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1 2 3 The Effect of Representing Bromine from VSLS on the 4 Simulation and Evolution of Antarctic Ozone 5 6 7 Luke D. Oman 1 , Anne R. Douglass 1 , Ross J. Salawitch 2 , 8 Timothy P. Canty 2 , Jerald R. Ziemke 1,3 , and Michael Manyin 1,4 9 10 11 1 NASA Goddard Space Flight Center, Greenbelt, MD, USA 12 2 University of Maryland, College Park, MD, USA 13 3 Morgan State University, Baltimore, MD, USA 14 4 Science Systems and Applications, Inc., Lanham, MD, USA 15 16 17 18 Submitted to Geophysical Research Letters 19 20 21 22 23 24 25 Key points: 26 27 1. Including 5 ppt of Br from VSLS reduces biases with observed ozone and BrO 28 29 2. Resolves a discrepancy with an observational derived parametric model 30 31 3. Causes a decade later recovery of Antarctic ozone to 1980 levels 32 33 34 35 Corresponding Author: 36 Luke D. Oman 37 NASA Goddard Space Flight Center 38 Atmospheric Chemistry and Dynamics Laboratory 39 Code 614 40 Greenbelt, MD 20771 41 Email: [email protected] 42 43 https://ntrs.nasa.gov/search.jsp?R=20170002555 2020-04-04T11:18:28+00:00Z

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Page 1: The of Representing Bromine from VSLS on the and Evolution of Antarctic Ozone … · 2017-10-20 · 127 bromine from VSLS on both the recovery of the ozone layer over the 21st century

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3TheEffectofRepresentingBrominefromVSLSonthe4

SimulationandEvolutionofAntarcticOzone567

LukeD.Oman1,AnneR.Douglass1,RossJ.Salawitch2,8TimothyP.Canty2,JeraldR.Ziemke1,3,andMichaelManyin1,49

1011

1NASAGoddardSpaceFlightCenter,Greenbelt,MD,USA122UniversityofMaryland,CollegePark,MD,USA133MorganStateUniversity,Baltimore,MD,USA14

4ScienceSystemsandApplications,Inc.,Lanham,MD,USA15161718

SubmittedtoGeophysicalResearchLetters19202122232425Keypoints:26271.Including5pptofBrfromVSLSreducesbiaseswithobservedozoneandBrO28292.Resolvesadiscrepancywithanobservationalderivedparametricmodel30313.CausesadecadelaterrecoveryofAntarcticozoneto1980levels32333435CorrespondingAuthor:36LukeD.Oman37NASAGoddardSpaceFlightCenter38AtmosphericChemistryandDynamicsLaboratory39Code61440Greenbelt,MD2077141E‐mail:[email protected] 43

https://ntrs.nasa.gov/search.jsp?R=20170002555 2020-04-04T11:18:28+00:00Z

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Abstract44

WeusetheGoddardEarthObservingSystemChemistry‐ClimateModel45

(GEOSCCM),acontributortoboththe2010and2014WMOOzoneAssessment46

Reports,toshowthatinclusionof5partspertrillion(ppt)ofstratosphericbromine47

(Bry)fromveryshort‐livedsubstances(VSLS)isresponsibleforaboutadecade48

delayinozoneholerecovery.Theseresultspartiallyexplainthesignificantlylater49

recoveryofAntarcticozonenotedinthe2014report,asbrominefromVSLSwasnot50

includedinthe2010Assessment.Weshowmultiplelinesofevidencethat51

simulationsthataccountforVSLSBryareinbetteragreementwithbothtotal52

columnBrOandtheseasonalevolutionofAntarcticozonereportedbytheOzone53

MonitoringInstrument(OMI)onNASA’sAurasatellite.Inaddition,thenearzero54

ozonelevelsobservedinthedeepAntarcticlowerstratosphericpolarvortexare55

onlyreproducedinasimulationthatincludesthisBrysourcefromVSLS.56

1.Introduction57

Simulationsofthefutureevolutionoftheozonelayershowthatthetime58

frameofozonerecoverydependsonthehalogenandgreenhousegas(GHG)59

emissionsscenariosandforecastchangesinthetemperatureandcirculationofthe60

stratosphere,eachwithvaryingimportancedependentonlatitudeandseason61

[Eyringetal.,2013a;Omanetal.,2014;WorldMeteorologicalOrganization(WMO),62

2014].Bromineplaysanintegralpartindeterminingtheatmosphericabundanceof63

ozoneanditseffectivenesspermoleculeatdestroyingozoneisapproximately45‐6564

timesgreaterthanchlorine[Danieletal.,1999;Sinnhuberetal.,2009].Inaddition,65

thebromineimpactonozonedepletionislargerwithhigherchlorine[McElroyetal.,66

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1986]aswellaswithenhancedsulfateaerosolloading,likefollowinglargevolcanic67

eruptions[Salawitchetal.,2005].68

Brominefromveryshort‐livedsubstances(VSLS),mainlybromoform69

(CHBr3)anddibromomethane(CH2Br2)hasalsobeenshowntobeanimportant70

partofthetotalatmosphericburdenofbromineandozonelayerchemistry[Koet71

al.,1997;Sturgesetal.,2000;Salawitchetal.,2005].Theysetal.[2007]estimated72

thatVSLSsupply6to8partspertrillion(ppt)ofstratosphericBrybasedon73

retrievalofstratosphericandtroposphericcolumnBrOatReunion‐Island(20.9°S).74

Salawitchetal.[2010],focusingontheArctic,foundthat5to10pptofstratospheric75

brominefromVSLSisneededtoachieveconsistencywithaircraftandsatellite76

measurementsofBrO.Liangetal.[2014]quantifiedthechemicalandphysical77

transformationsofVSLSafterreleaseintothemarineboundarylayerusingthe78

GoddardEarthObservingSystemChemistry‐ClimateModel(GEOSCCM)and79

concludedVSLSsupplyabout8pptofbrominetothebaseofthetropical80

tropopauselayer.MeasurementsofupperstratosphericBrOfromtheMicrowave81

LimbSounder(MLS),balloon‐borneDOAS(DifferentialOpticalAbsorption82

Spectroscopy),andtheScanningImagingAbsorptionSpectrometerforAtmospheric83

Chartography(SCIAMACHY)yieldestimatesforVSLSsupplyofstratosphericBryof84

5±4.5ppt[Millanetal.,2012],5.2±2.5ppt[Dorfetal.,2008],and7±6ppt85

[Parrellaetal.,2013],respectively.86

Afewstudiesexaminedtheimpactofthisadditionalbromineon87

stratosphericozoneconcentrations.Frieleretal.[2006]showedinclusionof88

brominefromVSLSledtobetteragreementbetweenobservedandmodeledlossof89

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Arcticozoneforaparticularwinter.Fengetal.[2007],focusingonmidlatitude90

ozone,founda10DUdecreasebyincluding5pptofbrominefromVSLS.Yangetal.91

[2014]madearoughestimateof6‐8yearslaterrecoveryoftheAntarcticozonehole92

dueto5pptofbrominefromVSLSbasedontime‐sliceexperimentswithvarious93

chlorineandbrominelevels.SinnhuberandMeul[2015]foundcloseragreementina94

simulationwiththechemistryclimatemodel(CCM)EMACtoobservedtrendsof95

globalcolumnozonewhenincludingbrominefromVSLS.96

AnoutstandingissuehasbeenthedifferenceinAntarcticozonerecovery97

projectionsobtainedusingCCMsandprojectionsderivedfromobservations.98

Newmanetal.[2006]usedanobservationallyderivedparametricmodelofozone99

holeareatopredictrecoveryofAntarcticozoneto1980levelsaround2068under100

theAbhalogenscenario[WMO,2003].CCMsusedintheWMO2010Assessment101

[WMO,2011]returnedAntarcticcolumnozoneto1980levelsby2051onaverage,102

muchearlierthanforecastbytheparametricmodel.Thescientificsummary103

suggestedthatfailureoftheparametricmodeltoaccountforanupperstratospheric104

ozoneincrease,whichwouldbecausedbyGHG‐inducedchangesincirculationand105

temperature,couldexplainthisdifference[WMO,2011],.However,Eyringetal.106

[2010]foundonlyasmalldifferenceinOctoberAntarcticozonevaluesfor107

simulationsusingvariousGHGscenarios.108

SignificantlylaterrecoveryofOctoberAntarcticozonewasnotedinChapter109

3ofthe2014WMOOzoneAssessment[WMO,2014]byeachofthefourmodels110

(CMAM,GEOSCCM,UMSLIMCAT,WACCM)thatcontributedsimulationsforthis111

mostrecentAssessment,comparedtoresultsfromalargernumberofmodelsthat112

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contributedtothe2010Assessment[WMO,2011].However,theywereunableto113

explainthecauseofthelaterrecovery,giventhemodelsimulationsavailableatthe114

time.Themulti‐modelmeanoftheselatestsimulationsindicatedthatreturnof115

AntarcticO3to1980levelswouldnotoccuruntilafter2080.Smalldifferencesinthe116

baseozonedepletingsubstance(ODS)scenariorelativetothatusedintheprior117

Assessment[VeldersandDaniel,2014]causedasmall3‐4%increaseinvortexClyin118

thelaterhalfofthe21stcenturyfortheupdatedsimulations[OmanandDouglass,119

2014]anddonotexplainthelaterrecovery.However,allofthenewsimulations120

representedtheimpactofVSLSonstratosphericBryintheformofaconstant,extra121

5pptofbromine(note:VSLSbromineisindependentofODSspecifications,since122

theVSLSarebiogenicandnotanthropogenic).TheimpactofVSLS‐basedBryon123

ozonerecoverywasnotsimulatedinthe2010Assessment.124

HereweusetheGEOSCCM,whichcontributedtoboththe2010and2014125

WMOAssessments,toquantifytheeffectofanadditional5pptofstratospheric126

brominefromVSLSonboththerecoveryoftheozonelayeroverthe21stcentury127

andthecurrentseasonalevolutionoftheAntarcticozonehole.Weuse5pptfor128

VSLSbrominebecausethisisthebestestimategivenbyWMO[2014].Weshowthat129

inclusionofbrominefromVSLSpartlyexplainswhythe2014Assessmentreported130

asignificantdelayintherecoveryoftheAntarcticozonelayer.Section2describes131

themodelandforcingscenariosaswellasthemeasurementsusedtoevaluatethe132

effectofthisadditionalbromine.Resultsofthesesimulationsandconclusions133

follow.134

135

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2. Model,ForcingScenarios,andObservations136

TheGEOSCCMcoupledtothestratosphericchemistrymodule,StratChem137

[Pawsonetal.,2008;OmanandDouglass,2014],wasusedtoquantifytheimpactof138

includingVSLSbromineontheozonelayer,focusingontheeffectsoverAntarctica.139

Themodelwasrunat2°2.5°(lat.long.)horizontalresolutionwith72vertical140

layersfromthesurfaceupto80km,withphotochemicalinputdatafromJPL2010141

[Sanderetal.,2011].EvaluationofGEOSCCMusingprocess‐orienteddiagnostics142

wasconductedinbothCCMVal‐1[Eryingetal.,2006]andCCMVal‐2[SPARCCCMVal143

2010].GEOSCCMperformedwellinbothchemicalandtransportrelatedprocesses144

[SPARCCCMVal2010;Strahanetal.,2011;Douglassetal.,2012]andsome145

additionalimprovementswerereportedinOmanandDouglass[2014].146

BothGEOSCCMsimulationsdescribedhereusedGHGconcentrationsfromthe147

RepresentativeConcentrationPathway(RCP)6.0,whichproduces6.0W/m2148

anthropogenicradiativeforcingofclimateby2100[Meinshausenetal.,2011;Moss149

etal.,2010].BothusedtheA12014scenarioforODS[VeldersandDaniel,2014],the150

sameasusedinthe2014WMOAssessment[WMO,2014].Thefirstofthese,the151

controlsimulation(A12014_0Br),doesnotincludeanyBryfromVSLS,asassumed152

forthe2010WMO[WMO,2011]andearlierAssessments.Thesecondsimulation153

(A12014_5Br)includesanextra5pptofCH3BrtorepresentVSLS,asrecommended154

bytheChemistryClimateModelingInitiative(CCMI)[Eyringetal.,2013b].155

Seasurfacetemperatureandseaiceconcentrationswereprescribedfroma156

simulationusingtheCommunityEarthSystemModelversion1(CESM1)conducted157

from1960‐2099[Gentetal.,2011],forcedwiththesameRCP6.0GHGscenario.158

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ObservationsfromtheOzoneMonitoringInstrument(OMI)andMicrowaveLimb159

Sounder(MLS)ontheNASAAurasatelliteareusedtoevaluatethesimulationof160

ozoneandbrominemonoxide(BrO)fromJan.2005toDec.2015.OMIlevel‐3161

griddeddailytotalcolumnozonevaluesaredeterminedusingtheOMTO3version162

8.5retrievalalgorithm(Bhartia,2007).Inaddition,verticaldailyozone163

measurementsfromMLSlevel‐2version4.2[Liveseyetal.,2015]wereusedinthe164

evaluation.Descriptionandaccesstothesesatellitedatarecordsisat165

http://disc.sci.gsfc.nasa.gov/Aura.166

ForthecomparisonofmodeledandmeasuredBrO,modeloutputissampled167

atthelocationsforwhichOMImeasurementsareavailable.Duetothedielcycleof168

BrO,modeloutputwassamplingat2p.m.localsolartime,closetothetimeofOMI169

overpass.Version3retrievalsoftotalcolumnBrOfromOMIwereusedfor170

comparisonwiththeGEOSCCMoutput;dataanddescriptionareat171

http://disc.sci.gsfc.nasa.gov/Aura/data‐holdings/OMI/ombro_v003.shtml.172

Destriped,level‐2totalcolumnobservations(OMBRO.003)and1σuncertainties173

(basedonspectralfitting)werefilteredusingflags“xtrackqualityflag”toaccountfor174

theOMIrowanomalyand“maindataqualityflag”toremoveinvaliddata.The175

filtereddatawerethengriddedtomatchthelatitudesandlongitudesofthe176

GEOSCCMsimulations.Daily,griddedsatelliteobservationsoftotalcolumnBrOand177

theassociateduncertaintywerecosineweightedandaveragedbetween60to90°S.178

Similarly,GEOSCCMoutputat2p.m.wasweightedandaveraged,butonlyforthose179

modelgridpointswherecorrespondingobservationswereavailable.Finally,time180

seriesofseasonalaverages(JJA)weregeneratedformodeledtotalcolumnBrO,as181

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wellasforsatelliteobservationanduncertaintyoftotalcolumnBrO.182

183

3.Results/Discussion184

Here,weshowthatinclusionof5pptofCH3Brtorepresentthebrominefrom185

VSLSimpactsboththepresentseasonalevolutionoftheAntarcticozonelayerand186

itsrecoveryoverthe21stcentury.Thesimulatedpresentdayseasonalcycleof187

ozoneoverAntarcticacomparesbetterwithOMItotalcolumnozonemeasurements188

whentheVSLScontributionisincluded.Figure1showsthedailyaveragetotal189

columnozone(DU)amountsfrom60‐90°SfortheA12014_5Br(bluecurve)and190

A12014_0Br(redcurve)simulationsandfromOMIobservations(blackcurve),with191

bothobservationsandsimulationsaveragedover2005‐2015.Theadditional192

brominedecreasesozonebetween6‐20DU,withthelargestdeclineoccurringin193

September.Thefasteronsetoftheozoneholeformationandtheminimumozone194

amounts,around1Octoberareinbetteragreementwithobservationthanfound195

usingthesimulationwithoutVSLSbromine.GEOSCCMdoeshaveasomewhat196

delayedbreakupofthepolarvortex,whichisseenintheslowerozoneincrease197

duringNovemberandDecember.198

ItiswellknownthatozonedeepintheAntarcticpolarvortexbetween14‐18199

kmdropstonearzerolevels,typicallyinthelastweekofSeptemberandthefirst200

weekofOctober[Hofmannetal.,1997].Figure2showsthedailyozonepartial201

pressure(millipascals)at80°SforthesimulationsA12014_5BrandA12014_0Br,202

andMLSozonefrom1Septemberto30October,allaveragedover2005‐2009.The203

simulationincludingVSLSbromineismuchclosertotheverylowabundanceof204

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ozoneobservedfromMLSandtheSouthPoleozonesonderecordinthelower205

stratosphere,withthenearzerovaluesroutinelyreachedduringthemid‐late1990s206

andearly2000s.ThesenearzerovaluesarenotseentheA12014_0Brsimulation.207

Theozoneprofiledifference(%)betweenthesetwosimulationsandMLS208

observationsover60to82°S,forafewselectdayssurroundingtheozoneminimum,209

isshowninFigureS1.Thiscomparisonalsoshowsimprovedagreementbetween210

pressuresof200to10hPawhentheVSLSsourceof5pptofbromineisincluded.211

OctoberaverageAntarctictotalcolumnozoneisthecommonlyusedmeasure212

ofozonedepletionandrecoveryinWMOOzoneAssessmentsandtheSPARC213

CCMVal‐2Report(SPARCCCMVal,2010).Figure3showstheOctoberaveragetotal214

columnozone(DU)over60‐90°Sfrom1960‐2099forourtwosimulations.The215

A12014_5BrsimulationshowsalmostadecadelaterrecoveryofAntarcticpolar216

ozoneto1980levels.Asexpected,thelargestozonedifferencesbetweenthesetwo217

simulationsoccurwhenchlorineloadinglevelsarewithin50%ofthemaximum.218

GEOSCCMOctobertotalcolumnozonereturnsto1980levelsbyapproximately219

2062intheA12014_0Brsimulationandaround2071intheA12014_5Brsimulation.220

Thesesimulationsrepresentapairofruns,thedifferencebetweenthesetwo221

simulationscouldbeamplifiedofdampedbynaturalinternalvariability.However,222

therecoverydateisalsodelayedbyoveradecadeforthefourmodelsthatincluded223

VSLSbromineforthe2014assessmentbutnotfor2010.Therefore,weexpectthat224

thesignificantdifferencebetweenourpairofsimulationswouldpersistover225

multipleensemblemembers.Thislaterrecoverydateisnowsimilartotheestimate226

fromaparametricmodel[Newmanetal.,2006]usingavailabledataatthetimeand227

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resolvesadiscrepancybetweenitandrecoveryestimatesfrompreviousWMO228

Assessments[2011].229

ComparisonsoftotalcolumnBrOretrievedfromtheOMIinstrumentwith230

simulatedBrOcolumnssupportsinclusionofacontributionofVSLS,similarto231

resultsobtainedbySalawitchetal.[2010]andLiangetal.[2014].FigureS2shows232

totalcolumnBrOfromOMIaveragedoverthemonthsofJunetoAugust,for60to233

90°S,fortheyears2005to2015comparedtoGEOSCCMsimulationsforthesame234

months,latituderange,andyear.Inclusionoftheextra5pptofbrominereduces,235

butdoesnotcompletelyeliminate,asystematiclowbiasbetweensimulatedand236

observedcolumnBrO.EnhancedtroposphericBrOfromsurfacereleaseisnot237

includedinourGEOSCCMsimulations,whichcouldaccountforthelowbiasin238

modeledBrO.Roscoeetal.[2014]showsurfacereleaseofbrominetypically239

contributesbetween1and31013molcm2oftroposphericBrO,distributed240

throughoutthefreetroposphere,atHalleyBay(75.6°S).Anotherpossibilityforthe241

underestimateofcolumnBrOcouldbemodelmisrepresentationoftheBrO/Bryin242

thetroposphere.Ontheotherhand,theactualcontributionfromVSLSto243

stratosphericBrycouldbelargerthan5ppt.TheresultspresentedinFigureS2are244

consistentwithestimatesofatleast5pptofbrominebeingsuppliedbyVSLS245

[Salawitchetal.,2005;Dorfetal.,2008;Theysetal.,2007;Salawitchetal.,2010;246

Parrellaetal.,2013,Liangetal.,2014].247

TimeseriesofBrO,BrCl,andOClOat50hPafromthetwoGEOSCCM248

simulations,averagedover60‐90°SduringAug.‐OctareshowninFigureS3.Neither249

BrO,BrCl,norOClOreturntotheirrespective1980levelsbytheendofthe250

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simulations.ThetimeseriesofOClObehavesinasimilarmannertoBrOandBrCl251

becausetheabundanceofOClOinthepolarvortexismuchmoresensitivetoBrO252

thanClO[Salawitchetal.,1988].Thedifferencebetweenthetwosimulationsgrows253

largerwithtime,reflectingamuchlargerroleforozonelossduetotheBrO+ClO254

cycleinA12014_5BrthantheA12014_0Brsimulationduringthelatterpartofthis255

century.Together,Figures3,S2,andS3showthatincludingallthesourcesof256

stratosphericbrominecausesaboutadecadedelayintherecoveryoftheAntarctic257

ozonehole.258

IncludingsupplyofstratosphericbrominefromVSLSreducesozonecolumns259

nearlyeverywhereinthemodel,withthesmallestchangesinthetropicsandthe260

largestdecreasesoverthehighlatitudesduringspring(Figure4).Theeffectofthis261

extrabromineislargestduringthetimeperiodofpeakchlorine(1990–2019).For262

thisthree‐decadeperiod,inclusionofBryfromVSLSdecreasestotalcolumnozone263

by16‐22DUoverAntarcticaduringSeptember.IntheNorthernHemispherehigh264

latitudes,ozoneisreducedby10‐20DUduringMarch.Thetropicaltotalcolumn265

ozonedecreaseistypicallylessthan2DU.Thisthree‐decadetimeperiodalso266

includestheeruptionofMt.PinatuboinJune1991,shortlyafterwhichozoneloss267

duetobrominewaslargerintheA1204_5Brsimulation.However,theenhanced268

ozonelossfollowingtheeruptionofMtPinatubofollowstheaerosollifetimeinthe269

stratosphereof1‐3yearsanddoesnotsignificantlyimpactthe30‐yearaverage270

response.271

272

4.Conclusions273

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Inclusionof5pptofstratosphericbrominetorepresentVSLSinGEOSCCM274

resultsinbetteragreementwithOMImeasurementoftotalcolumnBrOandcauses275

severalimportantchangesinthesimulationoftheseasonalevolutionandrecovery276

overthe21stcenturyofAntarcticozone.AhighbiasinsimulatedSHpolartotal277

columnozonewithrespecttoOMIobservationscollectedover2005to2015is278

significantlyreduced.IncludingVSLSbrominecausestheminimumseasonalozone279

columntooccuraboutaweekearlier,incloseragreementwithOMIobservations.280

TheverylowtonearzeroozoneconcentrationsobservedinthedeepAntarctic281

lowerstratosphericpolarvortexduringlateSeptemberintoearlyOctoberduring282

themid‐late1990sandintotheearly2000sareonlysimulatedwhentheVSLS283

brominesourceisincluded.284

AccordingtoourGEOSCCMsimulations,recoveryofAntarcticozoneis285

delayedbyaboutadecadeuponincludingtheVSLScontributiontostratospheric286

bromine.OctoberAntarcticozonecolumnsareprojectedtoreturnto1980levels287

around2071,incloseagreementwitharecoveryyearof2068basedonan288

empirical,parametricmodel[Newmanetal.,2006].The2010WMOAssessment289

[WMO,2011]attributedanearlierrecoveryyearof~2051,providedbysimulations290

from17CCMs,tometeorologicalanddynamicaleffectsofGHGsonAntarcticozone291

thatwerenotconsideredintheparametricmodel.However,mostoftheCCM292

simulationsusedinWMO[2011]neglectedVSLSbromineandWMO[2014]showed293

themeteorologicalanddynamicaleffectsofGHGsonAntarcticozonerecoverywas294

small.Theseresultsshowthataconstantadditionof5pptofbrominecausealmost295

adecadelaterrecoveryofAntarcticozoneandsuggestthatanyfuturegrowthor296

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newemissionsofbrominecontainingcompounds,aslowasacoupleppt,could297

significantlyimpacttheprojectedozonerecoverydate.Ourstudyalsosuggests298

modelsestimatesofpolarozonerecoveryforthenextAssessmentshouldincludea299

realistictreatmentoftheVSLScontributiontostratosphericbromine.Ifbromine300

fromVSLSareneglected,recoverydateswillbebiasedearlybyperhapsasmuchas301

adecade.302

303

Acknowledgements304

We thank the NASA ACMAP, Aura, and MAP program for supporting this305

research. We would like to thank two anonymous reviewers for their helpful306

commentsandsuggestiontoimprovethismanuscript.Wealsothankthoseinvolved307

in model development at GSFC, and high‐performance computing resources308

providedbyNASA’sAdvancedSupercomputing(NAS)DivisionandtheNASACenter309

forClimateSimulation(NCCS).Alldataandmodeloutputusedinthesefigureswill310

beavailablewiththe linktothispublicationat theGEOSCCMwebsite(http://acd‐311

ext.gsfc.nasa.gov/Projects/GEOSCCM/), additional information is available by312

contactingthecorrespondingauthor([email protected]).313

314

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Figures455456457458

459460Figure1.Thedailyaveragetotalcolumnozone(DU)between60‐90Sfor2005‐4612015.ThebluecurveshowstheA12014_5Brsimulation,theredcurveisthe462A12014_0Brsimulation,andtheblackcurveistheOMIobservation.Adashedblack463lineshows1October.464465

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466467Figure2.Dailyozonepartialpressure(millipascals)at80°Sfora)A12014_5Br,b)468A12014_0Br,andc)MLSmeasurementsfrom1Septemberto30Octoberaveraged469over2005‐2009.Thecontourintervalis0.25between0and1and0.5between1470and3and1above3.471472

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473474475Figure3.TheOctoberaveragetotalcolumnozone(DU)between60‐90Sfrom1960476to2099.Thebluecurvesshowtheindividualyearvalues(thin)andlowpass477filteredvalues(thick)forthesimulationwithanextra5pptofbromine.Thered478curvesshowtheindividualyearvalues(thin)andlowpassfilteredvalues(thick)for479thesimulationwithoutarepresentationofbrominefromVSLS.Theverticaldashed480redandblacklinesrepresentthereturnto1980levelsusingthesmoothedcurves481withouttheextraBrandthesimulationwiththeextraBr.482 483

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484Figure4.Thelatitudebymonthtotalcolumnozone(DU)fortheA12014_5Br(top485panel)andA12014_0Br(middlepanel)simulationsaverageover1990‐2019.The486bottompanelshowsthedifferenceintotalcolumnozone(DU)betweenthetwo487simulations.488489