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2015
Fortems-Cheiney, A, Saunois M, Pison I, Chevallier F, Bousquet P, Cressot C, Montzka SA, Fraser PJ, Vollmer MK, Simmonds PG, Young D, O'Doherty S, Weiss RF, Artuso F, Barletta B, Blake DR, Li S, Lunder C, Miller BR, Park S, Prinn R, Saito T, Steele LP, Yokouchi Y.  2015.  Increase in HFC-134a emissions in response to the success of the Montreal Protocol. Journal of Geophysical Research-Atmospheres. 120   10.1002/2015jd023741   AbstractWebsite

The 1,1,1,2-tetrafluoroethane (HFC-134a), an important alternative to CFC-12 in accordance with the Montreal Protocol on Substances that Deplete the Ozone Layer, is a high global warming potential greenhouse gas. Here we evaluate variations in global and regional HFC-134a emissions and emission trends, from 1995 to 2010, at a relatively high spatial and temporal (3.75 degrees in longitude x 2.5 degrees in latitude and 8 day) resolution, using surface HFC-134a measurements. Our results show a progressive increase of global HFC-134a emissions from 19 +/- 2 Gg/yr in 1995 to 167 +/- 5 Gg/yr in 2010, with both a slowdown in developed countries and a 20%/yr increase in China since 2005. A seasonal cycle is also seen since 2002, which becomes enhanced over time, with larger values during the boreal summer.

Wells, KC, Millet DB, Bousserez N, Henze DK, Chaliyakunnel S, Griffis TJ, Luan Y, Dlugokencky EJ, Prinn RG, O'Doherty S, Weiss RF, Dutton GS, Elkins JW, Krummel PB, Langenfelds R, Steele LP, Kort EA, Wofsy SC, Umezawa T.  2015.  Simulation of atmospheric N2O with GEOS-Chem and its adjoint: evaluation of observational constraints. Geoscientific Model Development. 8:3179-3198.   10.5194/gmd-8-3179-2015   AbstractWebsite

We describe a new 4D-Var inversion framework for nitrous oxide (N2O) based on the GEOS-Chem chemical transport model and its adjoint, and apply it in a series of observing system simulation experiments to assess how well N2O sources and sinks can be constrained by the current global observing network. The employed measurement ensemble includes approximately weekly and quasicontinuous N2O measurements (hourly averages used) from several long-term monitoring networks, N2O measurements collected from discrete air samples onboard a commercial aircraft (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container; CARIBIC), and quasi-continuous measurements from the airborne HIAPER Pole-to-Pole Observations (HIPPO) campaigns. For a 2-year inversion, we find that the surface and HIPPO observations can accurately resolve a uniform bias in emissions during the first year; CARIBIC data provide a somewhat weaker constraint. Variable emission errors are much more difficult to resolve given the long lifetime of N2O, and major parts of the world lack significant constraints on the seasonal cycle of fluxes. Current observations can largely correct a global bias in the stratospheric sink of N2O if emissions are known, but do not provide information on the temporal and spatial distribution of the sink. However, for the more realistic scenario where source and sink are both uncertain, we find that simultaneously optimizing both would require unrealistically small errors in model transport. Regardless, a bias in the magnitude of the N2O sink would not affect the a posteriori N2O emissions for the 2-year timescale used here, given realistic initial conditions, due to the timescale required for stratosphere-troposphere exchange (STE). The same does not apply to model errors in the rate of STE itself, which we show exerts a larger influence on the tropospheric burden of N2O than does the chemical loss rate over short (< 3 year) timescales. We use a stochastic estimate of the inverse Hessian for the inversion to evaluate the spatial resolution of emission constraints provided by the observations, and find that significant, spatially explicit constraints can be achieved in locations near and immediately upwind of surface measurements and the HIPPO flight tracks; however, these are mostly confined to North America, Europe, and Australia. None of the current observing networks are able to provide significant spatial information on tropical N2O emissions. There, averaging kernels (describing the sensitivity of the inversion to emissions in each grid square) are highly smeared spatially and extend even to the midlatitudes, so that tropical emissions risk being conflated with those elsewhere. For global inversions, therefore, the current lack of constraints on the tropics also places an important limit on our ability to understand extratropical emissions. Based on the error reduction statistics from the inverse Hessian, we characterize the atmospheric distribution of unconstrained N2O, and identify regions in and downwind of South America, central Africa, and Southeast Asia where new surface or profile measurements would have the most value for reducing present uncertainty in the global N2O budget.

2014
Patra, PK, Krol MC, Montzka SA, Arnold T, Atlas EL, Lintner BR, Stephens BB, Xiang B, Elkins JW, Fraser PJ, Ghosh A, Hintsa EJ, Hurst DF, Ishijima K, Krummel PB, Miller BR, Miyazaki K, Moore FL, Muhle J, O'Doherty S, Prinn RG, Steele LP, Takigawa M, Wang HJ, Weiss RF, Wofsy SC, Young D.  2014.  Observational evidence for interhemispheric hydroxyl-radical parity. Nature. 513:219-+.   10.1038/nature13721   AbstractWebsite

The hydroxyl radical (OH) is a key oxidant involved in the removal of air pollutants and greenhouse gases from the atmosphere(1-3). The ratio of Northern Hemispheric to Southern Hemispheric (NH/SH) OH concentration is important for our understanding of emission estimates of atmospheric species such as nitrogen oxides and methane(4-6). It remains poorly constrained, however, with a range of estimates from 0.85 to 1.4 (refs 4,7-10). Here we determine the NH/SH ratio of OH with the help of methyl chloroform data (a proxy for OH concentrations) and an atmospheric transport model that accurately describes interhemispheric transport and modelled emissions. We find that for the years 2004-2011 the model predicts an annual mean NH-SH gradient of methyl chloroform that is a tight linear function of the modelled NH/SH ratio in annual mean OH. We estimate a NH/SH OH ratio of 0.97 +/- 0.12 during this time period by optimizing global total emissions and mean OH abundance to fit methyl chloroform data from two surface-measurement networks and aircraft campaigns(11-13). Our findings suggest that top-down emission estimates of reactive species such as nitrogen oxides in key emitting countries in the NH that are based on a NH/SH OH ratio larger than 1 may be overestimated.

Thompson, RL, Ishijima K, Saikawa E, Corazza M, Karstens U, Patra PK, Bergamaschi P, Chevallier F, Dlugokencky E, Prinn RG, Weiss RF, O'Doherty S, Fraser PJ, Steele LP, Krummel PB, Vermeulen A, Tohjima Y, Jordan A, Haszpra L, Steinbacher M, Van der Laan S, Aalto T, Meinhardt F, Popa ME, Moncrieff J, Bousquet P.  2014.  TransCom N2O model inter-comparison - Part 2: Atmospheric inversion estimates of N2O emissions. Atmospheric Chemistry and Physics. 14:6177-6194.   10.5194/acp-14-6177-2014   AbstractWebsite

This study examines N2O emission estimates from five different atmospheric inversion frameworks based on chemistry transport models (CTMs). The five frameworks differ in the choice of CTM, meteorological data, prior uncertainties and inversion method but use the same prior emissions and observation data set. The posterior modelled atmospheric N2O mole fractions are compared to observations to assess the performance of the inversions and to help diagnose problems in the modelled transport. Additionally, the mean emissions for 2006 to 2008 are compared in terms of the spatial distribution and seasonality. Overall, there is a good agreement among the inversions for the mean global total emission, which ranges from 16.1 to 18.7 TgN yr(-1) and is consistent with previous estimates. Ocean emissions represent between 31 and 38% of the global total compared to widely varying previous estimates of 24 to 38%. Emissions from the northern mid- to high latitudes are likely to be more important, with a consistent shift in emissions from the tropics and subtropics to the mid- to high latitudes in the Northern Hemisphere; the emission ratio for 0-30A degrees N to 30-90A degrees N ranges from 1.5 to 1.9 compared with 2.9 to 3.0 in previous estimates. The largest discrepancies across inversions are seen for the regions of South and East Asia and for tropical and South America owing to the poor observational constraint for these areas and to considerable differences in the modelled transport, especially inter-hemispheric exchange rates and tropical convective mixing. Estimates of the seasonal cycle in N2O emissions are also sensitive to errors in modelled stratosphere-to-troposphere transport in the tropics and southern extratropics. Overall, the results show a convergence in the global and regional emissions compared to previous independent studies.

Thompson, RL, Chevallier F, Crotwell AM, Dutton G, Langenfelds RL, Prinn RG, Weiss RF, Tohjima Y, Nakazawa T, Krummel PB, Steele LP, Fraser P, O'Doherty S, Ishijima K, Aoki S.  2014.  Nitrous oxide emissions 1999 to 2009 from a global atmospheric inversion. Atmospheric Chemistry and Physics. 14:1801-1817.   10.5194/acp-14-1801-2014   AbstractWebsite

N2O surface fluxes were estimated for 1999 to 2009 using a time-dependent Bayesian inversion technique. Observations were drawn from 5 different networks, incorporating 59 surface sites and a number of ship-based measurement series. To avoid biases in the inverted fluxes, the data were adjusted to a common scale and scale offsets were included in the optimization problem. The fluxes were calculated at the same resolution as the transport model (3.75 degrees longitude x 2.5 degrees latitude) and at monthly time resolution. Over the 11-year period, the global total N2O source varied from 17.5 to 20.1 Tg a(-1) N. Tropical and subtropical land regions were found to consistently have the highest N2O emissions, in particular in South Asia (20 +/- 3% of global total), South America (13 +/- 4 %) and Africa (19 +/- 3 %), while emissions from temperate regions were smaller: Europe (6 +/- 1 %) and North America (7 +/- 2 %). A significant multi-annual trend in N2O emissions (0.045 Tg a(-2) N) from South Asia was found and confirms inventory estimates of this trend. Considerable interannual variability in the global N2O source was observed (0.8 Tg a(-1) N, 1 standard deviation, SD) and was largely driven by variability in tropical and subtropical soil fluxes, in particular in South America (0.3 Tg a(-1) N, 1 SD) and Africa (0.3 Tg a(-1) N, 1 SD). Notable variability was also found for N2O fluxes in the tropical and southern oceans (0.15 and 0.2 Tg a(-1) N, 1 SD, respectively). Interannual variability in the N2O source shows some correlation with the El Nino-Southern Oscillation (ENSO), where El Nino conditions are associated with lower N2O fluxes from soils and from the ocean and vice versa for La Nina conditions.

2013
Fraser, A, Palmer PI, Feng L, Boesch H, Cogan A, Parker R, Dlugokencky EJ, Fraser PJ, Krummel PB, Langenfelds RL, O'Doherty S, Prinn RG, Steele LP, van der Schoot M, Weiss RF.  2013.  Estimating regional methane surface fluxes: the relative importance of surface and GOSAT mole fraction measurements. Atmospheric Chemistry and Physics. 13:5697-5713.   10.5194/acp-13-5697-2013   AbstractWebsite

We use an ensemble Kalman filter (EnKF), together with the GEOS-Chem chemistry transport model, to estimate regional monthly methane (CH4) fluxes for the period June 2009-December 2010 using proxy dry-air column-averaged mole fractions of methane (XCH4) from GOSAT (Greenhouse gases Observing SATellite) and/or NOAA ESRL (Earth System Research Laboratory) and CSIRO GASLAB (Global Atmospheric Sampling Laboratory) CH4 surface mole fraction measurements. Global posterior estimates using GOSAT and/or surface measurements are between 510-516 Tg yr(-1), which is less than, though within the uncertainty of, the prior global flux of 529 +/- 25 Tg yr(-1). We find larger differences between regional prior and posterior fluxes, with the largest changes in monthly emissions (75 Tg yr(-1)) occurring in Temperate Eurasia. In non-boreal regions the error reductions for inversions using the GOSAT data are at least three times larger (up to 45 %) than if only surface data are assimilated, a reflection of the greater spatial coverage of GOSAT, with the two exceptions of latitudes >60 degrees associated with a data filter and over Europe where the surface network adequately describes fluxes on our model spatial and temporal grid. We use CarbonTracker and GEOS-Chem XCO2 model output to investigate model error on quantifying proxy GOSAT XCH4 (involving model XCO2) and inferring methane flux estimates from surface mole fraction data and show similar resulting fluxes, with differences reflecting initial differences in the proxy value. Using a series of observing system simulation experiments (OSSEs) we characterize the posterior flux error introduced by non-uniform atmospheric sampling by GOSAT. We show that clear-sky measurements can theoretically reproduce fluxes within 10% of true values, with the exception of tropical regions where, due to a large seasonal cycle in the number of measurements because of clouds and aerosols, fluxes are within 15% of true fluxes. We evaluate our posterior methane fluxes by incorporating them into GEOS-Chem and sampling the model at the location and time of surface CH4 measurements from the AGAGE (Advanced Global Atmospheric Gases Experiment) network and column XCH4 measurements from TCCON (Total Carbon Column Observing Network). The posterior fluxes modestly improve the model agreement with AGAGE and TCCON data relative to prior fluxes, with the correlation coefficients (r(2)) increasing by a mean of 0.04 (range: -0.17 to 0.23) and the biases decreasing by a mean of 0.4 ppb (range: -8.9 to 8.4 ppb).

Simmonds, PG, Manning AJ, Athanassiadou M, Scaife AA, Derwent RG, O'Doherty S, Harth CM, Weiss RF, Dutton GS, Hall BD, Sweeney C, Elkins JW.  2013.  Interannual fluctuations in the seasonal cycle of nitrous oxide and chlorofluorocarbons due to the Brewer-Dobson circulation. Journal of Geophysical Research-Atmospheres. 118:10694-10706.   10.1002/jgrd.50832   AbstractWebsite

The tropospheric seasonal cycles of N2O, CFC-11 (CCl3F), and CFC-12 (CCl2F2) are influenced by atmospheric dynamics. The interannually varying summertime minima in mole fractions of these trace gases have been attributed to interannual variations in mixing of stratospheric air (depleted in CFCs and N2O) with tropospheric air with a few months lag. The amount of wave activity that drives the stratospheric circulation and influences the winter stratospheric jet and subsequent mass transport across the tropopause appears to be the primary cause of this interannual variability. We relate the observed seasonal minima of species at three Northern Hemisphere sites (Mace Head, Ireland; Trinidad Head, U.S.; and Barrow, Alaska) with the behavior of the winter stratospheric jet. As a result, a good correlation is obtained between zonal winds in winter at 10 hPa, 58°N–68°N, and the detrended seasonal minima in the stratosphere-influenced tracers. For these three tracers, individual Pearson correlation coefficients (r) between 0.51 and 0.71 were found, with overall correlations of between 0.67 and 0.77 when “composite species” were considered. Finally, we note that the long-term observations of CFCs and N2O in the troposphere provide an independent monitoring method complementary to satellite data. Furthermore, they could provide a useful observational measure of the strength of stratosphere-troposphere exchange and, thus, could be used to monitor any long-term trend in the Brewer-Dobson circulation which is predicted by climate models to increase over the coming decades.

Rigby, M, Prinn RG, O'Doherty S, Montzka SA, McCulloch A, Harth CM, Muhle J, Salameh PK, Weiss RF, Young D, Simmonds PG, Hall BD, Dutton GS, Nance D, Mondeel DJ, Elkins JW, Krummel PB, Steele LP, Fraser PJ.  2013.  Re-evaluation of the lifetimes of the major CFCs and CH3CCl3 using atmospheric trends. Atmospheric Chemistry and Physics. 13:2691-2702.   10.5194/acp-13-2691-2013   AbstractWebsite

Since the Montreal Protocol on Substances that Deplete the Ozone Layer and its amendments came into effect, growth rates of the major ozone depleting substances (ODS), particularly CFC-11, -12 and -113 and CH3CCl3, have declined markedly, paving the way for global stratospheric ozone recovery. Emissions have now fallen to relatively low levels, therefore the rate at which this recovery occurs will depend largely on the atmospheric lifetime of these compounds. The first ODS measurements began in the early 1970s along with the first lifetime estimates calculated by considering their atmospheric trends. We now have global mole fraction records spanning multiple decades, prompting this lifetime re-evaluation. Using surface measurements from the Advanced Global Atmospheric Gases Experiment (AGAGE) and the National Oceanic and Atmospheric Administration Global Monitoring Division (NOAA GMD) from 1978 to 2011, we estimated the lifetime of CFC-11, CFC-12, CFC-113 and CH3CCl3 usin!

2008
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.

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.

2006
Simmonds, PG, Manning AJ, Cunnold DM, McCulloch A, O'Doherty S, Derwent RG, Krummel PB, Fraser PJ, Dunse B, Porter LW, Wang RHJ, Greally BR, Miller BR, Salameh P, Weiss RF, Prinn RG.  2006.  Global trends, seasonal cycles, and European emissions of dichloromethane, trichloroethene, and tetrachloroethene from the AGAGE observations at Mace Head, Ireland, and Cape Grim, Tasmania. Journal of Geophysical Research-Atmospheres. 111   10.1029/2006jd007082   AbstractWebsite

[1] In situ observations ( every 4 hours) of dichloromethane (CH(2)Cl(2)) from April 1995 to December 2004 and trichloroethene (C(2)HCl(3)) and tetrachloroethene (C(2)Cl(4)) from September 2000 to December 2004 are reported for the Advanced Global Atmospheric Gases Experiment (AGAGE) station at Mace Head, Ireland. At a second AGAGE station at Cape Grim, Tasmania, CH(2)Cl(2) and C(2)Cl(4) data collection commenced in 1998 and 2000, respectively. C(2)HCl(3) is below the limit of detection at Cape Grim except during pollution episodes. At Mace Head CH(2)Cl(2) shows a downward trend from 1995 to 2004 of 0.7 +/- 0.2 ppt yr(-1) ( ppt: expressed as dry mole fractions in 10(12)), although from 1998 to 2004 the decrease has been only 0.3 +/- 0.1ppt yr(-1). Conversely, there has been a small but significant growth of 0.05 +/- 0.01 ppt yr(-1) in CH(2)Cl(2) at Cape Grim. The time series for C(2)HCl(3) and C(2)Cl(4) are relatively short for accurate trend analyses; however, we observe a small but significant decline in C(2)Cl(4) (0.18 +/- 0.05 ppt yr(-1)) at Mace Head. European emissions inferred from AGAGE measurements are compared to recent estimates from industry data and show general agreement for C(2)HCl(3). Emissions estimated from observations are lower than industry emission estimates for C(2)Cl(4) and much lower in the case of CH(2)Cl(2). A study of wildfires in Tasmania, uncontaminated by urban emissions, suggests that the biomass burning source of CH(2)Cl(2) may have been previously overestimated. All three solvents have distinct annual cycles, with the phases and amplitudes reflecting their different chemical reactivity with OH as the primary sink.

2005
Reimann, S, Manning AJ, Simmonds PG, Cunnold DM, Wang RHJ, Li JL, McCulloch A, Prinn RG, Huang J, Weiss RF, Fraser PJ, O'Doherty S, Greally BR, Stemmler K, Hill M, Folini D.  2005.  Low European methyl chloroform emissions inferred from long-term atmospheric measurements. Nature. 433:506-508.   10.1038/nature03220   AbstractWebsite

Methyl chloroform (CH3CCl3, 1,1,1,-trichloroethane) was used widely as a solvent before it was recognized to be an ozone-depleting substance and its phase-out was introduced under the Montreal Protocol(1). Subsequently, its atmospheric concentration has declined steadily(2-4) and recent European methyl chloroform consumption and emissions were estimated to be less than 0.1 gigagrams per year(1,5). However, data from a short-term tropospheric measurement campaign ( EXPORT) indicated that European methyl chloroform emissions could have been over 20 gigagrams in 2000 (ref. 6), almost doubling previously estimated global emissions(1,4). Such enhanced emissions would significantly affect results from the CH3CCl3 method of deriving global abundances of hydroxyl radicals ( OH) (refs 7 - 12) - the dominant reactive atmospheric chemical for removing trace gases related to air pollution, ozone depletion and the greenhouse effect. Here we use long-term, high-frequency data from MaceHead, Ireland and Jungfraujoch, Switzerland, to infer European methyl chloroform emissions. We find that European emission estimates declined from about 60 gigagrams per year in the mid-1990s to 0.3 - 1.4 and 1.9 - 3.4 gigagrams per year in 2000 - 03, based on Mace Head and Jungfraujoch data, respectively. Our European methyl chloroform emission estimates are therefore higher than calculated from consumption data(1,5), but are considerably lower than those derived from the EXPORT campaign in 2000 ( ref. 6).

2002
Rhein, M, Fischer J, Smethie WM, Smythe-Wright D, Weiss RF, Mertens C, Min DH, Fleischmann U, Putzka A.  2002.  Labrador Sea Water: pathways, CFC inventory, and formation rates. Journal of Physical Oceanography. 32:648-665.   10.1175/1520-0485(2002)032<0648:lswpci>2.0.co;2   AbstractWebsite

In 1997, a unique hydrographic and chlorofluorocarbon (CFC: component CFC-11) dataset was obtained in the subpolar North Atlantic. To estimate the synopticity of the 1997 data, the recent temporal evolution of the CFC and Labrador Sea Water (LSW) thickness fields are examined. In the western Atlantic north of 50degreesN, the LSW thickness decreased considerably from 1994-97, while the mean CFC concentrations did not change much. South of 50degreesN and in the eastern Atlantic, the CFC concentration increased with little or no change in the LSW thickness. On shorter timescales, local anomalies due to the presence of eddies are observed, but for space scales larger than the eddies the dataset can be treated as being synoptic over the 1997 observation period. The spreading of LSW in the subpolar North Atlantic is described in detail using gridded CFC and LSW thickness fields combined with Profiling Autonomous Lagrangian Circulation Explorer (PALACE) float trajectories. The gridded fields are also used to calculate the CFC-11 inventory in the LSW from 40degrees to 65degreesN, and from 10degrees to 60degreesW. In total, 2300 +/- 250 tons of CFC-11 (equivalent to 16.6 million moles) were brought into the LSW by deep convection. In 1997, 28% of the inventory was still found in the Labrador Sea west of 45degreesW and 31% of the inventory was located in the eastern Atlantic. The CFC inventory in the LSW was used to estimate the lower limits of LSW formation rates. At a constant formation rate, a value of 4.4-5.6 Sv (Sv = 10(6) m(3) s(-1)) is obtained. If the denser modes of LSW are ventilated only in periods with intense convection, the minimum formation rate of LSW in 1988-94 is 8.1-10.8 Sv, and 1.8-2.4 Sv in 1995-97.

1996
Landrum, LL, Gammon RH, Feely RA, Murphy PP, Kelly KC, Cosca CE, Weiss RF.  1996.  North Pacific Ocean CO2 disequilibrium for spring through summer, 1985-1989. Journal of Geophysical Research-Oceans. 101:28539-28555.   10.1029/96jc02100   AbstractWebsite

Extensive measurements of CO2 fugacity in the North Pacific surface ocean and overlying atmosphere during the years 1985-1989 are synthesized and interpreted to yield a basin-wide estimate of Delta fCO(2). The observations, taken from February through early September, suggest that the subtropical and subarctic North Pacific is a small sink for atmospheric CO2 (0.07 to 0.2 Gton C (half year)(-1) for the region north of 15 degrees N). Objective analysis techniques are used to estimate uncertainty fields resulting from constructing basin-wide contours of oceanic fCO(2) on the basis of individual cruise transects. The uncertainties are significant and imply that future sampling programs need to recognize that estimating oceanic uptake of anthropogenic CO2 from ship-transect observations of oceanic fCO(2) alone will require very extensive sampling.