale transport from Beijing that is not adequately captured by the model. Based on HFC-23 measurements, the inversion algorithm could successfully identify the locations of factories known to produce HCFC-22 and emit HFC-23 as an unintentional byproduct. This lends substantial credibility to the inversion method. We report national emissions for China, North Korea, South Korea and Japan, as well as emissions for the Taiwan region. Halocarbon emissions in China are much larger than the emissions in the other countries together and contribute a substantial fraction to the global emissions. Our estimates of Chinese emissions for the year 2008 are 65.3 +/- 6.6 kt/yr for HCFC-22 (17% of global emissions extrapolated from Montzka et al., 2009), 12.1 +/- 1.6 kt/yr for HCFC-141b (22%), 7.3 +/- 0.7 kt/yr for HCFC-142b (17%), 6.2 +/- 0.7 kt/yr for HFC-23 (> 50%), 12.9 +/- 1.7 kt/yr for HFC-134a (9% of global emissions estimated from Velders et al., 2009) and 3.4 +/- 0.5 kt/yr for HFC-152a (7%).

Xiao, X, Prinn RG, Fraser PJ, Simmonds PG, Weiss RF, O'Doherty S, Miller BR, Salameh PK, Harth CM, Krummel PB, Porter LW, Muhle J, Greally BR, Cunnold D, Wang R, Montzka SA, Elkins JW, Dutton GS, Thompson TM, Butler JH, Hall BD, Reimann S, Vollmer MK, Stordal F, Lunder C, Maione M, Arduini J, Yokouchi Y.  2010.  Optimal estimation of the surface fluxes of methyl chloride using a 3-D global chemical transport model. Atmospheric Chemistry and Physics. 10:5515-5533.   10.5194/acp-10-5515-2010   AbstractWebsite

Methyl chloride (CH(3)Cl) is a chlorine-containing trace gas in the atmosphere contributing significantly to stratospheric ozone depletion. Large uncertainties in estimates of its source and sink magnitudes and temporal and spatial variations currently exist. GEIA inventories and other bottom-up emission estimates are used to construct a priori maps of the surface fluxes of CH(3)Cl. The Model of Atmospheric Transport and Chemistry (MATCH), driven by NCEP interannually varying meteorological data, is then used to simulate CH(3)Cl mole fractions and quantify the time series of sensitivities of the mole fractions at each measurement site to the surface fluxes of various regional and global sources and sinks. We then implement the Kalman filter (with the unit pulse response method) to estimate the surface fluxes on regional/global scales with monthly resolution from January 2000 to December 2004. High frequency observations from the AGAGE, SOGE, NIES, and NOAA/ESRL HATS in situ networks and low frequency observations from the NOAA/ESRL HATS flask network are used to constrain the source and sink magnitudes. The inversion results indicate global total emissions around 4100 +/- 470 Ggyr(-1) with very large emissions of 2200 +/- 390 Gg yr(-1) from tropical plants, which turn out to be the largest single source in the CH(3)Cl budget. Relative to their a priori annual estimates, the inversion increases global annual fungal and tropical emissions, and reduces the global oceanic source. The inversion implies greater seasonal and interannual oscillations of the natural sources and sink of CH(3)Cl compared to the a priori. The inversion also reflects the strong effects of the 2002/2003 globally widespread heat waves and droughts on global emissions from tropical plants, biomass burning and salt marshes, and on the soil sink.

Muhle, J, Ganesan AL, Miller BR, Salameh PK, Harth CM, Greally BR, Rigby M, Porter LW, Steele LP, Trudinger CM, Krummel PB, O'Doherty S, Fraser PJ, Simmonds PG, Prinn RG, Weiss RF.  2010.  Perfluorocarbons in the global atmosphere: tetrafluoromethane, hexafluoroethane, and octafluoropropane. Atmospheric Chemistry and Physics. 10:5145-5164.   10.5194/acp-10-5145-2010   AbstractWebsite

We present atmospheric baseline growth rates from the 1970s to the present for the long-lived, strongly infrared-absorbing perfluorocarbons (PFCs) tetrafluoromethane (CF(4)), hexafluoroethane (C(2)F(6)), and octafluoropropane (C(3)F(8)) in both hemispheres, measured with improved accuracies (similar to 1-2%) and precisions (<0.3%, or <0.2 ppt (parts per trillion dry air mole fraction), for CF(4); <1.5%, or <0.06 ppt, for C(2)F(6); <4.5%, or <0.02 ppt, for C3F8) within the Advanced Global Atmospheric Gases Experiment (AGAGE). Pre-industrial background values of 34.7 +/- 0.2 ppt CF(4) and 0.1 +/- 0.02 ppt C(2)F(6) were measured in air extracted from Greenland ice and Antarctic firn. Anthropogenic sources are thought to be primary aluminum production (CF(4), C(2)F(6), C(3)F(8)), semiconductor production (C(2)F(6), CF(4), C(3)F(8)) and refrigeration use (C(3)F(8)). Global emissions calculated with the AGAGE 2-D 12-box model are significantly higher than most previous emission estimates. The sum of CF(4) and C(2)F(6) emissions estimated from aluminum production and non-metal production are lower than observed global top-down emissions, with gaps of similar to 6 Gg/yr CF(4) in recent years. The significant discrepancies between previous CF(4), C(2)F(6), and C(3)F(8) emission estimates and observed global top-down emissions estimated from AGAGE measurements emphasize the need for more accurate, transparent, and complete emission reporting, and for verification with atmospheric measurements to assess the emission sources of these long-lived and potent greenhouse gases, which alter the radiative budget of the atmosphere, essentially permanently, once emitted.

Muhle, J, Huang J, Weiss RF, Prinn RG, Miller BR, Salameh PK, Harth CM, Fraser PJ, Porter LW, Greally BR, O'Doherty S, Simmonds PG.  2009.  Sulfuryl fluoride in the global atmosphere. Journal of Geophysical Research-Atmospheres. 114   10.1029/2008jd011162   AbstractWebsite

The first calibrated high-frequency, high-precision, in situ atmospheric and archived air measurements of the fumigant sulfuryl fluoride (SO(2)F(2)) have been made as part of the Advanced Global Atmospheric Gas Experiment (AGAGE) program. The global tropospheric background concentration of SO(2)F(2) has increased by 5 +/- 1% per year from similar to 0.3 ppt (parts per trillion, dry air mol fraction) in 1978 to similar to 1.35 ppt in May 2007 in the Southern Hemisphere, and from similar to 1.08 ppt in 1999 to similar to 1.53 ppt in May 2007 in the Northern Hemisphere. The SO(2)F(2) interhemispheric concentration ratio was 1.13 +/- 0.02 from 1999 to 2007. Two-dimensional 12-box model inversions yield global total and global oceanic uptake atmospheric lifetimes of 36 +/- 11 and 40 +/- 13 years, respectively, with hydrolysis in the ocean being the dominant sink, in good agreement with 35 +/- 14 years from a simple oceanic uptake calculation using transfer velocity and solubility. Modeled SO2F2 emissions rose from similar to 0.6 Gg/a in 1978 to similar to 1.9 Gg/a in 2007, but estimated industrial production exceeds these modeled emissions by an average of similar to 50%. This discrepancy cannot be explained with a hypothetical land sink in the model, suggesting that only similar to 2/3 of the manufactured SO(2)F(2) is actually emitted into the atmosphere and that similar to 1/3 may be destroyed during fumigation. With mean SO(2)F(2) tropospheric mixing ratios of similar to 1.4 ppt, its radiative forcing is small and it is probably an insignificant sulfur source to the stratosphere. However, with a high global warming potential similar to CFC-11, and likely increases in its future use, continued atmospheric monitoring of SO(2)F(2) is warranted.

O'Doherty, S, Cunnold DM, Miller BR, Muhle J, McCulloch A, Simmonds PG, Manning AJ, Reimann S, Vollmer MK, Greally BR, Prinn RG, Fraser PJ, Steele LP, Krummel PB, Dunse BL, Porter LW, Lunder CR, Schmidbauer N, Hermansen O, Salameh PK, Harth CM, Wang RHJ, Weiss RF.  2009.  Global and regional emissions of HFC-125 (CHF2CF3) from in situ and air archive atmospheric observations at AGAGE and SOGE observatories. Journal of Geophysical Research-Atmospheres. 114   10.1029/2009jd012184   AbstractWebsite

High-frequency, in situ observations from the Advanced Global Atmospheric Gases Experiment (AGAGE) and System for Observation of halogenated Greenhouse gases in Europe (SOGE) networks for the period 1998 to 2008, combined with archive flask measurements dating back to 1978, have been used to capture the rapid growth of HFC-125 (CHF(2)CF(3)) in the atmosphere. HFC-125 is the fifth most abundant HFC, and it currently makes the third largest contribution of the HFCs to atmospheric radiative forcing. At the beginning of 2008 the global average was 5.6 ppt in the lower troposphere and the growth rate was 16% yr(-1). The extensive observations have been combined with a range of modeling techniques to derive global emission estimates in a top-down approach. It is estimated that 21 kt were emitted globally in 2007, and the emissions are estimated to have increased 15% yr(-1) since 2000. These estimates agree within approximately 20% with values reported to the United Nations Framework Convention on Climate Change (UNFCCC) provided that estimated emissions from East Asia are included. Observations of regionally polluted air masses at individual AGAGE sites have been used to produce emission estimates for Europe (the EU-15 countries), the United States, and Australia. Comparisons between these top-down estimates and bottom-up estimates based on reports by individual countries to the UNFCCC show a range of approximately four in the differences. This process of independent verification of emissions, and an understanding of the differences, is vital for assessing the effectiveness of international treaties, such as the Kyoto Protocol.

Petrenko, VV, Smith AM, Brook EJ, Lowe D, Riedel K, Brailsford G, Hua Q, Schaefer H, Reeh N, Weiss RF, Etheridge D, Severinghaus JP.  2009.  14CH4 measurements in Greenland ice: investigating last glacial termination CH4 sources. Science. 324:506-508.   10.1126/science.1168909   AbstractWebsite

The cause of a large increase of atmospheric methane concentration during the Younger Dryas-Preboreal abrupt climatic transition (similar to 11,600 years ago) has been the subject of much debate. The carbon-14 (C-14) content of methane ((CH4)-C-14) should distinguish between wetland and clathrate contributions to this increase. We present measurements of (CH4)-C-14 in glacial ice, targeting this transition, performed by using ice samples obtained from an ablation site in west Greenland. Measured (CH4)-C-14 values were higher than predicted under any scenario. Sample (CH4)-C-14 appears to be elevated by direct cosmogenic C-14 production in ice. C-14 of CO was measured to better understand this process and correct the sample (CH4)-C-14. Corrected results suggest that wetland sources were likely responsible for the majority of the Younger Dryas-Preboreal CH4 rise.

Stohl, A, Seibert P, Arduini J, Eckhardt S, Fraser P, Greally BR, Lunder C, Maione M, Muhle J, O'Doherty S, Prinn RG, Reimann S, Saito T, Schmidbauer N, Simmonds PG, Vollmer MK, Weiss RF, Yokouchi Y.  2009.  An analytical inversion method for determining regional and global emissions of greenhouse gases: Sensitivity studies and application to halocarbons. Atmospheric Chemistry and Physics. 9:1597-1620.   10.5194/acp-9-1597-2009   AbstractWebsite

A new analytical inversion method has been developed to determine the regional and global emissions of long-lived atmospheric trace gases. It exploits in situ measurement data from three global networks and builds on backward simulations with a Lagrangian particle dispersion model. The emission information is extracted from the observed concentration increases over a baseline that is itself objectively determined by the inversion algorithm. The method was applied to two hydrofluorocarbons (HFC-134a, HFC-152a) and a hydrochlorofluorocarbon (HCFC-22) for the period January 2005 until March 2007. Detailed sensitivity studies with synthetic as well as with real measurement data were done to quantify the influence on the results of the a priori emissions and their uncertainties as well as of the observation and model errors. It was found that the global a posteriori emissions of HFC-134a, HFC-152a and HCFC-22 all increased from 2005 to 2006. Large increases (21%, 16%, 18%, respectively) from 2005 to 2006 were found for China, whereas the emission changes in North America (-9%, 23%, 17%, respectively) and Europe (11%, 11%,-4%, respectively) were mostly smaller and less systematic. For Europe, the a posteriori emissions of HFC-134a and HFC-152a were slightly higher than the a priori emissions reported to the United Nations Framework Convention on Climate Change (UNFCCC). For HCFC-22, the a posteriori emissions for Europe were substantially (by almost a factor 2) higher than the a priori emissions used, which were based on HCFC consumption data reported to the United Nations Environment Programme (UNEP). Combined with the reported strongly decreasing HCFC consumption in Europe, this suggests a substantial time lag between the reported time of the HCFC-22 consumption and the actual time of the HCFC-22 emission. Conversely, in China where HCFC consumption is increasing rapidly according to the UNEP data, the a posteriori emissions are only about 40% of the a priori emissions. This reveals a substantial storage of HCFC-22 and potential for future emissions in China. Deficiencies in the geographical distribution of stations measuring halocarbons in relation to estimating regional emissions are also discussed in the paper. Applications of the inversion algorithm to other greenhouse gases such as methane, nitrous oxide or carbon dioxide are foreseen for the future.

Patra, PK, Takigawa M, Ishijima K, Choi B-C, Cunnold D, Dlugokencky EJ, Fraser P, Gomez-Pelaez AJ, Goo T-Y, Kim J-S, Krummel P, Langenfelds R, Meinhardt F, Mukai H, O'Doherty S, Prinn RG, Simmonds P, Steele P, Tohjima Y, Tsuboi K, Uhse K, Weiss R, Worthy D, Nakazawa T.  2009.  Growth rate, seasonal, synoptic, diurnal variations and budget of methane in the lower atmosphere. Journal of the Meteorological Society of Japan. 87:635-663.: Meteorological Society of Japan, 1-3-4, Ote-machi Chiyoda-ku Tokyo 100-0004 Japan, [], [URL:]   10.2151/jmsj.87.635   AbstractWebsite

We have used an AGCM (atmospheric general circulation model)-based Chemistry Transport Model (ACTM) for the simulation of methane (CH sub(4)) in the height range of earth's surface to about 90 km. The model simulations are compared with measurements at hourly, daily, monthly and interannual time scales by filtering or averaging all the timeseries appropriately. From this model-observation comparison, we conclude that the recent (1990-2006) trends in growth rate and seasonal cycle at most measurement sites can be fairly successfully modeled by using existing knowledge of CH sub(4) flux trends and seasonality. A large part of the interannual variability (IAV) in CH sub(4) growth rate is apparently controlled by IAV in atmospheric dynamics at the tropical sites and forest fires in the high latitude sites. The flux amplitudes are optimized with respect to the available hydroxyl radical (OH) distribution and model transport for successful reproduction of latitudinal and longitudinal distribution of observed CH sub(4) mixing ratio at the earth's surface. Estimated atmospheric CH sub(4) lifetime in this setup is 8.6 years. We found a small impact (less than 0.5 integrated over 1 year) of OH diurnal variation, due to temperature dependence of reaction rate coefficient, on CH sub(4) simulation compared to the transport related variability (order of +/-15 at interannual timescales). Model-observation comparisons of seasonal cycles, synoptic variations and diurnal cycles are shown to be useful for validating regional flux distribution patterns and strengths. Our results, based on two emission scenarios, suggest reduced emissions from temperate and tropical Asia region (by 13, 5, 3 Tg-CH sub(4) for India, China and Indonesia, respectively), and compensating increase (by 9, 9, 3 Tg-CH sub(4) for Russia, United States and Canada, respectively) in the boreal Northern Hemisphere (NH) are required for improved model-observation agreement.

Rhew, RC, Miller BR, Weiss RF.  2008.  Chloroform, carbon tetrachloride and methyl chloroform fluxes in southern California ecosystems. Atmospheric Environment. 42:7135-7140.   10.1016/j.atmosenv.2008.05.038   AbstractWebsite

Chloroform (CHCl3), carbon tetrachloride (CCl4), and methyl chloroform (CH3CCl3) are important carriers of chlorine to the stratosphere and account for an estimated 159 of the total organic chlorine in the troposphere, roughly equivalent to chlorine load due to methyl chloride (CH3Cl). The tropospheric burden of chlorine has declined since 1994, largely due to the restriction of CH3CCl3 and CCl4 use as specified by the Montreal Protocol. However, few field studies have been conducted on the terrestrial-atmosphere exchange of these chlorinated hydrocarbons, leading to uncertainties about the natural cycling of these trace gases. This work shows the results of 75 flux measurements conducted in a variety of southern California ecosystems, including coast sagebrush, chamise chaparral, creosote bush scrub, shoreline, and coastal salt marsh. We find no evidence of a significant soil sink in these ecosystems but rather a small net source of CHCl3 and possibly CCl4. (c) 2008 Elsevier Ltd. All rights reserved.

Huang, J, Golombek A, Prinn R, Weiss R, Fraser P, Simmonds P, Dlugokencky EJ, Hall B, Elkins J, Steele P, Langenfelds R, Krummel P, Dutton G, Porter L.  2008.  Estimation of regional emissions of nitrous oxide from 1997 to 2005 using multinetwork measurements, a chemical transport model, and an inverse method. Journal of Geophysical Research-Atmospheres. 113   10.1029/2007jd009381   AbstractWebsite

Nitrous oxide (N2O) is an important ozone-depleting gas and greenhouse gas with multiple uncertain emission processes. Global nitrous oxide observations, the Model of Atmospheric Transport and Chemistry (MATCH) and an inverse method were used to optimally estimate N2O emissions from twelve source regions around the globe. MATCH was used with forecast center reanalysis winds at T62 resolution (192 longitude by 94 latitude surface grid, and 28 vertical levels) from 1 July 1996 to 30 June 2006. The average concentrations of N2O in the lowest four layers of the model were then compared with the monthly mean observations from four national/international networks measuring at 65 surface sites. A 12-month-running-mean smoother was applied to both the model results and the observations, due to the fact that the model was not able to reproduce the very small observed seasonal cycles. The inverse method was then used to solve for the time-averaged regional emissions of N2O for two time periods (1 January 1997 to 31 December 2001 and 1 January 2002 to 31 December 2005). The best estimate inversions assume that the model stratospheric destruction rates, which lead to a global N2O lifetime of 125 years, are correct. It also assumes normalized emission spatial distributions within each region from Bouwman et al. (1995). We conclude that global N2O emissions with 66% probability errors are 16.3(-1.2)(+1.5) and 15.4(-1.3)(+1.7) TgN (N2O) a(-1), for 1997-2001 and 2001-2005 respectively. Emissions from the equator to 30 degrees N increased significantly from the initial Bouwman et al. (1995) estimates while emissions from southern oceans (30 degrees S-90 degrees S) decreased significantly. The quoted uncertainties include both the measurement errors and modeling uncertainties estimated using a separate flexible 12-box model. We also found that 23 +/- 4% of the N2O global total emissions come from the ocean, which is slightly smaller than the Bouwman et al. (1995) estimate. For the estimation of emissions from the twelve model regions, we conclude that, relative to Bouwman et al. (1995), land emissions from South America, Africa, and China/Japan/South East Asia are larger, while land emissions from Australia/New Zealand are smaller. Our study also shows a shift of the oceanic sources from the extratropical to the tropical oceans relative to Bouwman et al. (1995). Between the periods 1997-2001 and 2002-2005, emissions increased in China/Japan/South East Asia, 0 degrees-30 degrees N oceans, and North West Asia and decreased in Australia/New Zealand, 30 degrees S-90 degrees S oceans, 30 degrees N-90 degrees N oceans, and Africa. The lower tropical ocean emissions in 1997-2001 relative to 2002-2005 could result from the effects of the 1997-1998 El Nino in the earlier period.

Weiss, RF, Muhle J, Salameh PK, Harth CM.  2008.  Nitrogen trifluoride in the global atmosphere. Geophysical Research Letters. 35   10.1029/2008gl035913   AbstractWebsite

Background atmospheric abundances and trends of nitrogen trifluoride (NF(3)), a potent anthropogenic greenhouse gas, have been measured for the first time. The mean global tropospheric concentration of NF(3) has risen quasi-exponentially from about 0.02 ppt (parts-per-trillion, dry air mole fraction) at the beginning of our measured record in 1978, to a July 1, 2008 value of 0.454 ppt, with a rate of increase of 0.053 ppt yr(-1), or about 11% per year, and an interhemispheric gradient that is consistent with these emissions occuring overwhelmingly in the Northern Hemisphere, as expected. This rise rate corresponds to about 620 metric tons of current NF(3) emissions globally per year, or about 16% of the poorly-constrained global NF(3) production estimate of 4,000 metric tons yr(-1). This is a significantly higher percentage than has been estimated by industry, and thus strengthens the case for inventorying NF(3) production and for regulating its emissions. Citation: Weiss, R. F., J. Muhle, P. K., Salameh, and C.M. Harth (2008), Nitrogen trifluoride in the global atmosphere, Geophys. Res. Lett., 35, L208121, doi: 10.1029/2008GL035913.

Rigby, M, Prinn RG, Fraser PJ, Simmonds PG, Langenfelds RL, Huang J, Cunnold DM, Steele LP, Krummel PB, Weiss RF, O'Doherty S, Salameh PK, Wang HJ, Harth CM, Muhle J, Porter LW.  2008.  Renewed growth of atmospheric methane. Geophysical Research Letters. 35   10.1029/2008gl036037   AbstractWebsite

Following almost a decade with little change in global atmospheric methane mole fraction, we present measurements from the Advanced Global Atmospheric Gases Experiment (AGAGE) and the Australian Commonwealth Scientific and Industrial Research Organisation (CSIRO) networks that show renewed growth starting near the beginning of 2007. Remarkably, a similar growth rate is found at all monitoring locations from this time until the latest measurements. We use these data, along with an inverse method applied to a simple model of atmospheric chemistry and transport, to investigate the possible drivers of the rise. Specifically, the relative roles of an increase in emission rate or a decrease in concentration of the hydroxyl radical, the largest methane sink, are examined. We conclude that: 1) if the annual mean hydroxyl radical concentration did not change, a substantial increase in emissions was required simultaneously in both hemispheres between 2006 and 2007; 2) if a small drop in the hydroxyl radical concentration occurred, consistent with AGAGE methyl chloroform measurements, the emission increase is more strongly biased to the Northern Hemisphere. Citation: Rigby, M., et al. (2008), Renewed growth of atmospheric methane, Geophys. Res. Lett., 35, L22805, doi: 10.1029/2008GL036037.

Miller, BR, Weiss RF, Salameh PK, Tanhua T, Greally BR, Muhle J, Simmonds PG.  2008.  Medusa: A sample preconcentration and GC/MS detector system for in situ measurements of atmospheric trace halocarbons, hydrocarbons, and sulfur compounds. Analytical Chemistry. 80:1536-1545.   10.1021/ac702084k   AbstractWebsite

Significant changes have occurred in the anthropogenic emissions of many compounds related to the Kyoto and Montreal Protocols within the past 20 years and many of their atmospheric abundances have responded dramatically. Additionally, there are a number of related natural compounds with underdetermined source or sink budgets. A new instrument, Medusa, was developed to make the high frequency in situ measurements required for the determination of the atmospheric lifetimes and emissions of these compounds. This automated system measures a wide range of halocarbons, hydrocarbons, and sulfur compounds involved in ozone depletion and/or climate forcing, from the very volatile perfluorocarbons (PFCs, e.g., CF(4) and CF(3)CF(3)) and hydrofluorocarbons (HFCs, e.g., CH(3)CF(3)) to the higher-boiling point solvents (such as CH(3)CCl(3) and CCl(2)= CCl(2)) and CHBr(3). A network of Medusa systems worldwide provides 12 in situ ambient air measurements per day of more than 38 compounds of part per trillion mole fractions and precisions up to 0.1% RSD at the five remote field stations operated by the Advanced Global Atmospheric Gases Experiment (AGAGE). Ihis custom system couples gas chromatography/mass spectrometry (GC/MSD) with a novel scheme for cryogen-free low-temperature preconcentration (-165 degrees C) of analytes from 2 L samples in a two-trap process using HayeSep D adsorbent.

Deeds, DA, Muhle J, Weiss RF.  2008.  Tetrafluoromethane in the deep North Pacific Ocean. Geophysical Research Letters. 35   10.1029/2008gl034355   AbstractWebsite

Dissolved tetrafluoromethane (CF(4)) has been measured for the first time in the North Pacific Ocean. Surface water collected during calm weather is near equilibrium with the modern atmosphere. Deep water, isolated from atmospheric exchange for centuries, is near equilibrium with the preindustrial atmosphere, after accounting for an expected 5% addition of this low-solubility gas due to air injection during high-latitude deep-water formation. These results strongly suggest that dissolved CF(4) is conservative in seawater and that the oceanic imprint of anthropogenic increases in atmospheric CF(4) can be used as a time-dependent tracer of ocean ventilation and subsurface circulation processes. Although the continental lithosphere is a source of natural atmospheric CF(4), we find no evidence of an oceanic lithospheric CF(4) input into deep Pacific waters. The estimated upper limit of a potential oceanic lithospheric CF(4) flux to the global atmosphere is on the order of 4% of that from the continental lithosphere.

Fine, RA, Smethie WM, Bullister JL, Rhein M, Min DH, Warner MJ, Poisson A, Weiss RF.  2008.  Decadal ventilation and mixing of Indian Ocean waters. Deep-Sea Research Part I-Oceanographic Research Papers. 55:20-37.   10.1016/j.dsr.2007.10.002   AbstractWebsite

Chlorofluorocarbon (CFC) and hydrographic data from the World Ocean Circulation Experiment (WOCE) Indian Ocean expedition are used to evaluate contributions to decadal ventilation of water masses. At a given density, CFC-derived ages increase and concentrations decrease from the south to north, with lowest concentrations and oldest ages in Bay of Bengal. Average ages for thermocline water are 0-40 years, and for intermediate water they are less than 10 years to more than 40 years. As compared with the marginal seas or throughflow, the most significant source of CFCs for the Indian Ocean south of 12 degrees N is the Southern Hemisphere. A simple calculation is used to show this is the case even at intermediate levels due to differences in gas solubilities and mixing of Antarctic Intermediate Water and Red Sea Water. Bottom water in the Australia-Antarctic Basin is higher in CFC concentrations than that to the west in the Enderby Basin, due to the shorter distance of this water to the Adelie Land coast and Ross Sea sources. However, by 40 degrees S, CFC concentrations in the bottom water of the Crozet Basin originating from the Weddell Sea are similar to those in the South Australia Basin. Independent observations, which show that bottom water undergoes elevated mixing between the Australia-Antarctic Basin and before entering the subtropics, are consistent with high CFC dilutions (3-14-fold) and a substantial concentration decrease (factor of 5) south to north of the Southeast Indian Ridge. CFC-bearing bottom waters with ages 30 years or more are transported into the subtropical South Indian Ocean by three western boundary currents, and highest concentrations are observed in the westernmost current. During WOCE, CFC-bearing bottom water reaches to about 30 degrees S in the Perth Basin, and to 20 degrees S in the Mascarene Basin. Comparing subtropical bottom water-CFC concentrations with those of the South Pacific and Atlantic oceans, at comparable latitudes, Indian Ocean bottom water-CFC concentrations are lower, consistent with its high dissipation rates from tidal mixing and current fluctuations as shown elsewhere. Thus, the generally high dilutions and low CFC concentrations in bottom water of the Indian Ocean are due to distance to the water mass source regions and the relative effectiveness of mixing. While it is not surprising that at thermocline, intermediate, and bottom levels, the significant ventilation sources on decadal time scales are all from the south, the CFCs show how local sources and mixing within the ocean affect the ventilation. (c) 2007 Elsevier Ltd. All rights reserved.

Deeds, DA, Vollmer MK, Kulongoski JT, Miller BR, Muhle J, Harth CM, Izbicki JA, Hilton DR, Weiss RF.  2008.  Evidence for crustal degassing of CF4 and SF6 in Mojave Desert groundwaters. Geochimica Et Cosmochimica Acta. 72:999-1013.   10.1016/j.gca.2007.11.027   AbstractWebsite

Dissolved tetrafluoromethane (CF(4)) and sulfur hexafluoride (SF(6)) concentrations were measured in groundwater samples from the Eastern Morongo Basin (EMB) and Mojave River Basin (MRB) located in the southern Mojave Desert, California. Both CF(4) and SF(6) are supersaturated with respect to equilibrium with the preindustrial atmosphere at the recharge temperatures and elevations of the Mojave Desert. These observations provide the first in situ evidence for a flux of CF(4) from the lithosphere. A gradual basin-wide enhancement in dissolved CF(4) and SF(6) concentrations with groundwater age is consistent with release of these gases during weathering of the surrounding granitic alluvium. Dissolved CF(4) and SF(6) concentrations in these groundwaters also contain a deeper crustal component associated with a lithospheric flux entering the EMB and MRB through the underlying basement. The crustal flux of CF(4), but not of SF(6), is enhanced in the vicinity of local active fault systems due to release of crustal fluids during episodic fracture events driven by local tectonic activity. When fluxes of CF(4) and SF(6) into Mojave Desert groundwaters are extrapolated to the global scale they are consistent, within large uncertainties, with the fluxes required to sustain the preindustrial atmospheric abundances of CF(4) and SF(6). (c) 2007 Elsevier Ltd. All rights reserved.

Papadimitriou, VC, Portmann RW, Fahey DW, Muhle J, Weiss RF, Burkholder JB.  2008.  Experimental and theoretical study of the atmospheric chemistry and global warming potential of SO2F2. Journal of Physical Chemistry A. 112:12657-12666.   10.1021/jp806368u   AbstractWebsite

In this work, potential atmospheric loss processes for SO(2)F(2), a commercially used biocide (fumigant), have been studied and its global warming potential calculated. Rate coefficients for the gas-phase reactions OH + SO(2)F(2) -> products, k(1), and Cl + SO(2)F(2) -> products, k(4), were determined using a relative rate technique to be k(1) < 1 x 10(-16) cm(3) molecule(-1) s(-1) at 296 and 333 K and k(4)(296 K) < 5 x 10(-17) cm(3) molecule(-1) s(-1). UV absorption cross sections of SO(2)F(2) were measured at 184.9, 193, and 213.9 nm, and its photolysis quantum yield at 193 urn was determined to be <0.02. The atmospheric lifetime of SO(2)F(2) with respect to loss by OH, Cl, and O((1)D) reaction and UV photodissociation is estimated to be >300, >10 000, 700, and >4700 years, respectively. The stratospheric lifetime of SO(2)F(2) is calculated using a two-dimensional model to be 630 years. The global warming potential (GWP) for SO(2)F(2) was calculated to be 4780 for the 100 year time horizon using infrared absorption cross sections measured in this work and a SO(2)F(2) globally averaged atmospheric lifetime of 36 years, which is determined primarily by ocean uptake, reported by Muhle et al. (Muhle, J.; Huang, J.; Weiss, R. F.; Prinn, R. G.; Miller, B. R.; Salameh, P. K.; Harth, C. M.; Fraser, P. J.; Porter, L. W.; Greally, B. R.; O'Doherty, S.; Simonds, P. G. J. Geophys. Res., submitted for publication, 2008). Reaction channels and the possible formation of stable adducts in reactions 1 and 4 were evaluated using ab initio, CCSD(T), and density functional theory, B3P86, quantum mechanical electronic Structure calculations. The most likely reaction product channels were found to be highly endothermic, consistent with the upper limits of the rate coefficients measured in this work.

LeBel, DA, Smethie WM, Rhein M, Kieke D, Fine RA, Bullister JL, Min DH, Roether W, Weiss RF, Andrie C, Smythe-Wright D, Jones EP.  2008.  The formation rate of North Atlantic Deep Water and Eighteen Degree Water calculated from CFC-11 inventories observed during WOCE. Deep-Sea Research Part I-Oceanographic Research Papers. 55:891-910.   10.1016/j.dsr.2008.03.009   AbstractWebsite

The accumulation of man-made chlorofluorocarbons (CFCs) in subsurface water masses is directly related to their formation rate, and the water mass formation rate can be calculated from its CFC inventory. CFC-11 inventories between 65 degrees N and 10 degrees S in the Atlantic Ocean have been calculated for Eighteen Degree Water (EDW) and the components of North Atlantic Deep Water (NADW) from data collected primarily between 1996 and 1998 as part of the World Ocean Circulation Experiment (WOCE). CFC-11 inventories for individual water masses are 5.4 million moles for EDW, 10.5 million moles for Upper Labrador Sea Water (ULSW) (4.6 million moles south of 42 degrees N), 23.4 million moles for Classical Labrador Sea Water (CLSW), 10.4 million moles for Iceland-Scotland Overflow Water (ISOW), and 8.3 million moles for Denmark Strait Overflow Water (DSOW). The estimated error for these inventories is about +/- 10%. The sum of the NADW components (ULSW, CLSW, ISOW, DSOW) is 53.2 million moles which is about half of the total CFC-11 inventory, 103.8 million moles, in the North Atlantic Ocean. Maps of water column inventories illustrate the formation mechanisms and spreading pathways within these water masses. The inventories directly reflect the input of newly formed water in the North Atlantic over the time scale of the CFC transient, about 3 decades. The interior regions of the North Atlantic contain most (75-80%) of the CFC-11 inventory in NADW indicating strong recirculation and mixing of newly formed NADW from the DWBC into the interior with a time scale of 2-3 decades. Average water mass formation rates between 1970 and 1997 are: 3.3Sv for EDW, 3.5Sv for ULSW (2.0Sv from the central Labrador Sea and 1.5 Sv from the southern Labrador Sea), 8.2 Sv for CLSW, 5.7 Sv for ISOW, and 2.2 Sv for DSOW. Estimated errors are +/- 20% for CLSW and +/- 16% for the other water masses. The total for NADW, which forms the deep limb of the North Atlantic Meridional Overturning Circulation, is 19.6 Sv. An extensive test of the effects of temporal variability on the average formation rate calculated from the CFC inventory indicates that the error introduced by the assumption of a constant water mass formation rate is no greater than 15% for CLSW and 10% for the other water masses. (c) 2008 Elsevier Ltd. All rights reserved.

Petrenko, VV, Severinghaus JP, Brook EJ, Muhle J, Headly M, Harth CM, Schaefer H, Reeh N, Weiss RF, Lowe D, Smith AM.  2008.  A novel method for obtaining very large ancient air samples from ablating glacial ice for analyses of methane radiocarbon. Journal of Glaciology. 54:233-244.   10.3189/002214308784886135   AbstractWebsite

We present techniques for obtaining large (similar to 100 L STP) samples of ancient air for analysis of (14)C of methane ((14)CH(4)) and other trace constituents. Paleoatmospheric (14)CH(4) measurements should constrain the fossil fraction of past methane budgets, as well as provide a definitive test of methane clathrate involvement in large and rapid methane concentration ([CH(4)]) increases that accompanied rapid warming events during the last deglaciation. Air dating to the Younger Dryas-Preboreal and Oldest Dryas-Bolling abrupt climatic transitions was obtained by melt extraction from old glacial ice outcropping at an ablation margin in West Greenland. The outcropping ice and occluded air were dated using a combination of delta(15)N of N(2), delta(18)O of O(2), delta(18)O(ice) and [CH(4)] measurements. The [CH(4)] blank of the melt extractions was <4 ppb. Measurements of delta(18)O and delta(15)N indicated no significant gas isotopic fractionation from handling. Measured Ar/N(2), CFC-11 and CFC-12 in the samples indicated no significant contamination from ambient air. Ar/N(2), Kr/Ar and Xe/Ar ratios in the samples were used to quantify effects of gas dissolution during the melt extractions and correct the sample [CH(4)]. Corrected [CH(4)] is elevated over expected values by up to 132 ppb for most samples, suggesting some in situ CH(4) production in ice at this site.

Nevison, CD, Mahowald NM, Weiss RF, Prinn RG.  2007.  Interannual and seasonal variability in atmospheric N2O. Global Biogeochemical Cycles. 21   10.1029/2006gb002755   AbstractWebsite

The increase in atmospheric N2O observed over the last century reflects large- scale human perturbations to the global nitrogen cycle. High- precision measurements of atmospheric N2O over the last decade reveal subtle signals of interannual variability (IAV) superimposed upon the more prominent growth trend. Anthropogenic sources drive the underlying growth in N2O, but are probably too monotonic to explain most of the observed IAV. The causes of both seasonal and interannual variability in atmospheric N2O are explored on the basis of comparisons of a 1993 - 2004 atmospheric transport simulation to observations of N2O at five stations of the Advanced Global Atmospheric Gases Experiment (AGAGE). The complementary tracers chlorofluorocarbons (CFCs) 11 and 12 and SF6 also are examined. The model simulation does not include a stratospheric sink and thus isolates the effects of surface sources and tropospheric transport. Both model and observations yield correlations in seasonal and interannual variability among species, but only in a few cases are model and observed variability correlated to each other. The results suggest that tropospheric transport contributes substantially to observed variability, especially at Samoa station. However, some features of observed variability are not explained by the model simulation and appear more consistent with a stratospheric influence. At Mace Head, Ireland, N2O and CFC growth rate anomalies are weakly correlated to IAV in polar winter lower stratospheric temperature, a proxy for the strength of the mean meridional stratospheric circulation. Seasonal and interannual variability in the natural sources of N2O may also contribute to observed variability in atmospheric N2O.

Greally, BR, Manning AJ, Reimann S, McCulloch A, Huang J, Dunse BL, Simmonds PG, Prinn RG, Fraser PJ, Cunnold DM, O'Doherty S, Porter LW, Stemmler K, Vollmer MK, Lunder CR, Schmidbauer N, Hermansen O, Arduini J, Salameh PK, Krummel PB, Wang RHJ, Folini D, Weiss RF, Maione M, Nickless G, Stordal F, Derwent RG.  2007.  Observations of 1,1-difluoroethane (HFC-152a) at AGAGE and SOGE monitoring stations in 1994-2004 and derived global and regional emission estimates. Journal of Geophysical Research-Atmospheres. 112   10.1029/2006jd007527   AbstractWebsite

[1] Ground-based in situ measurements of 1,1-difluoroethane (HFC-152a, CH3CHF2) which is regulated under the Kyoto Protocol are reported under the auspices of the AGAGE (Advanced Global Atmospheric Gases Experiment) and SOGE (System of Observation of halogenated Greenhouse gases in Europe) programs. Observations of HFC-152a at five locations (four European and one Australian) over a 10 year period were recorded. The annual average growth rate of HFC-152a in the midlatitude Northern Hemisphere has risen from 0.11 ppt/yr to 0.6 ppt/yr from 1994 to 2004. The Southern Hemisphere annual average growth rate has risen from 0.09 ppt/yr to 0.4 ppt/yr from 1998 to 2004. The 2004 average mixing ratio for HFC-152a was 5.0 ppt and 1.8 ppt in the Northern and Southern hemispheres, respectively. The annual cycle observed for this species in both hemispheres is approximately consistent with measured annual cycles at the same locations in other gases which are destroyed by OH. Yearly global emissions of HFC-152a from 1994 to 2004 are derived using the global mean HFC-152a observations and a 12-box 2-D model. The global emission of HFC-152a has risen from 7 Kt/yr to 28 Kt/yr from 1995 to 2004. On the basis of observations of above-baseline elevations in the HFC-152a record and a consumption model, regional emission estimates for Europe and Australia are calculated, indicating accelerating emissions from Europe since 2000. The overall European emission in 2004 ranges from 1.5 to 4.0 Kt/year, 5-15% of global emissions for 1,1-difluoroethane, while the Australian contribution is negligible at 5-10 tonnes/year, < 0.05% of global emissions.

Muhle, J, Lueker TJ, Su Y, Miller BR, Prather KA, Weiss RF.  2007.  Trace gas and particulate emissions from the 2003 southern California wildfires. Journal of Geophysical Research-Atmospheres. 112   10.1029/2006jd007350   AbstractWebsite

In October 2003, thirteen major wildfires in southern California burned more than 300,000 hectares of mainly chaparral biome. High-precision in situ trace gas and particle measurements of the wildfire plumes in La Jolla, California, showed a high degree of correlation among carbon dioxide (CO(2)), methane (CH(4)), nonmethane hydrocarbons, and methyl halide mixing ratios, as well as with particle number concentrations (10-300 nm and 500-2500 nm aerodynamic diameter). Aerosol time-of-flight mass spectrometry of individual aerosol particles (50-2500 nm range) showed that 70-85% had typical biomass burning signatures (levoglucosan coupled with potassium). Only 5-18% of particles in the 50 - 300 nm range had vehicle signatures. Molar trace gas enhancement ratios (ERs) versus ethane and CO(2) were calculated and showed a narrow age distribution, consistent with the short distance from the wildfires. ERs for N(2)O and CH(3)CCl(3) versus CO(2) were determined, but correlations were poor. No significant CH(2)Cl(2) or CHCl(3) emissions were detected. CO2 emissions from the nearby Cedar fire were estimated both with a simple Lagrangian atmospheric transport model and a burned area approach and extrapolated to 11 Tg CO(2) for the total burned area in southern California. Total CO(2), CH(4), C(2)-hydrocarbons, benzene, toluene, methyl chloride, methyl iodide, and PM(2.5) emissions were similar to 0.2-3.5% of yearly global extratropical forest fire emissions and more than 28% of CH(4), C(6)H(6), and PM(2.5) 2003 San Diego and South Coast Air Basins anthropogenic emissions. Particle distributions and single particle chemistry are discussed. PM(2.5) considerably exceeded the EPA short-term exposure limit.

Xiao, X, Prinn RG, Simmonds PG, Steele LP, Novelli PC, Huang J, Langenfelds RL, O'Doherty S, Krummel PB, Fraser PJ, Porter LW, Weiss RF, Salameh P, Wang RHJ.  2007.  Optimal estimation of the soil uptake rate of molecular hydrogen from the Advanced Global Atmospheric Gases Experiment and other measurements. Journal of Geophysical Research-Atmospheres. 112   10.1029/2006jd007241   AbstractWebsite

[1] Hydrogen (H(2)), a proposed clean energy alternative, warrants detailed investigation of its global budget and future environmental impacts. The magnitudes and seasonal cycles of the major ( presumably microbial) soil sink of hydrogen have been estimated from high-frequency in situ AGAGE H(2) observations and also from more geographically extensive but low-frequency flask measurements from CSIRO and NOAA-GMD using the Kalman filter in a two-dimensional (2-D) global transport model. Hydrogen mole fractions exhibit well-defined seasonal cycles in each hemisphere with their phase difference being only about 3 months. The global production rate of H(2) is estimated to be 103 +/- 10 Tg yr(-1) with only a small estimated interannual variation. Soil uptake ( 84 +/- 8 Tg yr(-1)) represents the major loss process for H(2) and accounts for 81% of the total destruction. Strong seasonal cycles are deduced for the soil uptake of H(2). The soil sink is a maximum over the northern extratropics in summer and peaks only 2 to 3 months earlier in the Northern Hemisphere than in the Southern Hemisphere. Oxidation by tropospheric OH (18 +/- 3 Tg yr(-1)) accounts for 17% of the destruction, with the remainder due to destruction in the stratosphere. The calculated global burden is 191 +/- 29 Tg, indicating an overall atmospheric lifetime of 1.8 +/- 0.3 years. Hydrogen in the troposphere ( 149 +/- 23 Tg burden) has a lifetime of 1.4 +/- 0.2 years.