4
GEOPHYSICAL RESEARCH LETTERS, VOL. 23, NO. 15, PAGES 195i'-1960, JULY 15,1996 Examining a coupled climate model using CFC-ll as an ocean! tracer Keith W. Dixon,! John L. Bullister,2 Richard H. Gammon,3 and Ronald J. StDuffi~rl Abstract. Anthropogenic CFC-II dissolved in seawater is used to analyze ocean ventilation simulated in a global coupled air-sea model. Modeled CFC-II distributions are compared to observations gathered on three Southern Hemisphere research cruises. The total amount of CFC-11 absorbed by the model's Southern Ocean is realistic, though some notable differences in the vertical structure exist. Observed and simulated CFC-II distributions are qualitatively consistent with the coupled model's predictions that the ocean may delay greenhouse gas-induced warming of surface air temperatures at high southern latitudes. The sensitivity of model-predicted CFC-II levels in the deep Southern Ocean to the choice of gas exchange parameterization suggeststhat quantitative assessments of model performance based upon simulated CFC-II distributions can be limited by air-sea gas flux uncertainties in areas of rapid ocean ventilation. Such sensitivities can complicate the quantitative aspects of CFC-II comparisons between models and observations, and between different models. Introduction In this letter, we examine the ocean component of a global coupled air-sea model developed at NOAA's Geophysical Fluid Dynamics Laboratory (GFDL). The model's control state and its transient responses to gradual changes of atmospheric CO2 have been reported previously [e.g., Manabe et al., 1991; Mallabe and Stouffer, 1994]. Of particular interest is the interhemispheric asym- metry in the response of modeled surface air temperatures to increasing CO2, with exceptionally slow warming simulated south of -4SoS. This asymmetry is attributed primarily to the Southern Ocean's large effective thermal inertia, an effect which is the product of the Southern Hemisphere's large ocean surface area, and deep and rapid mixing in the model's Southern Ocean. Here we inspect the ocean component of the GFDL coupled model's co/1trol simulation (constant C°2> using anthropogenic trichlorofluoromethane (CCI3F or CFC-1 I) as a tracer of ocean ventilation. By comparing modeled CFC-II transient tracer distri- butions to observations, we seek to assess whether the simulated oceanic ventilation largely responsible for the uptake of excess greenhouse heat in the model's Southern Hemisphere is plausible. Additionally, by using different gas exchange parameterization schemes, we examine the sensitivity of modeled tracer distribu- tions to the manner in which CFC- I I air-sea fluxes are specified. Accurate techniques to measure oceanic chlorofluorocarbons (CFCs) were developed in the early 1980s [Gammon et al., 1982]. Since then, oceanographers have gathered and analyzed a substan- tial quantity ofCFC data (for an overview seeBullister [I 989]). The I NOAA, Geophysical Fluid Dynamics Laboratory, Princeton. NJ. 2 NOAA. Pacific Marine Environmental Laboratory, Seattle,WA. 3 Chemistry Depanment and School of Oceanography, University of Washington. Seattle. WA. Copyright1996 by the American Geophysical Union. Paper number 96GLO1470 0O94-8534/96/96GL-OI470$O5.00 19 feasibility of using CFCs a!. ,malysis aids in global ocean general circulation models (GCJVfs) has been demonstrated recently [e.g., England et al. , 1994; Roj}itailleandWeaver, 1995;England,1995]. Model Description and! Experimental Design Details of the GFDIJ coupled model's construction are found in Manabe et al. [1991]; hence,. only a brief summary of the model configuration is given below, followed by a description of how CFC-11 is incorporate,d intci the ocean model component. The GFDL coupled climate model incorporates three-dimen- sional GCMs of the global oc(~an and atmosphere with simpler land hydrology and seaice m'~els, Seasonally varying insolation drives the coupled model, witt! air-sea heat and freshwater flux adjust- ments included to redLl(:e climate drift. The atmospheric spectral model uses rhomboidal 15 truncation and has 9 vertical levels. Atmospheric CO2 leve:l!; art~ prescribed to be time invariant in this configuration. The sea u:e model predicts sea ice thickness, but not fractional coverage. Tt!t: glotlal ocean model has -4.50 latitude by 3.750 longitude grid !.pacing;, 12 vertical levels and a maximum depth of 5000m. The rol:ateld diffusion tensor method described by Cox [1987] is used to parameterize the mixing of heat, salinity and passive tracers by unr(~solvc:d ocean motions. Using the following relationship, a CFC-11 air-sea flux (F) is calculated at each oce:arl sulrf;lcegrid cell every model timestep. F = a K(S,;,1\1:i [C~(Co,T,S)-C".J (I) CFC-11 air-sea flu~:es ar,e ,directly proportional to the difference between model-predi,cted levels of CFC-II dissolved in surface water (C".) and local ~;eawat(~r saturation equilibrium values (C~). C~ values are the product clf atmospheric CFC-II levels (Co) and CFC-II seawater solubilitil~S [Warner and Weiss. 1985] at model- predicted sea surface temperatures (T) and salinities (S). C,v approaches C~at a ratt: set by the local gas transfer (piston) velocity (K). Values of K are c:alculal:ed as a function of the atmospheric model's daily mean surface wind speed(I VI) and water temperature dependent Schmidt nllJmbers, (Sc(T). The influence of sea ice on CFC-11 air-sea fluxes u; represented by a in equation (1). Because this stud~I" prirlcipal goal is to examine ventilation pathways associated withl the ocean model's uptake of excess greenhouse heat, we st:ek tCI simulate CFC-II air-sea fluxes in a manner consistent with the coupled model's computation of air-sea sensible heat and evaporative fluxes via bulk formulae. Thus, CFC-ll air-sea fluxes are cl:>rnputed using model-predicted J: S, I VI and sea ice fields rat!1t:r than values derived from observational climatologies. This (:onsistency is maximized by setting a in a binary manner (i.e., 0=1 ati,:e-free grid cells and a=O at grid cells where model-predicted sea ic:e thicknesses are greater than zero). Time varying Co value!i are prescribed (the atmospheric GCM does not carry CFC-ll alsa prognostic tracer). Tropospheric CFC-ll levels have incre;ased rapidly since production began in the 1930s. Direct mea:;ure:ments of Co were not made before the late 1970s; however, earlic:r tropospheric CFC-ll levels can been deduced from produ(:tion/release data and CFC-ll 's atmospheric lifetime. Warner and We.'s;, [1992) discuss the relatively small magnitude of errors a,s~;ociated with such reconstructions. 157

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  • GEOPHYSICAL RESEARCH LETTERS, VOL. 23, NO. 15, PAGES 195i'-1960, JULY 15, 1996

    Examining a coupled climate model using CFC-ll as an ocean! tracer

    Keith W. Dixon,! John L. Bullister,2 Richard H. Gammon,3 and Ronald J. StDuffi~rl

    Abstract. Anthropogenic CFC-II dissolved in seawater is used toanalyze ocean ventilation simulated in a global coupled air-seamodel. Modeled CFC-II distributions are compared toobservations gathered on three Southern Hemisphere researchcruises. The total amount of CFC-11 absorbed by the model'sSouthern Ocean is realistic, though some notable differences in thevertical structure exist. Observed and simulated CFC-IIdistributions are qualitatively consistent with the coupled model'spredictions that the ocean may delay greenhouse gas-inducedwarming of surface air temperatures at high southern latitudes. Thesensitivity of model-predicted CFC-II levels in the deep SouthernOcean to the choice of gas exchange parameterization suggests thatquantitative assessments of model performance based uponsimulated CFC-II distributions can be limited by air-sea gas fluxuncertainties in areas of rapid ocean ventilation. Such sensitivitiescan complicate the quantitative aspects of CFC-II comparisonsbetween models and observations, and between different models.

    IntroductionIn this letter, we examine the ocean component of a global

    coupled air-sea model developed at NOAA's Geophysical FluidDynamics Laboratory (GFDL). The model's control state and itstransient responses to gradual changes of atmospheric CO2 havebeen reported previously [e.g., Manabe et al., 1991; Mallabe andStouffer, 1994]. Of particular interest is the interhemispheric asym-metry in the response of modeled surface air temperatures toincreasing CO2, with exceptionally slow warming simulated southof -4SoS. This asymmetry is attributed primarily to the SouthernOcean's large effective thermal inertia, an effect which is theproduct of the Southern Hemisphere's large ocean surface area,and deep and rapid mixing in the model's Southern Ocean.

    Here we inspect the ocean component of the GFDL coupledmodel's co/1trol simulation (constant C°2> using anthropogenictrichlorofluoromethane (CCI3F or CFC-1 I) as a tracer of oceanventilation. By comparing modeled CFC-II transient tracer distri-butions to observations, we seek to assess whether the simulatedoceanic ventilation largely responsible for the uptake of excessgreenhouse heat in the model's Southern Hemisphere is plausible.

    Additionally, by using different gas exchange parameterizationschemes, we examine the sensitivity of modeled tracer distribu-tions to the manner in which CFC- I I air-sea fluxes are specified.

    Accurate techniques to measure oceanic chlorofluorocarbons(CFCs) were developed in the early 1980s [Gammon et al., 1982].Since then, oceanographers have gathered and analyzed a substan-tial quantity ofCFC data (for an overview see Bullister [I 989]). The

    I NOAA, Geophysical Fluid Dynamics Laboratory, Princeton. NJ.2 NOAA. Pacific Marine Environmental Laboratory, Seattle, WA.3 Chemistry Depanment and School of Oceanography, University of

    Washington. Seattle. WA.

    Copyright 1996 by the American Geophysical Union.

    Paper number 96GLO1470

    0O94-8534/96/96GL-OI470$O5.00

    19

    feasibility of using CFCs a!. ,malysis aids in global ocean generalcirculation models (GCJVfs) has been demonstrated recently [e.g.,England et al. , 1994; Roj}itailleandWeaver, 1995;England,1995].

    Model Description and! Experimental Design

    Details of the GFDIJ coupled model's construction are found inManabe et al. [1991]; hence,. only a brief summary of the modelconfiguration is given below, followed by a description of howCFC-11 is incorporate,d intci the ocean model component.

    The GFDL coupled climate model incorporates three-dimen-sional GCMs of the global oc(~an and atmosphere with simpler landhydrology and sea ice m'~els, Seasonally varying insolation drivesthe coupled model, witt! air-sea heat and freshwater flux adjust-ments included to redLl(:e climate drift. The atmospheric spectralmodel uses rhomboidal 15 truncation and has 9 vertical levels.Atmospheric CO2 leve:l!; art~ prescribed to be time invariant in thisconfiguration. The sea u:e model predicts sea ice thickness, but notfractional coverage. Tt!t: glotlal ocean model has -4.50 latitude by3.750 longitude grid !.pacing;, 12 vertical levels and a maximumdepth of 5000m. The rol:ateld diffusion tensor method described byCox [1987] is used to parameterize the mixing of heat, salinity andpassive tracers by unr(~solvc:d ocean motions.

    Using the following relationship, a CFC-11 air-sea flux (F) iscalculated at each oce:arl sulrf;lce grid cell every model timestep.

    F = a K(S,;,1\1:i [C~(Co,T,S)-C".J (I)

    CFC-11 air-sea flu~:es ar,e ,directly proportional to the differencebetween model-predi,cted levels of CFC-II dissolved in surfacewater (C".) and local ~;eawat(~r saturation equilibrium values (C~).C~ values are the product clf atmospheric CFC-II levels (Co) andCFC-II seawater solubilitil~S [Warner and Weiss. 1985] at model-predicted sea surface temperatures (T) and salinities (S). C,vapproaches C~ at a ratt: set by the local gas transfer (piston) velocity(K). Values of K are c:alculal:ed as a function of the atmosphericmodel's daily mean surface wind speed (I VI) and water temperaturedependent Schmidt nllJmbers, (Sc(T). The influence of sea ice onCFC-11 air-sea fluxes u; represented by a in equation (1).

    Because this stud~I" prirlcipal goal is to examine ventilationpathways associated withl the ocean model's uptake of excessgreenhouse heat, we st:ek tCI simulate CFC-II air-sea fluxes in amanner consistent with the coupled model's computation of air-seasensible heat and evaporative fluxes via bulk formulae. Thus,CFC-ll air-sea fluxes are cl:>rnputed using model-predicted J: S, I VIand sea ice fields rat!1t:r than values derived from observationalclimatologies. This (:onsistency is maximized by setting a in abinary manner (i.e., 0=1 at i,:e-free grid cells and a=O at grid cellswhere model-predicted sea ic:e thicknesses are greater than zero).

    Time varying Co value!i are prescribed (the atmospheric GCMdoes not carry CFC-ll als a prognostic tracer). TroposphericCFC-ll levels have incre;ased rapidly since production began inthe 1930s. Direct mea:;ure:ments of Co were not made before thelate 1970s; however, earlic:r tropospheric CFC-ll levels can beendeduced from produ(:tion/release data and CFC-ll 's atmosphericlifetime. Warner and We.'s;, [1992) discuss the relatively smallmagnitude of errors a,s~;ociated with such reconstructions.

    157

  • ~~

    '" .'UbtlfiOCl time-Kale (~ where A: is lhe ocean's,...,..) f« CfCI iA d.e ocan's mi~ layer lO adjust.lO

    ..11'.1-"; a,..dI " ~I)' ~ thin one ~. But. uncertain-~~ ~. ~ '"ana: Ai I runc11on or envlronmenlal

    , ~ ~ ..trr. ...atJ-ity lO unccnainties in ~ is examined-, ~ ac.aa ~~kw ~mulalcd usin,lwo difTercnt

    ::-."-~ ~; namcly the rcillionships of Uss and

    ~~ (ItI6l8nd ~1 I \1 and So: 10 t:stimate J( arc likely to be flawed.

    ".c inltlaJlle our expcrimenls from year 1000 of the Stouffer et.sJ. [1994 J ~tand3rd run. The entry and redistribution of CFC-II inIhc OCt::ln :Ire simul:llcd for the period 1930 to 1994. In other,,'ords. for CFC-II purposes. model year 1000 is considered to be1930. The GFDL coupled model does not attempt to replicate thehistorical climate variability of specific months or years. Ralher,the model internally generalesils own variability as its externalforcings (top of the atmosphere insolation and the surface fluxadjustments) exactly repeat the same seasonal cycles each year.

    Results and DiscussionMuch more CFC-II uptake occurs in the ocean model's

    Southern Hemisphere than in the Northern Hemisphere (Figure I).Much of this interhemispheric asymmetry in the zonally integratedCFC-II air-sea fluxes arises from the distribution of land and sea;the area over which large CFC-II surface fluxes are simulated inthe Southern Ocean is greater than that found in the NorthernHemisphere's higher latitudes. The interhemispheric asymmetrypattern evident in the simulated CFC-II uptake is qualitativelysimilar to that seen in the GFDL coupled model's oceanic uptake ofgreenhouse heat [Manabe et ai., 1991].

    Coupled model results computed using the gas exchangerelationships of LM86 and W92 also appear in Figure I, and revealthat CFC-II air-sea fluxes are most sensitive to J( variations in highlatitude regions marked by deep mixing and large CFC-II air-seafluxes. The LM86 relationships yield a globally averaged J( value

    1.0

    0.8

    0~ 0.6II:

    0.4

    0.2

    0.0905 305 EO 30N 6ON 90N

    LATITUDE

    Figure 1. Solid Line: Zonally averaged CFC-II air-sea flux ratios(F simulated using LM86 divided by F simulated using W92).Dashed line: Zonally averaged CFC-II gas exchange velocity ratios(LM861C divided by W921C). Gray-filled area: Normalized, zonallyintegrated CFC-II surface input from the W92 simulation (theproduct of F and the distance along a latitude circle covered byocean). Surface inputs are normalized so the largest equals 1.0. Dataare averaged over the 10-year model period 1981 through 1990.

    ~r~

    700S 60.S !50.S 400S 30.S 200S 100S 0°LATITUDE

    ,.. C'CCCC::=m"'M~N."'T""""'C"-=-~0 0 0 " ." 0 0 -'" '"b b b :. j" :.. c. '" '" :..-'" '"'"

    Figure 2. (a) CFC-ll concentrations (pmol kg-I) measured alongthe Ajax prime meridian cruise track in Oct. 1983 and Jan. 1984[Weiss et al. , 1990]. (b) CFC-lllevels along the Ajax track as simu-lated by the coupled moclel using the W92 gas exchange equation.

    that is 57% of that prodllced by the W92 equation. The differencein the global mean net air-sea CFC-ll flux produced by the twoformulations is smaller (I he LJ\lf86 global mean F is 88% that of theW92 value); however, much more variability exists in the zonallyaveraged F ratios than in the" ratios. The F ratios are closer tounity than are the" ratios be

  • DIXON ET AL.: EXAMINING A COUPLED CLIMATE MODEL USING CFC:- lIAS A TRACER1959

    venically integrated CI~C-II column inventories (Figure 5). Thatthe total amount of CFI:-ll residing in the model's southern lati-tudes resembles the obselrvations indicates that the simulatedventilation's cumulativc:, la.r!:e-scale effect is reasonable, althoughpanly the result of compensating errors. For example, lower thanobserved CFC-ll levels in the upper portion of the model'sSouthern Ocean (-300m 1,0 -100m depth) largely compensateexcessive CFC-ll levels pre,dicted at greater depths.

    Our findings differ from those of two recent uncoupled oceanGCM studies (Robitaille a/ui Weaver [1995] and Engla11d [1995],hereafter RW95 an9 E~95) wllich independently investigated simu-lations of Southern O.:ean "'(:ntilation using CFC-ll as a tracer. Inboth the RW95 and E95 stu(:li,~s, simulated CFC-ll uptake along thesouthern ponion of the Aj~lx cruise track was overestimated whenCox's isopycnal mix.ing parameterization was used. Here, theGFDL coupled modl~l's Cf;C-ll levels along the Ajax section(Figure 2b) are markedl:v lei;s than those simulated by the E95 oceanGCM that used the Cox i!,opycnal mixing scheme. When usingCox's scheme, CFC-l 1. concentrations along RW95's simulatedAjax section lie betwe:ert the E95 and our coupled model results.

    Absent a detailed model intercomparison, the source of model-to-model differences in CFC-ll distributions can not be identifiedwith cenainty. Howe'l'eir, we offer two broad categories of possiblecauses as likely candidates. "rhe first being differences in modeledocean circulation and wat(:r mass formation rates and the secondbeing differences in the paJ:ameterized CFC-ll air-sea fluxes.

    (b)

    E'-':I:I-0.W£:)

    60.5 50.5 40.5 30.5 20.5 10.5LATITUDE

    00

    Figure 3. (a) CFC-II concentrations (pmol kg-I) measured alongthe CO2-89 cruise track (-I 05OW-II OOW) during February andMarch 1989 [Wisegarver et ai., 1993]. (b) CFC-Illevels along theCO2-89 cruise track as simulated by the coupled model using W92.

    mediate Water (AAIW) extends downward and northward from thesurface to intermediate depths. Equatorward of -300S, tracerpenetration is shallow. The observed pattern of deep CFC-llpenetration in the Southern Ocean is broadly consistent with thecoupled model results, and supports the thesis that extensiveSouthern Hemispheric ocean ventilation could delay greenhousegas induced warming of surface air temperatures in that region.

    The CFC-II comparisons expose some model deficiencies,such as insufficient AAIW formation and the lack of midwaterCFC-II minima at high southern latitudes (the latter partly arisesfrom excessive diapycnal mixing in areas of steeply sloping isopy-cnals). Yet, good agreement exists between observed and modeled

    (0)

    70s I;oS !;QS 4OS 3OS 2OS 1OS

    (b)

    i~

    i (c)(b)

    .':~~~'-"~" -....

    4000 r---,-- .'3500 CGC-90

    3000 r-170oW longitude)

    2500

    -2000~:;: '500~u ':1

    0 ---~---65S 55S 455 355 255 155 55 5N

    LATITUDE

    Figure S. CFC-ll cc'!umn inventories (nanomol m-2) along threecruise tracks (a) Ajax ,:ruis(:, (b) CO2-89 cruise, (c) CGC-90 cruise.Filled circle: columlll inve:ntories calculated from observations.Dashed Line: model-predi

  • 1960 DIXON ET AL.: EXAMINING A COUPLED CLIMATE MODEL USING CFC..)) AS A TRACER

    Ocean circulation and ventilation patterns may vary signifi-cantly among the models due to differences in surface forcings(buoyancy and momentum) and subgrid-scale mixing coefficients.For example, winds over the coupled model's Southern Ocean areweaker than the observed winds used as boundary conditions in theE95 and RW95 studies. Weaker winds can lead to less meridionaloverturning (a weaker Deacon Cell) and reduced vertical transportsof CFC-II. This is consistent with the RW95 finding that CFC-IIuptake is reduced when using a subgrid-scale mixing scheme thatlargely negates tracer advection associated with the Deacon Cell.

    The coupled model's weak Southern Ocean winds yield lower J(values than those used in the E95 and RW95 studies, thus contrib-uting to reduced CFC-II uptake. Also, deep ocean CFC-IIconcentrations may be sensitive to the treatment of how sea iceaffects F, the air-sea gas exchange. In the RW95 and E95 studies,CFC-II surface fluxes were reduced according to the observedfractional sea ice coverage data, which would allow larger CFC-llinputs than the binary method of setting (X used in this study.

    Acknowledgments: Drs. G. l"hiele and C. J. Beegle-Krause helpedassemble the CFC-I I boul\dary conditions. Discussions and correspon-dence with Drs. K. Bryal\. M. E:ngland, J. Mahlman. S. Manabe. D.Robitaille. J.R. Toggweiler. A. '~'eaver and anonymous reviewers werequite valuable and greatly appreciated. JISAO contribution number 363.

    Conclusions and Plans for Future WorkThe integrated oceanic uptake of CFC-ll in the GFDL coupled

    model's Southern Hemisphere is in general agreement with obser-vations. To the extent that CFC-ll uptake may be considered anal-ogous to the transient uptake of excess greenhouse heat, thissupports the interhemispheric asymmetry in greenhouse warmingresult of Manabe el al. [1991]. Observational evidence of deepCFC-ll penetration in the Southern Ocean also leads us to inferthat an interhemispheric asymmetry in greenhouse gas inducedwarming of surface temperatures is quite plausible in the realclimate system, and that it is not merely a model artifact.

    There is insufficient evidence to suggest that the specific mecha-nisms responsible for the GFDL coupled model's uptake oftransient greenhouse heat have been verified. Rather, comparisonsof the coupled model's CFC-II distributions to observations, andto previous uncoupled model studies, suggest that the GFDLcoupled model's ocean may be taking up about the right amount ofCFC-II for some wrong reasons. We speculate that the coupledmodel's weak winds and restrictive sea ice treatment counter atendency for Cox's isopycnal mixing scheme to overventilate. Toinvestigate this, a suite of coupled model runs using various combi-nations of model-predicted and observed variables to computeCFC-ll air-sea fluxes is planned (although such gas fluxes areinconsistent with the model's surface heat flux computations).

    The demonstrated sensitivity of high latitude CFC surface fluxesto variations in gas transfer velocities raises the question of to whatdegree present models can simulate these air-sea gas fluxes inregions of rapid ocean ventilation with sufficient accuracy to allowdetailed quallliialive assessments of model performance based oncomparisons of observed and simulated CFC distributions. For thisreason, and since the CFC-ll and excess greenhouse heat transientsare not completely analogous, the CFC-ll analyses do not allow usat present to draw definite conclusions concerning the magnitude ofthe greenhouse warming interhemispheric asymmetry.

    ReferencesBullister. J.L.. Chlorofluon>carbons as time-dependent tracers in the ocean.

    Oceanography, 2.12-1.7.1989.Cox. M.D. Isopycnal diffu!;ion in a z-coordinate ocean model. Ocean Mod-

    elling, 74.1-5.1987.England. M.H.. V. Gar~on. 3J1d J,,-I;: Minster. Chlorofluorocarbon uptake in

    a world ocean model. I. Seru;itivity to the surface gas forcing. J. Geo-phys. Res.. 99. 25215-25:~33. 1'~94.

    England. M.H.. Using chlor(Jfluorocarbons to assess ocean climate models.Geophys. Res. Let., 22, 3051.3054. 1995.

    Gammon. R.H.. J. Cline. and D. \llisegarver. Chlorolluoromethanes in theNortheast Pacific Ocean: Mea!;ured vertical distributions and applica-tion as transient tracer:; of upper ocean mixing. J. Geophys. Res., 87.9441-9454. 1982.

    Liss. P.S. and L. Merlivat. .I\i:r-sea ~:as exchange rates: Introduction and syn-thesis. in The Role of Air-Sea Ercllange in Geochemical Cycling. editedby P. Buat-Menard. pp. 113-12'7, D. Reidel. Norwell. Mass.. 1986.

    Manabe. S.. R.J. Stouffer. M.J. SIJelman. and K. Bryan. Transient responsesof a coupled ocean-atmosj;>here model to gradual changes of atmosphericCO2' Pan I: Annual meall resjp