GEOPHYSICAL RESEARCH LETTERS, VOL. 25, NO. 9, PAGES 1321-1324,MAY 1, 1998 Temporal variation in the interhemispheric offset F.G. McCormac 1,A.G. Hogg:,T.F.G.Higham:,J. Lynch-Stieglitz •, W.S.Broexker •, M.G.L. Baillie1,J.Palmer •, L. Xiong•, J.R.Pilcher 1,D. Brown• and$.T. Hoper• Abstract. Contemporaneoustree-ring dated wood, from trees carbon dates of wood of the same age are older by about 40 in thenorthern andsouthern hemispheres, givesdifferent14C yrs)[Lermanet a1.,1970]. This is becausethe larger expanseof dates.Previousstudies[Vogel et al., 1986; 1993] using wood ocean andslightly higherwindspeeds cause more14Cdepleted from SouthAfrica and The Netherlandshave shown depletion's of-4.56 + 0.85%0 and -5.12 + 0.62%0respectively. This translates to age differencesof 36 + 7 and 41 _+5 years(yrs) with the southern hemisphere giving the older dates. More recently, Stuiver and Braziunas [1998] have shown that an offset of 23 + 4 yrs exists between combined 19th century wood measurements from Tasmania and Chile in the southern hemisphere and the west coast of the U.S. (Washington) in the northern hemisphere. In this studymeasurementson contemporaneous decadalsamplesof oak from the British Isles and cedarfrom New Zealandover the period 1725 to 1885 AD show a depletion of-3.4 +_0.589'00(27.2 + 4.7 yrs). However, data after 1895 AD has a mean offset of 0.66 + 1.06%o (-5.3 + 8.5 yrs) with increasedvariance comparedto 19th century data. This, we believe, is attributable to anthropogenicfossil fuel, which, due to its long residencetime in the earth, has long since lost CO: from the oceanto enter the southern atmospherethan the northern [Cain and Suess, 1976]. This natural offset was thought to be constant through time, however, here we show that, small changeswith time do occur and the burning of fossil fuels in the industrial northernhemispherehas resulted in a slow changein the natural isotopic balance of the atmosphere between the hemispheres. Measurements In this studywe have usedoak (Quercuspetraea)from Sherwood Forest,England(53ø 12'N 01ø 04'W altitude80m) (1725 - 1745 AD)and Shane'sCastle, Co. Antrim, N. Ireland (54ø 44'N 06ø 16%V altitude 20m) (1755 - 1935 AD) and cedar (Libocedrusbidwillii) from Hihitahi State Forest Sanctuaryin the North Island of New Zealand (39ø 32'S 175ø 44'E altitude any 14Ccomponent andwhenburnedpreferentially depletes 976m). Two trees,one cedarone oak, were tree-ring datedand blocksof 125g were separated.Sampleswere pre-treatedto thenorthern hemisphere atmosphere of 14C. cellulose [Hoper et al., 1997] thereby removing all mobile fractionsandthe 14Cactivitieswere determined by liquid scintillation counting of benzene[McCormac, 1992; McCor- Introduction The growth rings of trees provide an annually datedrecord of atmosphericconditions at the location of growth. However, contemporaneous wood from different locations within a macet al., 1993]. Smalldifferences in the 14Cactivitiesof wood from different locationsare extremely difficult to detect. If woodfrom different regions is measuredin different laboratories then small systematicdifferencesbetweenlaboratories givenhemisphere doesnot alwaysgiveidenticalA14Cmeas- can easily mask any atmospheric signal that may exist urements [Damon, 1995; McCormac et al., 1995; Stuiver and [Damon et al., 1989; McCormac et al., 1995]. We therefore Braziunas, 1998]. Speciesto speciesfractionation effects can measuredboth the oak and cedar in the same laboratory and result in contemporaneous wood having a different specific ac- then replicatedthe measurements betweenthe laboratoriesat tivity but this is corrected using$13Cmeasurements. Pre- The Queen'sUniversityof Belfast, N. Ireland andThe Univertreatment of the wood to {z-cellulose ensures that the molecular compositionof the fraction of wood datedis the same for the differentspeciesused[Stuiveret al., 1984; Hoper et al., 1997] and so variable lignin and/or other cellulosecompoundscan- not contribute to A14C differences.Remainingoffsetsmust therefore reflectrealatmospheric differences in AI4c evenif theseare merely the result of early or late onset of tree growth in a given region with the tree sampling an annually varying AlnClevel[StuiverandBraziunas, 1998]. sity of Waikato,New Zealand. This approachis vindicatedbecausethe data showsan offset of -10 yrs between laboratories for identical samples. This does not in any way affect the measuredrelative differencesbetween the two speciesof tree. 300 ] 250 ' + Wk-Cedar T• + QUB Cedar Rings from trees, that grew in the same year, in opposite hemispheres,give different carbondates(southernhemisphere Palaeoecology Centre,TheQueen's University of Belfast,Belfast, Northern Ireland Radiocarbon DatingLaboratory, Universityof Waikato,Hamilton, 501 New Zealand o Lamont-Doherty EarthObservatory andDepartment of Earthand o o o o o o o , o Cal Year AD Environmental Sciences,ColumbiaUniversity,Palisades,NY PlantSciences Department, LincolnUniversity, Lincoln,NewZealand Figure 1. Independent 'nCmeasurements (yrs BP) on decM• s•ples of • •om New Ze•d (39•S) mMe in Q• and Copyright1998by theAmericanGeophysical Union. W•ato. E•or b•s for aH figures •e • lo which Mcludesthe Poisson counting e•or •d an e•r multiplier to account for Papernumber98GL01065. 0094-8534/98/98GL-01065505.00 overall laboratory reproducibility. 1321 1322 McCORMAC ET AL.: INTERHEMISPHERIC •sCOFFSET 250- T• • 0.51%o(19.7 + 4.1 yrs). However Figure 3 showsthat the offset changesconsiderablyafter 1895 and if data before and after this period are comparedthe offset is -3.40 + 0.589'00(27.2 + 4.7 yrs) for the period up to 1885 and 0.66 + 1.06%o(-5.3 + 8.5 yrs) for the post 1885 interval. An error weightedrunningmean on the combinedoffset data is shown in Figure 4. Here sets of 3 decadaloffset measurements from each laboratoryhave been averagedand the age difference plotted againstthe central date. This showssome variability with time of the hemispheric offset notably between the intervals 1725- 1795 AD (offset 23.1 +_7.0 yrs), 1805- • vv•-Oak --o--- 200. QUB Oak TT/• T •-150. i•- o 100. 1 50 o Cal Year AD Figure 2. Independent anCmeasurements (yrsBP) on decadal samplesof oak from the British Isles (53øN, SherwoodForest, England and 54øN, Shane'sCastle,N. Ireland) made in QUB and Waikato. The replicatemeasurements are shownin Figures1 and2. The time structure of both the cedar and oak measurements is simi- lar to previouslypublisheddatafrom the sameperiods[Stuiver and Becker, 1993; Pearson et al., 1986]. Weighted differencesof the cedar and oak measurements showsa consistentdepletion in the southernhemisphereof -3.4 + 0.58%0 until the decade centred on 1885. results from both laboratories After that the show a reversal such that the 1865 AD (offset34.6 + 7.1 yrs) and again the large change around1895 AD thoughtto be relatedto the anthropogenicinput of fossilfuel CO2 to the northernhemisphereatmosphere. The pre-anthropogenicchange in offset value for the two earlier intervals given above is 11.5 + 10.0 yrs. Although not highly significant this result is suggestiveof small temporal changes in the pre-anthropogenichemispheric offset value. The changes in AtnCasa functionof timeareevidentin Figure 5 which shows the combined oak measurements(circles) and combined cedar measurements(squares)from both laboratories. Modelling Therelativedepletionof 14Cin the southern hemisphere northernhemisphereis slightly depleted andthereafterthe depletion appearsto alternatebetweenhemispheres. A similar change in hemispheric offset has been recently reported [Stuiver and Braziunas, 1998]. Table ! gives our individual measurementson decadalsamples of oak and cedarfrom both ernOcean, surface ocean14C islow,reflecting theexposure of laboratories. Atlantic surfacewatersremainshigh reflecting their origins in Errors on the measurements include both the Poissoncountingerror and an error multiplier to accountfor overall laboratoryreproducibility. Also given are the per mil. differencesbetweencedarandoak determinedindependentlyin both laboratories. Table 2 showsthe errorweightedmeanof the differencesbetween oak and cedarfor selectedperiods.The offset betweencedar and oak over the entire set of measurements is -2.46 + atmospherebefore 1885 can be attributedto the differencesin oceancirculationbetweenthe two hemispheres. In the Southold, deep waters at the surface. While there is a similar but smallerdepletion of 14Cin theNorthPacific,the 14Cin North low latitudes.Theoceaneffecton atmospheric •4C gradients has previously been shown in both a simple one-dimensional atmosphericmodel [Levin et al., 1987] as well as an atmospheric transport model from the GISS GCM [Braziunaset al., 1995]. Here, we estimate the magnitude of this preanthropogenic interhemispheric gradient by using a simple two box (northern and southern hemispheres) atmospheric Table 1. tnCMeasurements (yrsBP)onDecadal Samples of CedarandOakandHemispheric Differences in 'nC(%0)Determined Independently in Belfast(QUB)andWaikato(Wk) Year AD 1725 1735 1745 1755 1765 1775 1785 1795 1805 1815 1825 1835 1845 1855 1865 1875 1885 1895 1905 1915 1925 1935 Cedar-Wk Cedar-QUB 162+20 213 + 19 232+19 224 + 18 248+20 218+19 246+19 242+20 176-+ 19 129+20 135+ 19 194 + 20 224+19 249 + 19 203+18 192+18 234+18 230+ 18 164+ 19 154+ 19 140+20 141+18 165 + 20 180+ 19 155_+19 167+17 158+18 120+ 17 147 + 19 136+20 178 + 19 173_+20 151+19 159+20 146 -+ 20 152+20 165+14 142+13 152+20 138+ 17 108 + 17 101+19 165 + 19 146+21 Oak-Wk 130+20 184 + 20 208_+19 208 -+ 18 208_+20 197_+18 226-+20 212_+20 124-+20 121_+20 104_+19 112-+18 144 _+20 147-+20 125_+18 148-+17 123_+20 126-+20 127 _+20 154-+21 164 -+ 20 187_+20 Oak-QUB 135+20 167 + 21 201+20 Diff.-Wk%o 184+18 170+19 209+18 208+20 121+ 19 134+ 19 110+20 91_+21 130_+21 104-+20 127+14 -4.0 + 3.5 -3.6 + 3.5 -3.0-+3.4 -2.0 _+3.1 -5.0_+3.5 -2.6_+3.2 -2.5-+3.5 -3.8+3.5 -6.5-+ 3.4 -1.0_+3.5 -4.5-+3.2 -3.6_+3.1 -2.6 _+3.5 -4.1-+3.5 -3.8-+3.2 143-+22 135+20 164+ 17 96 + 17 139+20 128 + 19 186+20 -2.4-+3.0 -4.4-+3.1 0.8-+3.0 -2.5 _+3.5 2.2+3.5 -1.7 _+3.4 1.7_+3.1 Diff.-QUB%o 0.0+3.5 -3.4 -+ 3.6 -2.9-+3.5 -2.4+3.1 -2.8+3.1 -3.1+3.1 -2.8-+3.4 -5.4-+3.4 -2.5_+3.4 -5.1-+3.5 -8.5_+3.5 -2.0 _+3.6 -6.0-+3.5 -4.8-+2.5 0.1-+1.9 -2.1-+3.5 3.2-+3.0 -1.5 _+3.0 4.8+3.5 -4.6 _+3.4 5.0_+3.6 McCORMACET AL.: INTERHEMISPHERIC•nCOFFSET 5O Table 2. Cedar Minus Oak DeterminedIndependently in Both Laboratories(offsets given in yrs) TTTTT-I-T • 251725-1935 1725- 1885 21.5 + 5.8 27.7 + 6.6 17.9+ 5.8 26.8+ 6.6 1895- 1935 QUB Combined 19.7 + 4.1 -0.4 + 27.2 + 4.7 8.50 x = Z (x/o,2)/Z (1/oi 2) and1/•= Z (1/oi 2) model in which 0 12.4 -9.6+ 11.7 -5.3 + TTTTT•T?o??øa, oTT o • Waikato 1323 ,_ -:25 ø-500 we assume that the concentration 666 of atmosCal Year AD pheric14Cin eachhemisphere reflectsa balance between pro- duction, exchange with the ocean, and exchange between Figure 4. Three decaderunning mean of hemisphericdifferin 14C.Modelresults aresuperimposed (solidline). hemispheres(Table 3). Our "best guess"valuesfor exchange ences terms and surfaceoceanvaluesgive a depletionin the southern hemisphereof-3.0 %0. This value is sensitive to the interhemisphericmixing time, the accuracyof our reconstruction of proportionto their areas and gas exchangerates. The magnipre-anthropogenic surface oceanA14Candtheproduction rate tude of the calculatednorthernhemispheredepletion is consisof 14C. Whilewepresent results for our"bestguess" values, tent with the observationsfrom the tree rings (Figure 4). The gradient in A14Cinduced by the inputof fossil reasonableadjustmentsin any of thesepoorly constrainedpa- atmospheric rameterscan bring the calculatedaverageinterhemisphericgra- fuel carbon into the atmosphereis, like the preindustrial gradidient into agreementwith the tree ring measurementsgiven ent, sensitiveto the interhemisphericmixing time, but is also above (-3.4%0) as well as the more complexmodels of Levin et sensitiveto the location of the uptake of fossil fuel carbon. If al. [1987] (-4 %0)andBraziunaset al. [1995] (-3.1%o). Also, we put 80% of the fossil fuel that doesnot remain in the atwhile we presentthe differencebetweenaveragevaluesin each mosphereinto a northernhemispheresink [Tans et al., 1990] hemisphere, the moredetailedstudyof Braziunaset al. [ 1995] the magnitudeof the interhemispheric gradient drops only to showsthat there is considerablestructurein A14C within each 0.9 %o in 1950 vs. 0.2%0 when 41% of the carbon is absorbed hemisphere. WhileweshowtheA14Cgradient hemisphere,with the differencefor the latitudesof the trees in in thenorthern induced by the input of fossil fuel carbon into the atmosphere this studyapproximately30% higher than the averageinterafter 1952, in reality the initiation of atmospherictesting of hemisphericgradient Theswitchto relativedepletion of 14Cin the northern atomicweaponsat this time wouldonce again producehigher hemisphere is a consequence of the additionof fossil fuel car- atmospheric InC in thenorthern hemisphere. bon (no 14C)primarilyto thenorthernhemisphere atmosphere. We can calculate the expectedchange in the atmos- phericAI4c gradient by calculating theincrease in carbon in each hemisphereof our two box model dueto the addition of fossil fuel carboninto the northernhemisphereand the uptake of part of this carbonby oceanand/or land biota. We addfossil fuel carbon to the northern hemisphere atmosphereusing the fluxes from Keeling [1973] (before 1950) and Marland and Rotty [1984] (after 1950). It is assumedthat 60% of the fossil fuel emissions remain in the atmosphere, consistent with ocean carbon cycle models [Siegenthaler and Joos, 1992]. While there is much debate [Tans et al., 1990; Heimann and Keeling, 1989; Broecker and Peng, 1982] as to where the excess carbon is actually absorbedinto the ocean and atmosphere,we simplyassumea null biosphereand addthe carbonto the northern (41%)and southern(59%)hemisphere ocean in Conclusions 14C measurements madeoncontemporaneous decadal blocksof tree rings from the British Isles and New Zealand show a depletion of-3.4 _+0.58 %0for the period 1725 to 1885 AD and a mean offset of 0.66 + 1.06 %0for the period post 1895 AD. Calculations using a simple two box atmospheric model are consistent withthis beingcaused by a depletionof the 14C contentof the atmosphereas a result of anthropogenicinput of fossil fuel CO2into the northern hemisphereatmospheresince the time of the industrial revolution. A small change in the pre-anthropogenicoffset beweenthe periods 1725 - 1795 AD and 1805 - 1865 AD is suggestive of a natural time varying componentto the hemisphericoffset. 100- ,'T 50- T / '• • o -50- --o--1 O0 o 6 QUB diff 6 6 6 • • o o o o o Cal Year AD Cal Year AD Figure5. A•C (%o)values forthecombined cedar (southern Figure 3. Differences in •4Cdates(yrs) of southernhemi- hemisphere) andcombined oak (northern hemisphere) meassphere(cedar)andnorthern hemisphere(oak) wood measured urements. Thedisappearance of the hemispheric offseta•und by QUB and Waikato (Wk). 1895 AD is evident. 1324 ' McCORMAC ETAL.:INTERHEMISPHERIC •nC OFFSET Table3. Parameters Usedto Calculate Steady Stateinc Concentration in Northern andSouthern Hemisphere Atmosphere. Air-sea Fluxes ofCarbon andincareCalculated for10øLatitude Bands forEach Ocean 1.2 yr Timeconstant forinterhemispheric exchange ofCO21 Northern Hemisphere 26 x 10•5molesC CO2inatmosphere 2 14Cproduction rate 3 230moles •4C/yr 2.5x 10•5moles C/yr Air-Seaexchange 4 -55 %0 AIncofCO2transfered fromseato• SouthernHemisphere 26 x 1015molesC CO2inatmosphere 2 14Cproduction rate 3 230moles •4C/yr 4.2x 10•5moles C/yr Air-Seaexchange 4 -65 %0 AI4CofCO2transferred fromseatoair• I Tansetal.[1978] 2Broecker andPeng[1982]3Broecker andPeng[1974] 4 Air-Sea fluxisarea weighted gross fluxusing wind-speed dependent exchange relationship inTans etal.[1990], pCO 2= 280. Sea-air exchange isarea weighted gross fluxusing wind-speed dependent exchange relationship andsurface ocean ApCO 2inTans etal.[1990], mean ocean pCO:z = 280.Modern ApCO 2areadjusted everywhere by6 Ilatm fornonetfluxofCO2totheocean. 5 Surface ocean InC(pre-bomb) from Broecker andPeng [1982] corrected topre-anthropogenic values byadding 10%0to warm surface water values. Thesurface ocean AI4cisweighted bytheCO2fluxfromtheocean foreach10ølatitude band and each ocean. F.G.,Liquidscintillation counter characterization, optimizaAcknowledgements.This work was supportedby a researchgrant McCormac, from the Natural Environment Research Council (NERC), Grant No GR9/02597to Dr F.G. McCormacat The Queen's Universityof Belfast andby a grantto Dr A.G. Hogg at The Universityof Waikato,by the New ZealandFoundationfor Research,Scienceand TechnologyGrant number UOW-508. tionandbenzene puritycorrection, Radiocarbon, 34,37-45,1992. McCormac, F.G., R.M.,Kalin,andA. Long,Radiocarbon datingbeyond 50,000yearsby liquidscintillation counting, in Liquid Scintillation Spectrometry, edited byNoakes, J.E.,Schonhofer, F.,and Polach, H.,pp.125-133, Radiocarbon, Tucson, Arizona, 1993. McCormac, F.G.,M.G.L., Baillie,J.l•, Pilcher, andR.M.Kalin,Loca- tiondependent differences intheinccontent of wood, Radiocarbon, References 37, 395-407, 1995. Pearson, G.W.,J.R.,Pilcher, M.G.L.,Baillie, D.M.,Corbett, andF. Qua, High-precision incmeasurement ofIrishoaks toshow thenatural •4C Braziunas,T.F., I.Y. Fung,and M. StuiverThe pre-industrial atmos- pheric14CO2 latitudinal gradient asrelatedtoexchanges among at- variations fromnD1840to 5210Bc,Radiocarbon, 28, 911-934,1986. Siegenthaler, U., andF.Joos, Useof a simple model for studying the mospheric, oceanicandterrestrial reservoirs. GlobalBiogeochemical Cycles9, 565-584,1995. Broecker,W.S., andT-H PengTracersin the Sea, Eldigio,Palisades, New York, 1982. oceanic tracerdistributions andthe globalcarboncycle,Tellus, 44B, 186-207, 1992. Stuiver, M.,R.L.Burk and, P.D.Quay, 13C/•2C ratios intreerings andthe transfer of biospheric carbon to theatmosphere, J. Geophys. Res., Broecker,W.S.,andT-H Peng,Gasexchange ratesbetweenair and sea, Tellus,26., 21-35, 1974. Cain,W.F.,andH.E. Suess, Carbon-14in tree-rings, J. Geophys. Res., 89, 11731-11748,1984. Stuiver, M., andB. Becker, High-precision decadal calibration of theradiocarbon timescale, AD1950-6000 Bc,Radiocarbon, 35, 35-65,1993. 82, 3688-3694, 1976. Stuiver, M., andT. Braziunas, Anthropogenic andsolarcomponents of Damon,P.E., S. Cheng,andT.W. Linick,Fineandhyperfine structure in hemispheric inC,Geophys. Res.Lett.,25,329-332, 1998. thespectrum of secular variations of atmospheric 14C, Radiocarbon Tans,P.P.,I.Y. Fung, andT. Takahashi, Observational constraints onthe 31,704-718, 1989. global atmospheric CO2budget, Science, 247,1431-1438, 1990. Damon,P.E.,A noteconcerning "location-dependent differences in the Vogel, J.C.,A.,Fuls, E.Visser, andB.Becker, Radiocarbon fluctuations •4Ccontent of wood"by McCormac et al.,Radiocarbon, 37, 829-830, during the third millennium BC, Radiocarbon, 28, 935-938, 1986. 1995. Heimann,M., and C.D. Keeling,A three-dimensional modelof atmos- Vogel,J.C.,A.,Fuls,E.Visser, andB.Becker, Pretoria calibration curve phericCO2transport based onobserved winds,2, Modeldescription andsimulated tracerexperiments, in Aspects of ClimateVariability in thePacificandWestern Americas, editedby D.H. Peterson, pp.237275,Geophy. Monograph Series, 55,AGU,Washington DC, 1989. forshort-lived samples, Radiocarbon, 35,73-85,1993. F.G. McCormac, M.G.L. Baillie, J.R. Pilcher, D. Brown and S.T. Hoper,Palaeoecology Centre,Schoolof Geosciences, The Queen's Hoper,S.T.,F.G.McCormac, A.G.Hogg,T.F.G.Higham, andJ.Head, Universityof Belfast,BelfastBT7 INN, NorthernIreland. (e-mail: @qub.ac.uk;m.baillie@qub.ac.uk; j.pilcher@qub.ac.uk; Evaluation of woodpre-treatment onoakandcedar,Radiocarbon (in f.mccormac @qub.ac.t/k; s.hoper @qub.ac.uk) press), Proceedings ofthe16thInternational •4CConference, 1997. d.brown A.G. Hoggand T.F.G.Higham,Radiocarbon DatingLaboratory, Keeling, C.D.,Industrial production of carbondioxide fromfossilfuels University of Waikato,PrivateBag3105,Hamilton, New Zealand.(eandlimestone, Tellus,35, 174-198, 1973. @waikato.ac. nz;thigham@waikato.ac.nz) Lerman,J.C.,W.G. Mook,andJ.C.Vogel,•4Cin treeringsfrom differ- mail:ahogg ent localities,in RadiocarbonVariationsand AbsoluteChronology, editedby I.U. Olsson, Proceedings, XII NobelSymlx•ium, Wiley, New York, 275-301, 1970. J.Lynch-Stieglitz andW.S.Broecker, Lamont-Doherty EarthObservatoryandDepartment of EarthandEnvironmental Sciences, Columbia University, Palisades, NY 10964 (e-mail:jean@ldgo.columbia. edu; edu) Levin,I., B. Kromer,D. Wagenbach, andK.O.Munnich, Carbon isotope broecker@ldgo.columbia. J.Palmer andL. Xiong,PlantSciences Department, LincolnUnivermeasurements of atmospheric CO:at a coastalstationin Antarctica, sity,Lincoln, NewZealand. (e-mail:palmer@kauri.lincoln.ac. nz) Tellus,39B, 89-95, 1987. Marland,G., andR.M. Rotty,Carbondioxideemissions fromfossilfuels: December 11, 1997;revised March2, 1998; a procedure for estimation andresults from1950-1982, Tellus,36B, (Received 232-261, 1984. acceptedMarch 11, 1998)