JOURNAL OF GEOPHYSICAL RESEARCH, VOL. 101, NO. D4, PAGES 8985-8999,APRIL 20, 1996 Decadal evolution of the Antarctic ozone hole Yibo JiangandYuk L. Yung Divisionof GeologicalandPlanetarySciences, CaliforniaInstituteof Technology,Pasadena Richard W. Zurek Earth and Space SciencesDivision, Jet PropulsionLaboratory,California Institute of Technology, Pasadena Abstract. Ozonecolumnamountsobtainedby thetotalozonemappingspectrometer (TOMS) in the southernpolarregionare analyzedduringlate australwinter and spring(days240-300) for 1980-1991usingarea-mapping techniquesandareaweightedvortexaverages.The vortexhereis definedusingthe-50 PVU (1 PVU- 1.0 x 10-6K kg-1m2s'l) contour onthe500K isentropic surface. Theprincipal results are: (1) thereis a distinctchangeafter 1985 in the vortex-averaged columnozone depletionrateduringSeptemberandOctober,theperiodof maximumozoneloss,and (2) the vortex-averaged columnozonein lateAugust(day240) hasdroppedby 70 Dobson units (DU) in a decadedue to the lossin the dark and the dilution effect. The meanozonedepletionratein the vortexbetweenday 240 andthe day of minimum 1 vortex-averaged ozoneis about1 DU d- at thebeginningof the decade,increasingto 1 about1.8 DU d- by 1985,andthenapparentlysaturatingthereafter.The vortexaveragecolumnozoneduringSeptemberandOctoberhasdeclinedat the rateof 11.3 DU yr-• (3.8%)from1980to 1987(90DU over8 years)andata smaller rateof 2 DU yr-• (0.9%)from1987to 1991(10DU over5 years,excluding theanomalous year 1988). We interpretthe year-to-yeartrendin the ozonedepletionrate duringthe earlierpart of the decadeas dueto the riseof anthropogenic chlorinein the atmosphere. The slowertrendat the endof the decadeindicatessaturationof ozone depletionin the vortexinterior,in that chlorineamountsin the mid-1980swere alreadysufficientlyhighto depletemostof the ozonein air withinthe isolatedregions of the lower-stratospheric polarvortex. In subsequent years,increases in stratospheric chlorinemay haveenhancedwintertimechemicallossof ozonein the southpolar vortexevenbeforemajorlossesduringtheAntarcticspring. I. Introduction The presenceof thesechlorineradicals[de Zafra et al., 1987], The dramatic decrease of the total column of ozone over Antarcticain southernlate winterand spring(Augustthrough November),a phenomenonknown as the Antarcticozonehole, was first describedusing observationsmade with Dobson spectrophotometer on the ground [Farman et al., 1985] and laterby satelliteobservations [Stolarskiet al., 1986]. It is now understood that the Antarcticozonedepletionis causedby the catalyticchlorinechemistryin the lower stratosphere, where low temperaturesprevail due to the special geographyand meteorologyof the Antarcticregions(e.g., Plate 1). This cold air in the lowerstratosphere at high southernlatitudespermits the formationand persistenceof polar stratospheric clouds (PSCs). Heterogeneous chemistry[Solomonet al., 1986] on theseice clouds,followedby the actionof sunlight,converts particularly of C10 andits anticorrelation with 0 3, hasbeen confirmedby in situ measurements from aircraft[Andersonet al., 1989a,b, 1991] andby remotesensingfrom the Upper AtmosphereResearchSatellite (UARS) [Manney et al., 1993b; Waters et al., 1993a, b]. While there is little doubt of the key role played by heterogeneous chemical reactions involvingstratospheric chlorine,thequantitative aspects of the mechanismsinvolvedin producingthe Antarcticozonehole are still the subjectsof intensestudyandobservation.This is dueprincipallyto the effectsof dynamics on the temperature (andthusthe ice cloudmicrophysics) andon the distributions of chemicaltrace gasesand their exposureto sunlight [Solomonet al., 1986; Bojkov, 1986; Mahlman and Fels, 1986; Tung et al., 1986; Garcia and Solomon, 1987; Mcintyre, 1989; Solomon,1990; Schoeberlet al., 1991, 1992; reservoir species of chlorine(HC1and C1ONO2)into very reactiveradicalssuchasC1andC10 [McElroyet al., 1986a,b; Tung and Yang, 1994a, b; Yang and Tung, 1994]. These attempts to Molina et al., 1987b; Toon et al., 1986; Tolbert et al., 1987]. effectsvaryfromyearto yearandthuscomplicate interpretthe observed 30% to 60% decline in total column ozoneamountsduringthe last decade.A thoroughdiscussion Copyright1996by theAmericanGeophysical Union. of the Antarcticozonehole was given by Solomon[1988, 1990] and WorldMeteorologicalOrganization(WMO) [1988, Paper number96JD00063. 0148-0227/96/96JD-00063 $05.00 1989, 1991]. 8985 8986 JIANG ET AL.: ANTARCTIC OZONE HOLE In this paperwe examinethe recordof total columnozone 3. Area-Mapping Method variationsobservedby the total ozonemappingspectrometer The ozonearea-mappingmethodusedhere was described (TOMS) over the period 1980 - 1991. Past analysesof the by Yung et al. [1990] and is similar to that used in area Antarctic ozone depletion have tended to use the ozone minimumvaluesor zonalaverageswhen examiningdecadal mappingof Ertel'spotentialvorticityon an isentropicsurface trends [Bowman, 1985, 1988, 1990; Herman et al., 1991, [Butchart and Remsberg,1986; Baldwin and Holten, 1988]. byanycontour valuegl*(• t) 1993; Krueger et al., 1992; Stolarski et al., 1991, 1992]. LetA(t,gl*)betheareaenclosed Other analyseshave focusedon interannualvariationsin the of ozonecolumnabundance,as a functionof time (0 and ( • ) onthesurface of theEarth.A convenient unitfor ozone minimum values and have found potentiallinks to position phenomenaassociatedwith the Quasi-BiennialOscillation the areaboundby an ozoneisoplethis the areaof the southern (QBO) [e.g., Garcia and Solomon,1987; Lait et al., 1989]. hemisphere, 2•R2 (R is theradius ofEarth).Forcomparison, More recently,Randel and Wu [1995] examinedtrends in the areas out to the Antarctic circle and 60øS latitude circle are ozoneby first averagingTOMS data alongpotentialvorticity 0.079 and 0.13, respectively,while the area of the Antarctica (PV) contoursin order to account for displacementand continent,includingthe ice shelf,is 5.5% of the area of the longitudinalasymmetries of the polarvortex. Anothernatural southernhemisphere. coordinatefor thesepurposes is ozoneitself. Here we will use Sincetotalcolumnozonegenerally changes monotonically the ozonearea-mappingtechniquefirst appliedto Antarctic outwardfrom a minimumin the interiorto the edgeof the ozoneby Yunget al. [1990] to reexaminethe declineratesof polar vortex, an area increase(decrease)of a total column Antarctic springtime column ozone from 1980 to 1991, ozoneisoplethwith time impliesthat the ozonehole (i.e., the emphasizing both generaland year-to-year changesoverthat regionof lowestcolumnozone)is expanding (shrinking).This period. A key modificationof the previousapplicationof this resultholdsno matterwherethe centerof ozoneholeis. Thus, techniqueis to constrainthe ozoneareamappingto the south to first order,this methodfiltersout planetary-scale (i.e., low polar vortex using values of PV derived from National longitudinal wavenumber) perturbations of theAntarcticpolar MeteorologicalCenter(NMC) datafor thesameperiod. vortexsuchas distortions of thevortexor displacements away In section2, we first briefly describethe data we used.The from the pole. We assumethat the ozonecolumnabundance area-mappingmethod is describedin section3. Then, in in the southpolar night regionis smallerthan that in the section4, we presentour main results obtainedfrom the daylightregion and only include daytimedata in the area TOMS ozone data using the area-mappingmethod in averages, adjusting theareaweightingto includejustthesunlit combinationwith the use of PV and of area-mapped NMC portionsof thesouthpolarregions.This haslittle effecton our temperaturesin the polar vortex. Two importantfeatures analyses aswe focusonthelatewinterandspringperiodwhen emergingfromthe analysisarea distinctchangein the decline the area with no TOMS measurements is very small (e.g., rate of vortex-averagedcolumn ozone after 1985 and the Plate 1). anomalyrepresented by the 1988Antarcticspring. The assumptionof monotonic variation breaks down beyondthe edgeof the polar vortex,in the regionof the total columnozonemaximain high midlatitudessometimescalled 2. TOMS Ozone Column Abundance,PV and the polar "collar"region. For somecontoursnear the vortex Temperature boundary,area-mappingwould mix data pointsfrom outside The Nimbus 7 spacecraftwas launchedinto a local-noon, of the vortex with that inside the vortex. Vortex-averaged Sun-synchronous, near-polarorbit on October24, 1978. Its quantitieshave been shownto be useful in examiningthe TOMS instrumenthas measuredthe spatial distributionof relationships among,for instance,ozone,temperature andC10 total ozonefrom 1978 until May 6, 1993, by scanningacross at variousheightsin the lower stratosphere [e.g., Manney et the track of the satellite to obtain data between successive al., 1994b]. Randel and Wu [1995] recentlymappedcolumn satellite orbital tracks. Total column ozone is retrieved from ozoneby averagingtheTOMS dataaroundPV contours at 520 the measured differential absorption of backscattered K. The issueis how to applya vortexconstraintgiventhat a ultraviolet irradiance using observationstaken with solar definitionof thepolarvortexin termsof PV contours will vary zenith anglesup to 88ø. No measurements are availablein with heightandfrom yearto year. regionsof polar night. In our analysiswe used the daily Becausethetotalcolumnozonevalueis heavilyweightedto TOMS gridded ozone data of version 6.0 [Herman et al., thelowerstratosphere [ e.g.,Manneyet al., 1994a;Froidevaux 1991] from NASA (on a 1ø x 1.25ø grid in latitude and et al., 1994], we have chosento definethe vortexusingPV longitude)from 1980 to 1991. The 1979 datawerenot usedin valuesthere. By inspectionwe have chosena singlevalue, our analysismainlydue to frequentlymissingdata (e.g. days namely,-50 PVU (1 PVU=I.0 x 10'6 K kg'l m2 s'l). In later 277, 278, 279) in this year. The more recentversion7 with years (1992 and 1993, not consideredhere), Chen [1994] datacoverage till 1994hasnotbeenofficiallyreleased yet. foundthatthisvalue,whichwas towardthe polewardedgeof The othertwo data setsusedare NMC temperatures and the region of large PV gradients,definedan isolatedinner Rossby-ErtelPV [Manney and Zurek, 1993a] derivedfrom vortexat 500 K. For the yearsand seasonconsidered herethe NMC analysesof temperature and geopotential heights[e.g., -50 PVU contouris typicallyin the middle of the regionof Gelman et al., 1986]. The PV and temperaturefields are strongPV gradientson the 500 K isentropicsurfaceand is griddedat 2.5ø x 5.0ø in latitudeand longitude.In our study outsidetheregionof largeozoneloss(Plate1), whichmakesit we will usetemperature andPV fieldson the500 K isentropic suitablefor limiting the ozone area-mapping. Interannual surfaceto help interpretvariationsin the total columnozone. variationsof the areawithin thisPV contourarerepresentative This level is in the lowerstratosphere nearthe ozonenumber of changesin vortex size and reflect at least indirectly densitypeak in earlyAugust,priorto the formationin recent variations in planetary wave activity, including minor yearsof theozoneholeduringtheaustralspring. warmings; these can affect both ozone transport and JIANG ET AL.: ANTARCTIC heterogeneouschemistry. To assess these effects more quantitativelyrequiresconsiderationof vertical as well as horizontalvariationsin bothozoneand PV and is beyondthe scopeof thispaper. OZONE HOLE 8987 constrainedby the locationof the -50 PVU contourat 500 K. The time intervalchosenfor eachyearis fromday 240 (August 28 for nonleapyear)to day 300, corresponding to theperiodof maximum ozone depletion in each year. These vortexconstrainedarea averagesof columnozoneare significantly largerthan the minimumozonecolumnabundance[e.g., Lait et al., 1989, Figure 2a], as they includelarge regionsof the vortexcloseto the boundary,where ozonevaluesare higher 4. Area Mapping of Ozone, PV, and Temperature' Results and Discussion 4.1. Average Column Ozone: The Ozone Hole Period (Plate 1). The dotted lines in Figure 1 indicatesthe area-weighted We will first investigatevariationsof area-averaged ozone columnabundance insidethepolarvortex.Figure1 showsthe averageof ozone column abundancein the region between temporalvariationsof the area-weightedaverageof ozone 60øS and 90øS. Differences between this zonal and the vortexcolumn abundanceinside the polar vortex (solid line), as limitedaveragereflectthe longitudinal asymmetry of thepolar . 180' 0 100 150 200 250 300 550 Colurn_nOzone (DU) Plate 1. Southernpolarorthographic projectionof ozonecolumnabundance(DU) on day 275 (October2) 1987. Thereareno TOMS datain the whitearea. The areaboundby the 300-DU contouris 13% of the area of the southernhemisphere. The smaller and larger circles are located at 60øS and 30øS latitudes, respectively. The thick red line indicatesregionswhere the temperatureis below 195 K on the 500 K isentropicsurfaceandpolarstratospheric clouds(PSCs)mayform. The -50 PVU contourof potentialvorticity (PV) (thickdarkline) at 500 K, usedto definethepolarvortex,is alsoshown. 8988 JIANG ET AL.: ANTARCTIC OZONE I October 350 I Septernber I October I Septernber 272 HOLE 274 280 271 268 276 278 277 263 276 274 278 1980 300 -''''' "• 350 • / \ z ''" " \ " 25O 300 ß, . . ß .... . , \ \/ / /x xl I \ \/ /\ t• \ -2_(3 \ , .. \ z 2OO 350 -30 cO z 300 o 250 N o z -40 • D 250 o 200 200 D 350 1984 810 .... 1985 815 90 ' -5o YEAR i,i 300 z t• 250 z < 200 z 350 1987 1986 300 Figure 2a. The area-weighted average ozone column abundance(DU) on day 240 of eachyear (dottedcurve);same for the minimumvalueattainedin eachyearbetweendays240 and 290 (solid curve). Dashedline givesthe percentlossof ozone(relativeto day 240). The dayson which the minimum value for the area-weightedaverageozonecolumnabundance occurred are indicated. o 250 z o 200 N O 35o 988 1989 dynamicallyactive [Krueger et al., 1989; Schoeberlet al., 1989; Kanzawaand Kawaguchi,1990]: the vortexand ozone holewere,by southern hemisphere standards, often.greatly 300 distorted anddisplaced awayfromthe geographic southpole. By contrast, thepolarzonalandvortex-averaged columnozone averages areremarkablysimilarin 1987and 1989,indicating thatin thoseyearsthevortexwasnearlyzonallysymmetric and 250 200 350 1991 1990 300 extended at least to 60øS. Similar differences extendto otheryearsas well, with the polar zonal and vortex area-weighted averagesof column ozoneagreeingmore closelyin Septemberduringodd than duringevenyears. Furthermore,as seenin Plate2, the vortex- • i i . i , i . , i . i , i , , i 200 . limitedaverageof columnozonetendsto decrease significantly from 1981 to 1982 and 1983 to 1984, but with the column ozoneaveragesrelativelyunchangedfrom 1980 to 1981, 1982 to 1983, and until October1984 to 1985. A differentpattern Figure 1. Area-weightedaverageozone column abundance followsin 1986, with ozoneaveragevaluessimilarto thosein (DU) insidethe polarvortexboundby PV contourof-50 PVU 1985. These are followed by a significantdecreasein from days 240 to 300 for 1980 - 1991. Dotted lines denote increased valuesin area-weighted average ozone column abundance (DU) September-October1987but substantially 1988,whenvortex-limited columnozonevaluesareashighor between 60øS and 90øS. higher than those for the same monthsin 1984. After the anomaly of 1988 the vortex-limitedozone averageagain vortex and its seasonaldecreasein area during southern declines,with the lowestaveragedvaluesoccurring in October spring. The latteris evidentas a tendencyfor the zonaland 1991. In Septemberthe years 1990 and 1991 are reminiscent vortexdelimitedaveragesto separateafterSeptember.As the of the patternin vortex-limitedaveragedcolumnozonebefore vortexshrinksseasonally, the zonalaverageincludesmoreof 1986. The lowest vortex-averaged ozonecolumn abundance 240 250 260 270 DAY 280 290 3•0 250 260 270 280 290 300 DAY the higherozonevaluesoutsidethe vortex. The short-periodoccurs in 1991. This result is consistent with that based on an fluctuations (i.e., of theorderof a few to severaldays)aremore analysisof the ozoneminimumvaluein October[Kruegeret pronouncedin the high-latitudezonal average.Similar but al., 1992]. Hofmannet al. [1992] arguedthat the penetration smaller amplitudefluctuationsappear in the vortex-limited of volcanicaerosols fromPinatuboandHudsoninto the polar area-weighted column ozone. These fluctuations, often correlatedwith those of the zonal average,suggestthat synoptic-scaledisturbancesof the vortex, of ozone in the vortex,or of both are not filteredout by averagingwithin the vortexmight haveenhancedthe depletionof ozone. However, Schoeberlet al. [1993] showedthat the polarvortexand the midlatitude regions were nearly isolated from each other duringthe late Augustperiod. The issueof what causedthe vortex. unusuallylow ozonein 1991 remainsunresolved. Both averages show the decline of column ozone in Figure2a showsthe vortex-averaged valueof columnozone September-Octoberoverthe lastdecade.The years1986 and on day 240, the minimumvaluebeforeday 290 (mid-October), 1988 are notable in that the 60øS latitude and vortex-limited and the day on which the minimumoccurredfor eachyear. averagesdiffer even in early September. Theseyearswere As seenhere and in Table 1, the minimumvortex-averaged JIANG ET AL.: ANTARCTIC OZONE HOLE 8989 z o 0.5 8•0 .... 815 , 9•0 , 80 85 9•0 YEAR YEAR Figure2b. Meanozonecolumndepletion rate(DUd -1)in the polarvortex. The solidline denotes the ratecomputed using Figure 2c. The relativerate of ozoneloss in October(solid line) as estimatedusing the model of Sanderet al. [1989]. ozonevalueson day 240 andthe dayof minimumozone. The dashedline is basedon a 5-dayaverageof the initial valueof ozonefrom days 240 to 244. The dottedline is basedon a Thetotalchlorine (Cly)in thestratosphere from1980to 1990 240 and the day of minimum ozone. Details are summarized proportional to CI_andClv2,respectively. All values are is taken from the model of Weisenstein et al. [1992]. The linearleastsquares fit to theaverage ozonevaluesbetween day dashedand dottedlines give the rate of ozonelossif it were in Table 1. columnamountoccurred in all yearsduringthelastweekof September andthefirstweekof October,exceptfor 1988 when it occurrednearlya weekearlierin mid-September. The divergenceof the day 240 and the minimum value curvesindicatesthat the averageloss of ozone during this seasonearly in the decadeis abouthalf that at the end of the decade,except for the anomalousyear 1988. The "initial value" of vortex-averagecolumn ozone on day 240 has declinedby 20% overthe decade. Recentobservations by the Microwave Limb Sounder(MLS) onboardUARS of higher C10 and lower ozone as early as mid-July [Waters et al., 1993a, b; Santee et al., 1995] indicate that some chlorine activation and photochemicalozone loss occur in southern midwinter.The depletionof ozoneat this earlytime (while the geographicsouthpole is still in the dark) can occurbecause the southpolarvortexis sufficientlylargethat its outerregions are in sunlightevenduringthe periodof polarnight. Air there may be exposedto polar stratosphericclouds in the same regionsor can moveinto the sunlitregionsfollowingexposure to PSCs in areasof polar night. The ensuingchemicallossof ozone in the sunlit portionsof the vortex due to chlorine photochemistry couldaccount,then,for the downwardtrendof vortex-average columnozoneat theendof August. Figure 2b showsthe decadalvariationin the mean ozone depletionrate from day 240 to the day when the minimum area-averaged columnozoneis foundin the polarvortex(solid normalized tothat Df1980, the year with Cly =1.44 ppbv. relatedto the computationof variousrates is summarizedin Table 1. The depletion rates are particularly difficult to estimatein 1988 and 1990, becausethe variationduring the seasonis more nonlinearin thoseyears(Plate2). The likely explanationfor the rapid increasein the ozone depletion rateis therapidriseof totalchlorine (Cly)in the lower stratospherein the early part of the decade. The dominant effect of chlorine chemistry on ozone loss is quadraticin C10 [Molina and Molina, 1987a; Sander et al., 1989; Anderson et al., 1991], with smaller contributionsfrom coupling to bromineandHOx chemistry. Thelattereffectsare linear in C10. Figure 2c (solid line) showsthe rate of ozone loss(relativeto 1980) as estimatedusingthe modelof Sander etal. [1989].Thevalues ofClyin thestratosphere aretaken from a model [Weisensteinet al., 1992], which is basedon the releaseof chlorofluorocarbons, atmosphericobservations,and modeling. This showsthat the chemicalforcingon the ozone hole has increasedfrom 1980 to 1985 by about40%, which is about60% of the increasein ozonedepletionrate in the same period(seeFigure 2b). For comparison,we alsocomputethe chemical forcing if it werelinear in Cly.!dashed line)or quadratic in Cly(dotted line).TheBrOm•mng ratiowasset equalto 5 (pptv) in all thesecalculations[Sanderet al., 1989]. We shouldpoint out that despitethe dominanceof theMolinaMolina catalyticcyclethat is quadraticin C10, the chemical forcing is notquadratic in C1 Thereason is thatasCly y' line). In the first threeyearsthe ozonedepletionrate during increases,part of the reactivechlorineis sequestered in the thisSeptember-October periodis onlyabout1 DUd -1. After C1202 dimer,thuslowering itsefficiency forthedestruction of 1982theozonedepletionrate increases to a valueof 1.8 DU d- ozone. 1 in 1985.Sincethen,theozonedepletion ratehasfluctuated After 1985 the depletion of ozone apparentlyreached around 1.5DUd -• andshows a possible QBOsignature. The saturation,in that the ozone depletionrates did not increase dashedline in Figure2b is obtainedin the sameway as for the solid line, exceptthat the meanof 5 days(days240 - 244) is usedfor the initial value. The dottedline is obtainedby using a linear least squaresfit to the data. Detailed information with increasingchlorineand,in fact, were probablymoderated in later years by dynamical processes. These could horizontallymodulatethe regionof photochemicallosswithin the vortex(i.e., the chemicallyperturbedregion)or the areaof 8990 JIANG ET AL.: ANTARCTIC OZONE HOLE September Octob,er •so.I.. ,SepteTber I Octob,er ß ' ß ß ' ' ß ' ß I ß ' ß ' ! ' ß ' ß ß ß "" ' <• r• Z ß ß i• ß t z ß ß ß t ßß ßß i •1ß o iii ßß 250 ß ß ., z o # N o • t e i ........ ........ 200 ........ ß ,i 240 ........ 1980 1981 1982 .19• i ........ ....... ........ •1991 1984 i I,i,i 250 1986 1987 191• 1989 1990 • i I 260 i i , ß I .... 270 I 280 .... I 290 i .... • DAY 240 i i i I 250 i i i ß ! 260 .... I .... 270 ! 280 .... I .... 290 300 DAY Plate 2. Alternativedisplayof thesolidlinesfromFigure1. The solidlinesarefor theoddyears;thedotted lines are for the even years. the vortex itself; they could also affect the rate of vertical motion and so the seasonaldownwellingof air with higher ozonemixing ratiosfrom the middlestratosphere in the polar vortex[Manneyet al., 1995]. The moderateddepletionrate after 1985 for columnozone may alsobe dueto the factthatthe lossrate dependson ozone itself, and ozoneamountsduringthis later periodare already verylow duringthis season.This effectcanbe illustratedby dividing for each year the differencebetweenthe day of minimumvortex-averaged columnozoneand day 240 by the vortex-averaged amounton Day 240. As seenin Figure 2a (dashedline), the 1985 loss rate is sustainedin later years, with 1988 againbeinga mostexceptionalyear. We can comparethe lossratesof the vortex-average areaweightedcolumnozoneof Figure2b to thosecomputed by Lait et al. [1989]. They usedthe minimumTOMS columnozone value found polewardof 30øS on any given day to estimate lineardeclineratesD for the late Augustto Septemberperiodß They thenestimatedthechangeoverthe period1979 - 1987 by leastsquaresfittingof the Septembervariationsandobtained: D [DUd'l] =-0.19(year-1980)- 0.65 This canbe comparedto comparable linearleastsquares fitting of the valuesshownin Figure2b for 1980- 1987' D [DUd'l] = -0.14(year-1980) - 0.71 As noted above, the distinctchangein declinerates for the vortex-averaged column ozoneoccursafter 1985. A linear leastsquaresfitting for the September declineratesfor 1980 1985 yields D [DU d'l] = -0.25(year - 1980) - 0.51 JIANG ET AL.: ANTARCTIC OZONE HOLE 8991 Table1. Column Ozone Depletion Rate(DUd-1)AsComputed byThreeMethods Method la Year 1980 1981 1982 1983 1984 1985 1986 1987 1988 1989 1990 1991 gl (DU) (240) 324 332 297 309 288 289 286 271 283 271 256 259 gl (DU) (Minimum) 293 291 261 262 241 225 233 214 251 217 213 198 Day of Minimum Method2b Depletion Rate 272 274 280 271 268 276 278 277 263 276 274 278 1.06 1.20 0.92 1.55 1.73 1,81 1.26 1.57 1.35 1.59 1.27 1.70 gl (DU) (240) 320 323 293 303 288 292 277 269 289 266 251 262 Method3c Depletion Rate 0.90 0.98 0.85 1,37 1.70 1,83 1.09 1.49 1.65 1.42 1.11 1.75 Depletion Rate 0.76 0.64 0.63 1,36 1.74 1.73 1.14 1.55 1.45 1.50 0.84 1.76 Meancolumn ozone depletion rate(DUd-]) inthepolarvortex. a Method 1 usesozonevalueson day 240 andthedayof minimumozone. b Method 2 isbased ona5-dayaverage oftheinitialvalueofozone fromdays240to244. c Method3 is basedon a linearleastsquaresfit to the ozonevaluesbetweenday 240 and the day of minimum ozone. whichtranslates into an increaseoverthoseyearsby a factorof 3 or more. This wouldreduceto a factorof 2 usingthe decline ratescomputedin Figure 2b as simpledifferences.Both of thesefactorsare largerthan that suggested by the growthin stratospheric chlorine(Figure2c). Lait et al. [1989] foundthat the residualsof the September mappingtechniqueis used to examinethe evolutionof the ozonehole in more detail. Plate 3 showsthe area enclosedby contoursof ozone column abundance,again plotted versus enclosed areain unitsof 2nR2. Asbefore, theperiodcovered is from days 240 to 300 for 1980 - 1991, and the domainof integrationis confinedinsidethepolarvortexby PV contourof decline rates of minimum column ozone values from the -50 PVU at 500 K. In these plots we have used 5-day interannual linearfit showeda distinctQBO signature.This is smoothingto remove high-frequencyvariations. Since there consistentwith the Septemberdecline rates of the vortex- are no ozonedata for the part of the vortex in the dark, the averagedcolumnozoneshownin Figure2b for yearsbefore bottomleft partsof thesefiguresareblank. Note thatthe areas 1986,exceptfor 1984. Oscillations in September declinerates boundedby columnozonecontourslessthan 250 DU increase after 1985 havethe characterand magnitudeof thoseduring Septemberin 1980 - 1982. However,the distinctiveQBO-like patternshownin Plate 2 for vortex-averaged columnozonein 1980 - 1985 is not apparentin lateryears. Figure 3 showsthe vortex-average area-weightedcolumn ozonefor the periodwhenthe ozoneholeis deepestfrom 1980 to 1991. The changein trendfrom year to year for the years beforeand after 1986 is clearlyseen,as is the anomalyof the 1988 column ozone variation. The area-averagedozone columnabundancedecreases with a slopeof 3.8% (11.3 DU) peryearbefore1987and0.9% (2.0 DU) peryearafterthat(the year 1988 is anomalous and is not included in the trend analysis).The averagerate of declineis 25% per decadefrom 1980 to 1991. Theseratesof declineof the vortex-averaged column ozone during one month (mid-September to mid80 85 90 October)of lowestozonemay be comparedto the value30% YEAR per decadeobtainedon the basis of zonal averagesin the southernpolar regionsfrom 1979 to 1990 [Herman et al., Figure3. The vortex-averaged area-weighted columnozone 3OO 250 1993]; similar rates of decline were also obtained when abundance (DU) in thevortexfromdays260 to 290 (mid- columnozonewas mappedas a functionof PV within the Septemberto mid-October),the seasonof minimumcolumn Antarcticpolar vortex for Septemberover the same period ozoneeach year. The steepdottedline is the linear least [Randel and Wu, 1995]. However, the distinct break in trend squaresfit to the dataduringthismonthfrom 1980 and 1987. Theslope is 3.8%(11.3DU) peryearwiththeaveraged ozone after 1985hasnot beenpreviouslynoted. value300 DU duringthistimein 1980asreference.The less steepdottedline is a similar fit to the data from 1987 to 1991 4.2. Growth of the Ozone Hole butexcluding 1988.Theslopeis 0.9%(2.0DU) peryearby The resultspresentedaboveutilizedarea-weighted averages usingthe averaged ozonevalue222 DU duringthistimein of columnozoneover the entirepolar vortex. Here the area- 1987. 8992 JIANG ET AL.: ANTARCTIC OZONE HOLE • d • d v'•yv • o V3•lV V•lV JIANG ET AL.: ANTARCTIC rapidly aroundday 260 (mid-September), implying that the ozonehole is expandingand the columnozoneis decreasing insidethe vortex. By day 280 (early October)the ozonehole has reachedits greatestextentand depth. Typically,the area remainsconstantthenfor a few daysbeforeit beginsto shrink. This reflectsfirst the warmingof the vortexair and eventually the seasonalweakening of the vortex itself, which has generallybrokenup by November. OZONE HOLE 272 277 275 8993 265 266 276 271 282 267 265 274 274 0.12 -61.6 0.08 -66.9 o o4 -73.7 As can be seen from Plate 3, the ozone column abundance contourof 200 DU doesnot appearuntil 1983 but occupiesa maximumareaof 7% of the southernhemisphere in 1991. The 150-DU contourappearsin 1987. These regions are well inside the polar vortex. On the vortexboundary,where the ozonecolumn abundanceis usuallygreaterthan 300 DU, the seasonalchangeof areareflectsthe areaof the vortex. In this region (e.g., the 300-DU contour)there is a little increase duringthe seasonalformationof the ozonehole,but mostlythe areais constantuntil the vortexbeginsto decreasein area. As seenin Plate 3, the ozonehole developsduringlate Augustto mid-Septemberand is largely independentof day-to-day variationsnearthe vortexboundary.Thesedifferenttrendsand the generalsteepeningof the gradientsat the vortexboundary 0 -90.0 80 85 90 YEAR Figure 4. The maximumarea (dots)enclosedby the 250 DU contourin eachyearbetweendays260 and 300. The dayson which the maximum area is attained are indicated. Also shown for the same days are the areas of the vortex, as indicatedby the -52 PVU contour(opencircle) on the 500 K isentropicsurfaceandof the 195 K isotherm(plus),alsoat 500 K. The equivalentlatitudeis indicatedin the right-handaxis. indicate that the air within the vortex is isolated in the lower stratosphere from air at similar levelsoutsidethe vortex. The steepeningof ozonegradientsat the vortexboundaryresults from the spatial expansionas well as the deepeningof the ozoneholeoverthatperiod. The anomalous behavior of 1988 is clearly seen by comparingthe areasbound by the 200-DU contourin the successive years1987, 1988, and 1989. The maximumareas in 1987 and 1989 exceed6% of the southernhemisphere, whereasin 1988 the maximum area is only about 2% of the southernhemisphere. Similar area mapping results were obtainedby Stolarskiet al. [ 1990,Figure3] for theseyears. In Plate 3 the increasingarea in successiveyears of the ozonecontoursinside the vortexon day 240 indicatesthat the ozonecolumnabundancemusthave alreadybegunto decrease earlierin the season. The area mapping(not shownhere) of column ozone from days 220 to 320 (early August to midNovember)showsozonedepletionevenbeforeday 220. This is consistentwith the trends in the vortex-averagedcolumn ozone(Plate2, Figure2a) and,asdiscussed earlier,with recent observations by UARS. Area mapping provides a convenientmeasure of the magnitudeof maximumozonedepletioneachyear. Consider the areaboundedby a low-ozonecontour,suchas the 250-DU contour(Plate 3). Figure4 showsthe maximumareaenclosed by this contourbetweendays260 and 300 (mid-September to late October)and the days on which the maximum area is attainedin eachyear. Exceptin 1981 and 1986 the increaseof the maximumarea before 1987 is roughlylinear. The linear maximum area of the ozone hole usually occurs in late Septemberor earlyOctober,consistent with the vortex-average trends discussedearlier, and also near or before the time when the minimum ozone column amounts(not shown) are found. One may ask whetherthis rapid growth in the chemical ozoneholeis accompanied (or partlydriven)by climatological changesin the stratosphere [e.g.,Mahlman et al., 1986, 1994; Angell, 1993]. To addressthis questionqualitatively,we computethe areas of the polar vortex using the -52 PVU contourand the 195 K isotherm,both on the 500 K isentropic surface. Figure 4 showsthese areason the same days of maximum area of the 250-DU column ozone contour. The vortex (PV) area has little trend over the decade(only 0.05ø yr-1;seeTable2), although it fluctuates interannually abouta more or less constant value. In 1980 the vortex area at 500 K is nearly twice that of the 250 DU contour,but the latter increasesuntil it fills more than 70% of the entire vortex by 1985. After 1985 the fluctuations in the area of the 250-DU contour reflect those of the vortex area itself, which limits the size of the 250-DU area and thus of the ozone hole. The lack of correlationin Figure 4 between the areas enclosedby the 195 K temperature,an indicatorof the horizontalextentof PSCs, and the areasenclosedthe 250-DU column ozone contour,on the days when the latter is a maximum,is notsurprising giventhatmuchof theprocessing of polar air would have occurredearlier. Furthermore, stratospheric windscanexpose mostof thevortexinteriorair leastsquares fit shows a slopeof 8.36x 10-3 peryearfrom to PSCs, even if the latter occupiesonly part of the vortex. 1980 to 1987. The samefitting procedureshowsno trendfor 1987 - 1991 (with 1988 excluded);the averageoverthe whole periodis 5.49 x 10-3 peryearfrom1980to 1991. Fromthe definition of equivalent latitude0e, Table2. Decadal Growth Rates(degree yr-1)of AreasBoundbyIsopleths of 03 (250DU), PV (-52 PVU), andT (195 K) AA(t,•*) = sin(90 ø+ 0e)A0e, we can expressthe changein the maximum area of the 250 DU contour as an equatorwardexpansion at a rate of approximately1.35øper yearbefore1987 andat a rate of 0.84ø per year for the full 1980 - 1991 period (see Table 2). The Oa PV T 1980-1987 1987-1991 1980-1991 1.35+0.27 - 0.00+0.28a - 0.84+0.16 0.05+0.10 0.05+0.19 Reference Figure4 Figure4 Figure4 aTheyear 1988is notincludedin thecalculation. 8994 JIANG ET AL.: ANTARCTIC EQUIVALENT -90.0 -73.7 OZONE HOLE LATITUDE EQUIVALENT -66.9 -61.6 3OO -90.0 300 LATITUDE -75.7 'ß -61.6 -66.9 I "'""" ' i u,•,, •,,• ._ III Ii1./ ........................................ I?.... i I 25O / I ! / / / 200 _1980 150 _1986 1981 1987 _1982 _1988 ..... 198,5 .... 1984 .... I990 ................. 1985 ......... 1991 . ,, ,, lOO 2 AREA 0 i I 4 0.04 I 1989 , ,, • I 0.08 0.12 AREA Plate 4. Ozonecolumnabundanceversusareaon the daysshownin Figure4 for eachyear for 1980 - 1991. The equivalentlatitudeis indicatedin the top axis. This has been shown most dramaticallyfor the north [Waters et al., 1993a], where PSCs are not so extensive. The more critical factor may be exposureto sunlight. For short time periodsthis exposuredependscritically on details of the air motionwithin the vortex,but for periodsof a few weeks or more this factor dependsmore cruciallyon the vortex extent and locationand may be reflectedin the vortexarea shownin Figure 4. At least to first order, most of the growth of the ozonehole over the last decadeappearsdrivenby chemistry alone,due to increasingstratospheric chlorine. This increase has slowed down, not becausethe stratosphericchlorine loading or activation has stopped increasingbut simply because the region of ozone-depleted air now fills (horizontally) much of the polar vortex, whose own fluctuationsin areareflectinterannualvariabilityin dynamical activity. This limiting of the ozone loss region to the vortex is reflectedin the fact that after 1983, high contourvalues of columnozone(largerthan300 DU) are nearthe vortexedgeas definedhere on the 500 K isentropicsurface(Plate 3), except in 1988. In that year the chemicallyperturbedregion was distinctlywithin the vortex(Plate3, Figure4), as describedby Schoeberlet al. [1989] in their analysisof the 1987 Antarctic campaign(AAOE) data. Plate 3 and Figure4 showthat 1988 is not representative in this regardof all otheryearsfollowing 1985. Thus further chemical ozone loss during this season now dependsupon factorsthat would expandthe southpolar vortex region horizontallyor which would extendthe zone of JIANG ET AL.: ANTARCTIC chemicaldepletionvertically, as happenedin 1993 due to heterogeneous chemical effects associated with the entrainmentof Mount Pinatuboaerosolsinto the southpolar vortex[Hofrnannet al., 1994]. Plate 4 shows the variations in ozone column abundance versus area on the days of maximum area in the 250-DU contour(Figure 4) eachyear from 1980 to 1991. The greater extent of ozone-poorair in the years after 1985 is again apparent,as is the anomalyof ozonevaluesin 1988. As more ozonegetsdepleted,the radial gradientof ozonein the vortex gets steeper,as can be seenfrom Figure 5, which showsthe averagegradientof the transitionregionbetween250 DU and 280DU, definedas[280-250(DU)]/[Oe(280DU)0e(250DU)]. OZONE HOLE 8995 days,with the changesbeingmoreprominentaway from the vortex center. These increasesmay be due to the action of synoptic-scale systemswhich are known to produceminor warmingsin the midstratosphere, as these systemshave a characteristic timescaleof 10 - 20 days [e.g., Fishbein,et al., 1993; Manney, et al., 1993a]. These dynamicaleventsaffect ozonein the lower stratosphere within the vortexby moving ozone into the vortex in midstratosphere and then down to lower levels[e.g.,Leovyet al., 1985;Manney,et al., 1994b]. Some care needsto be taken when interpretingthe areamappedfieldsshownin Plates3 and 5, as the areamapping tendsto filter out the planetary-scale features. However,after the ozonehole reachesits maximumdeptharoundday 280 in early spring,the polarvortexstartsto shrinkand ozonecolumn abundancestartsto recover. Significantwarmingeventsand erosionof the vortexare markedin Plate5 by ozoneincreases extending nearly to the vortex center. Because of the anomalouscirculationandextremelycoldtemperature of 1987 [Randel,1988] the final warmingandthe breakupof the ozone hole was delayed20 days (as comparedwith climatology). Plate 5 shows that the ozone depletionrate was never so Years since 1984 are typically characterizedby larger gradientsas a result of greaterozonedepletion,as discussed earlier,with notableexceptionsin 1988 and 1989. As we have remarkedrepeatedly,1988 is anomalousin many respects. The relativelyweak columnozonegradientin 1989 is partly due to the fact that the vortexarea in 1989 was the largestin the record(Figure 4). AlthoughPlate 4 and Figure 5 show resultsfor a singleday, the area-contours of Plate 3 showthat persistentand as extensiveas in 1987. This decreasewas theresultsare representative of the ozoneholeperiodin those interruptedby a minor warming aroundday 280 and then years. Finally,as pointedout by previousstudies[Mcintyre, terminatedby the final warmingafterday300. 1989;Hartmannet al., 1989], the steepgradientsof PV and In 1988 on the otherhand,stratospheric temperatures had ozoneindicaterelativeisolationof the chemicallyperturbed warmed significantlyby late September,terminatingmost regionfrom air outsidethe vortex. decreases in column ozone. The maximum total ozone decline Plate 5 showsthe time rate of changeof ozonecolumn is only 15% duringSeptember1988 comparedto nearly50% abundance overa periodfromdays240 to 300 (lateAugustto duringSeptember1987 [Schoeberlet al., 1989;Kruegeret al. late October)for eachyearfrom 1980to 1991. The resultsfor 1989]. This appearsto be the directresultof the brevityof the 1987havebeenshownpreviously by Yunget al. [1990,Figure declinethroughSeptember. Wave activity at the time was 4]; thisfigureextendsthatresultto 12 years.The averagerate anomalously strong [Manney et al., 1991] and the of ozonedepletionin the vortexis 1 to 2 DUd -1, consistent stratosphericsuddenwarming in late winter was reminiscent with thatshownin Figure2b. of major winter warmings in the northern hemisphere Largerdepletion rates(5 DUd -l) are prevalent nearthe [KanzawaandKawaguchi,1990]. The 1988ozoneholebegan centerof thevortex(Plate5). In someof therecentyears,such filling on October19, nearly six weeksearlierthan in 1987, asthedynamically quiescent years1987and1989,largeozone and driftedout of the polar regionsin mid-Novemberfor the depletionratescan persistfor long periodsof time. In most earliestbreakupsince1979. years the development of the ozonehole is periodically interrupted by increases of ozonewith a periodabout10 - 20 5. Conclusions The area-weighted ozonecolumnabundance averagedover the polar vortexin late August (day 240), oftenviewed as the 6O beginningof the ozonehole season,exhibitsa steadydecline from about 320 DU in 1980 to about 250 DU at the end of the o N o 40 z o o z • 20 810 .... 815 YEAR 910 ' decade. This amountsto a total drop of 70 DU in a decade (Table 1) and accountsfor a largepart of the overalldecrease of morethan90 DU in vortex-averaged Octoberozonecolumn abundance that has occurredover the sameperiod. Most of that drop occurredbefore 1987, as the declinesincethen has beenmuchsmaller(Figure3). Part of this decadal decline may be due to the recurrent presenceof the ozonehole every year. Becauseof the long lifetimeof ozonein the lowerstratosphere, thereis persistence of depletedozone from one year into the next. The effect, known as the dilutioneffect,has beenmodeledby Sze et al. [1989], Prather et al. [WMO, 1989, Chap. 1] andMahlman et al. [1994]. Thesemodelspredicta declineof ozoneof 5 - 7% at polarlatitudesin Junedue to the presenceof an ozonehole, or about 15 - 20 DU. That still leaves 50 - 55 DU in the Figure5. Averageozonecolumngradient withrespect to decadaldeclineunexplained.It is morelikely thattheresultis chlorineproducingincreasing equivalent latitude,computed as described in thetext,for the due to increasingstratospheric samedaysas in Plate4. chemicallossof ozonein the southpolarvortexevenduring 8996 JIANG ET AL.: ANTARCTIC •ClI'IJ. LLV1 J.N31VAII'103 3CIflILLV1 .I.N31VAIfI03 OZONE HOLE 3CIflILLV'I IN3'IVAIfI03 -8 ¸ -8 .8 ¸ .8 ¸ r..• o. o V3•1¾ V3Ei¾ V3t:lV ß ¸ ß •,-.• JIANG ET AL.: ANTARCTIC southern winter, as indicated by the recent UARS observations. Photochemical loss can occur because the OZONE HOLE 8997 vortex. The dilution effect discussedabove may also play a role. This view is necessarily speculative until more quantitative dynamic-chemical simulations of chlorine southernvortex is sufficientlylarge that it has regions in sunlightevenduringthisperiodof polarnight(suchlosscould activation and ozone loss are done. be moreheavily weightedin our methodbecauseof the areaAcknowledgments. We would like to expressour appreciationto weightingof ourvortexaverages). The mean ozonedepletionrate in the vortexbetweenlate R. S. Stolarskifor sharinghis insightsof the TOMS data with us. The NMC geopotentialheightand temperaturestratospheric analyseswere August (day 240) and the day of minimum vortex-averaged obtainedfrom theNationalCenterfor AtmosphericResearchas part of ozone (typically in late Septemberor early October) has an EOS interdisciplinaryscienceinvestigation;wind and PV fields changed fromabout1 DUd-1atthebeginning of thedecade,were derived and providedby Gloria Manney at JPL. We thank M. rapidly increasing toabout 1.8DUd-1by1985,andapparentlyAllen, L. Froidevaux,R. Herman, L. Jaegle,R. Salawitch,S. Sander, saturatingthereafter (Figure 2b). This change in ozone and three anonymousrefereesfor valuablecomments.This work was supportedprincipallyby NASA grant NAGW 2204 to the California depletionratesis qualitativelybut perhapsnot quantitatively Instituteof Technologyand was carriedout there and at JPL, under consistentwith chemicalforcingof the ozonehole solelyby contract with NASA. Contribution number 5465 from the Division of chlorine (Figure 2c). The character and magnitude of GeologicalandPlanetarySciences,CaliforniaInstituteof Technology. fluctuationsin the Septemberdepletionratesin 1980 - 1982 are comparableto thoseafter 1985, andit is possiblethat these References reflectthe extratropicalQBO in ozone. A QBO signaturein the depletionrates derivedhere is perhapsnot so strongas Anderson, J. G., W. H. Brune, and M. H. 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