JOURNAL OF GEOPHYSICAL RESEARCH, VOL. 106, NO. D23, PAGES 32,503-32,525,DECEMBER 16, 2001 Ozone in the Pacific tropical troposphere from ozonesonde observations Samuel J.Oltmans, 1BryanJ.Johnson, 1Joyce M. Harris, • HolgerV6mel, •'2AnneM. Thompson, 3Kanatathu Koshy, 4Patrick Simon, 5Richard J.Bendura, 6Jennifer A. Logan, ? FumioHasebe, 8Masato Shiotani, 9VolkerW.J.H.Kirchhoff, •øMatakite Maata, 4Gopal Sami, 4AnsariSamad, 4JiojiTabuadravu, 4Humberto Enriquez, TM MarioAgama, •2Jaime Cornejo, •: andFrancisco Paredes • Abstract. Ozoneverticalprofile measurements obtainedfrom ozonesondes flown at Fiji, Samoa,Tahiti, andthe Galapagosare usedto characterizeozonein the troposphereover the tropicalPacific. Thereis a significantseasonalvariationat eachof thesesites. At sitesin both the easternand westernPacific, ozonemixing ratiosare greatestat almostall levels in the troposphere duringthe September-November seasonand smallestduringMarch-May. The verticalprofile hasa relative maximumat all of the sitesin the midtroposphere throughoutthe year (the largestamountsare usuallyfound near the tropopause).This maximum is particularly pronouncedduringthe September-November season.On average,throughoutthe troposphere, the Galapagoshaslargerozoneamountsthanthe westernPacific sites. A trajectoryclimatology is usedto identify the major flow regimesthat are associatedwith the characteristicozone behaviorat variousaltitudesand seasons.The enhancedozoneseenin the midtroposphere duringSeptember-November is associatedwith flow from the continents.In the westernPacific this flow is usuallyfrom southernAfrica (although10-daytrajectoriesdo not alwaysreachthe continent)but also may come from Australiaand Indonesia. In the Galapagosthe ozonepeak in the midtroposphere is seenin flow from the SouthAmericancontinentandparticularlyfrom northernBrazil. High ozoneconcentrations within potentialsourceregionsand flow characteristicsassociatedwith the ozone mixing ratio peaksseenin both the westernand easternPacific suggestthat theseenhancedozone mixing ratiosresult from biomassburning. In the upper troposphere,low ozone amountsare seenwith flow that originatesin the convectivewestern Pacific. 1. Introduction The tropicalPacific is often consideredto be a regionremote from major polluting influences becauseof its isolation from heavilyindustrializedlandmasses.Recentfield campaigns[Hoell et al., 1999] have emphasizedthat though this is often the case, •Climate Monitoring andDiagnostics Laboratory, NOAA,Boulder, Colorado. 2Cooperative Institute forResearch intheEnvironmental Sciences, the signatureof pollution, particularly from biomassburning, makes a significantimprint on the air chemistryof the region [Singhet al., 2000]. In a numberof instances, layersof enhanced ozone (mixing ratios >80 ppbv) were found in the midtroposphere in the remotewesternPacific [Stolleret al., 1999]. Theselayersin additionto havingenhancedozonewere replete with markers of biomass burning such as carbon monoxide, ethane,ethyne, and notably methyl chloride [Gregory et al., 1999]. Beginning in August1995as partof the PacificExploratory Mission(PEM) TropicsA, ozoneverticalprofilemeasurements 3NASA Goddard Space FlightCenter, Greenbelt, Maryland. 4School ofPureandApplied Sciences, University oftheSouth Pacific, werebegunat PagoPago,AmericanSamoa(14.3øS,170.6øW), Suva, Fiji. andPapeete, Tahiti(18.0øS,149.0øW).At Samoa,profileswere 5MeteoFrance, Papeete, Tahiti,French Polynesia. also obtained as part of an earliermeasurement programfrom 6NASA Langley Research Center, Hampton, Virginia. 1986to 1989. Theseearlierprofilesprovidean opportunity for 7Department ofEarthandPlanetary Sciences, Harvard University, Cambridge,Massachusetts. comparison with measurements duringthe morerecentperiod. 8Department ofEnvironmental Sciences, Ibaraki University, Mito, Profile measurements were continued at Tahiti and Samoa Japan. through PEM TropicsB withtheprogramat Tahiticompleted in 9Graduate School of Environmental EarthScience, Hokkaido December 1999. At Samoa,weeklysoundings continue aspart University,Sapporo,Japan. løInstituto dePequisas Espaciasis, SaoJose dosCampos, Brazil. of theSouthern Hemisphere AdditionalOzonesondes (SHADOZ) •llnstituto Nacional deMeteorologia y Hidroligia, Quito,Ecuador. project (A.M. Thompson et al., The 1998-2000 SHADOZ •2Instituto Nacional deMeteorologia y Hidroligia, SanCfistobal, (Southern Hemisphere AdditionalOzonesondes) tropicalozone Galapagos,Ecuador. Universityof Colorado,Boulder,Colorado. Copyright 2001bytheAmerican Geophysical Union. Papernumber2000JD900834. 0148-0227/01/2000JD900834509.00 climatology: Seasonal patterns, the zonal wave-one, and comparisonwith TOMS and ground-basedmeasurements, submittedto Journalof GeophysicalResearch,2001, hereinafter referredto as A.M. Thompson et al., submitted manuscript, 2001). Duringmostof themeasurement period,soundings were 32,503 32,504 OLTMANS ET AL.' OZONE IN THE PACIFIC TROPICAL TROPOSPHERE i ! [ i t I i i .d. dl, -, , , J i i i i i r ! 4 Sep-Oct-Nov o 0 100 0 25 50 O0 75 OZONEM•XINGRATIO(PPBV) Figure1. Theaverage ozone profileandvariability for0.25kmlayers atTahitifortwoseasons (a)March-May and (b) September-November fortheperiod1995-1999. Themedian is thevertical lineinside thebox,andthebox represents theinner50thpercentile ofthedata.The"whiskers" represent theinner90thpercentile ofthedata.The solid diamond is the mean. of PEM TropicsB. As part of the Soundings of doneweekly. Duringthe aircraftfield campaigns in September- anticipation October1996 (PEM TropicsA) and March-April1999 (PEM Ozone and Water Vapor in the EquatorialRegion (SOWER) were startedon a campaign Tropics B) soundings weredonetwicea week.In January 1997, projectozoneprofile measurements weeklysoundings werebegunat Suva,Fiji (18.1øS,178.2øE) in basisin March 1998 at SanCristobal,Galapagos(0.9øS,89.6øW), i I I I • i , , t i i i • , .a. , i ..• , I o_ I • ,, • , . I IVlar-Apr-May o O0 0 1O0 OZONEMIXING •TIO(PP•) Figure2. Theaverage ozone profileandvariability for0.25-km layers atGalapagos fortwoseasons (a)MarchMay and(b) September-November for theperiod1998-2000. OLTMANS ET AL.' OZONE IN THE PACIFIC TROPICAL TROPOSPHERE 32,505 96 15 90 84 78 72 66 6O 54 48 42 36 30 24 18 12 6 0 ppb J F M A M J J A S 0 N D Month Plate 1. Time-height crosssectionof ozone mixing ratio at Pago Pago, American Samoa (14.3øE, 170.6øW), for 1996. Soundingsare weekly except during the Pacific Exploratory Mission (PEM) Tropics A intensive measurement periodfrom August-September when soundingswere donetwice weekly. 96 15 9O 84 78 72 66 60 54 48 42 36 3O 24 18 12 o ppb J F M A M J J A S 0 N D Month Plate 2. Time-heightcrosssectionof ozonemixingratio from weeklysoundings at San Cristobal,Galapagos (0.9øS, 89.6øW) for 1999. 32,506 OLTMANS ET AL.: OZONE IN THE PACIFIC TROPICAL TROPOSPHERE i . -- I i lOO Figure3. The averageozoneprofileandvariabilityfor 0.25-kmlayersat Samoafor two seasons (a) March-May and(b) September-November for the period1995-2000. were increasedto biweekly soundingsin September1998 and to throughoutthe troposphereof the tropical Pacific that has not weeklysoundings aspartof SHADOZ earlyin 1999. Soundings been available in the past. In particular, new insights on the continueat Fiji and the Galapagosin 2000 as part of SHADOZ short-termand seasonalvariability of ozonein this regionas well and SOWER. as differences between the eastern and western Pacific are This set of ozone profiles obtained using balloon-borne revealedin thesedata. In addition, isentropictrajectoriesare used ozonesondesprovides information on the distributionof ozone to look at the transport associatedwith particular features of i II I id, I i I I 4[' I • t.____•. i dl,_dl , i .I I P i L [ i --• ! i•lI' t I I i iI , i i---i.. , i I •-"..., •' • •. o_ • i r' i I i , i , i 1• ß • • i t i •' i & ,• i , i i , ,• , i • i , ,• •'" I i i •, • • i I i I ß • ,, i _ , i • i iI ar-apr-ay : Sep-Oct-Nov o 0 100 0 ' oZoN[ U•X•NG•0(•) Figure 4. The averageozoneprofile and variabilityfor 0.25-km layersat Fiji for two seasons(a) March-May and (b) September-November for the period 1997-2000. OLTMANS ET AL.' OZONE IN THE PACIFIC TROPICAL TROPOSPHERE 32,507 individual profiles and also at the influence of climatological ozonesondepump efficiency measurementsand sensitivitytests transport patterns on the principal features of the ozone of buffered and unbuffered sensor solutions, submitted to Journal of GeophysicalResearch,2001) at all of the sitesexcept distributionin the tropicaltroposphere in this region. the Galapagos where the new recipe was used /¾om the beginning. From comparisonflights made at these sites, as well 2. Methods as laboratorytests,an empirical correctionhas been derived, and 2.1. Ozonesondes the earlier data have been correctedusing this relationship. This The ozone vertical profiles were obtained using the correction is largest in the stratosphere.It leaves values for the electrochemical concentrationcell (ECC) ozonesonde[Komhyret earlier data at the surface unchangedand reduces amountsby al., 1995]. This has becomea standardtechniquefor obtaining -2% at 100 hPa. Data placed in the Global Troposphere ozone profiles with high vertical resolution in both the Experiment (GTE) archive /'or PEM Tropics at NASA Langley troposphere and stratosphereto altitudes of-35 km. The andin the SHADOZ archivehave this correctionapplied. measurementsof ozone have an accuracyof _+5%through most of the tropospherewith somewhatmore uncertainty(_+10%)/br very low mixing ratios (<10 ppbv) encounteredoccasionallyin the tropics. The only important interrelent in the measurement technique,which is basedon the oxidationreactionof ozonewith potassiumiodide in solution, is sulfur dioxide that is not 2.2. Trajectories For the purposes of characterizing the tropospheric airflow patterns influencing transport to the tropical sites, insentropic trajectorieshave been calculated. The trajectoriesare computed from the EuropeanCentre for Medium-RangeWeather Forecasts encountered at these sites at sufficient concentrations to be of (ECMWF) analysesusing the model describedby Harris and significance. One exceptionis the presenceof a layer of zero Kahl [1994]. The limitations in such trajectories must be ozonemeasuredat the Galapagosin a singleprofile shortlyafter recognizedin interpretingthe resultsthat are obtained,but they a volcaniceruption in Ecuador. The data were obtainedwith an do provide a useful tool for obtaining a picture of the flow altitude resolutionof-50 m but for the analysisperformedhere patternsthat may influence ozone behavior at these sites. In were averaged into 250-m layers. Only at Samoa are total particular for this work the role of convection needs to be column ozone measurements from a collocated Dobson consideredas a possible influence on the air parcel path. For spectrophotometer available for comparisonwith the integrated individual trajectory paths the outgoing longwave radiation total ozone from the ozonesonde. These comparisonsgive an (OLR) maps available from the NOAA-CIRES Climate average ratio of i.04 +_0.05 between the Dobson total ozone Diagnostics Center, Boulder, Colorado, Web site measurementand the integratedtotal ozone from the ozonesonde, (http://www.cdc.noaa.gov/HistData/), that are constructedfrom giving confidencethat the ozonesondemeasuredozone amounts NCEP operationalOLR data, were inspected/'oreach of the 10 from all of the sitescan be comparedwith each other. During the days to see if low OLR values indicative of convection were courseof the measurementprogram a change was made in early found at the air parcel location. The computedtrajectoriesare 1998 in the sensing solution recipe (B.J. Johnsonet al., ECC used both to investigateindividual cases and by grouping the • . a, FI -- ....... •r "•.. '-••..• I [ --, _77•%• ....... i _ •••d•=-• •.e;., ..... - 7 -' , •_ - _ •' ß 1995-2000 (•as•) Mar-Apr-May o o 1oo o 1oo OZONE•IXlNO •TIO(PP•) Figure5. Comparison oftheozonemixingratioprofiles atSamoa fortheperiods 1986-1989 and1995-2000 for(a) March-May and (b) September-November. 32,508 OLTMANS "- i ET AL.: OZONE IN THE PACIFIC '- TROPOSPHERE J _- - 7- *---- •-• •.-• TROPICAL , =1= _-• - - -, ,&.-Tc•=•--; •,'• . , .... , , i I i - • .... , 4• Samoa(solid) .... ß Galapagos(dashed) -' 0 Mar-Apr-May s'o OZONEM•X•N0RAT•O(PPm') Sep-Oct-Nov 0 o ' •'•F-•-••1 OZONEMIXINGRATIO(PPBV) Figure6. Comparison of theozonemixingratioprofilesat Samoa(1995-2000)andtheGalapagos (1998-2000)for (a) March-May and (b) September-November. trajectoriesusing an objective clustering technique [Moody, 1986; Harris and Kahl, 1990] that gives an indicationof the primary flow regimesinfluencinga particularlocationat a given altitude. The trajectoriesare computedtwice daily (0000 and 1200 UT) for 10 days backward in time. During 10 days of travel,air parcelsmay have undergonediabaticprocesses that are percentileof the data. The whiskers representthe inner 90th percentile of the data. The solid diamond is the mean. The September-Novemberperiod has greatly enhanced variability especiallyin the 2-10 km layer when comparedto the MarchMay period. These seasonalprofiles are basedon severalyears of data and representthe variability that is primarily contributed not accounted for in the model used here, and these are an by the short-termfluctuationswithin a season. In the Galapagosthe time-height crosssectionfor 1999 (Plate important contribution to the uncertainty in the computed pathwayof the air parcel [Merrill, 1996]. Transportfrom sources 2), the only completeyear available for this site, showsmany of or sinksmore than 10 daystravel time from a particularsite could the samefeaturesseen at Samoa.The seasonalprofiles for the also have a significantinfluence on ozone levels measuredat the Galapagos (Figure 2) show similar behavior to Tahiti with a site. maximum in the variability in September-Novemberand a minimum in the March-May season.The variability is greaterat 3. Day-to-Day Variations Tahiti in September-Novemberthan it is in the Galapagos.At Samoa(Figure 3) the variability in September-November is also Variationson a timescaleof severaldaysare a largesourceof the variabilityseenin tropospheric ozoneat thePacifictropical larger than at the Galapagosbut not quite as large as at Tahiti. sitesstudiedhereas will be shownin the analysisin this section. Since Fiji (Figure 4) also showsgreater variability than that of Thesevariationshavebeenstudiedusingsurfaceobservations at the Galapagosduring this September-November,this feature is likely a real differencebetweenthe easternand westernPacific. Samoa [Harris and Oltmans, 1998]. The surfacevariationswere foundto resultfrom changesin airflow to the sitethat tapped differentsources andsinks.Duringall seasons, air comingfrom 4. Seasonal Variation higher latitudesand altitudeshas -50% more ozone than air with a tropicalorigin [Harris and Oltmans,1998]. Althoughthe As canbe seenin Figures1 - 4, notonlyis thevariability of ozonesoundings are doneon an approximately weeklyschedule ozonein thetroposphere greaterin September-November thanin compared to the continuous observationsat the surface, the March-May, but also the mean (and the median)valuesare variabilityfromsounding-to-sounding captured in thetime-height greateras well. Time-heightcrosssections basedon 14-day crosssectionof ozonemixing ratio for 1996 at Samoa(Plate 1) is averagesover the entire recordof measurements (which varies also apparent.During 1996 at Samoathe soundingswere done somewhat foreachsite)areshownin Plate3. Although thereare twicea weekduringAugustandSeptember sothatthevariability unique featuresat each site, a pattern is discernablethat is is well represented duringthis time of the year.This can alsobe reflected at all sites.In thewesternPacific,thereis a prominent seenin the plot of the averageprofilesat 0.25-km incrementsfor layerof enhanced ozonein themidtroposphere in September and individualseasons at Tahiti (Figure1). The medianis the vertical October. Therealsoseems to bea distinct pulsein JuneandJuly line insideof the box, and the box represents the inner 50th of somewhatsmallermagnitudewith a relativeminimumin late OLTMANS ET AL.: OZONE IN THE PACIFIC TROPICAL TROPOSPHERE 32,509 0 0 ..,-• 0 0 • ß 4-o 0 U3 0 U3 0 •Z3 0 ,._ .- U3 ...., 0 ._ [m•] opn•:•lV [Ua>l]opnl,llV E• '"" 0 0 • • o o [tull oPn11•,IV [m>[] oPn•I!:IIV • 0 :• O 32,510 OLTMANS ET AL.: OZONE IN THE PACIFIC TROPICAL TROPOSPHERE B 0ou , 0ø ' •- .-• ' •",,, • - • 1• 30os •_ 234X • 523 % 3 60os - 10øE 40øE 70øE 100øE 130øE 160øE 170øW 140øVV 110øVV 80øW Longitude ß ,. 30ON -• 30os _ 60øS-• 3 • 10øE 40øE • 70øE • • • • 100øE 130øE 160øE 170øW • 140øW 110øW 80øW Longitude Figure7. Clusters of trajectories arrivingat Tahitiat 1 km for (a) December-February and(b) SeptemberNovember for theperiod1990-1999.Theclusters arenumbered 1-6,andthepercentage of thetotalnumber of trajectories in eachclusteris alsoshown. JulyandAugust.Associated withthisJune-July enhancement in 1986-1990periodhas somewhatmoreozonethan in the 1995the midtroposphere, ozonein the boundarylayeralsoincreases, 2000 periodthat appearsto be drivenby severalprofileswith and this producesa seasonalmaximumnear the surfacethat greater ozone amounts,particularlyin the low and mid(Figure5a). In September-November, however,the occursearlier than the peak in the midtroposphere.During troposphere amountsand variabilityare very similarduringthe two periods (Figure5b). In the Galapagosthe generalpictureis similarto the western stratosphere. In January-May, ozone at all altitudes is almost alwayslessthan at a correspondingaltitude during the rest of the Pacificsites(Figure6), but with someimportantdifferences.The ozonemaximumoccursearlierin the year and year. Also, at this time of year, ozone in the upper troposphere midtropospheric australwinter and spring, greaterozone amountsdescendto -10-12 km. This seems to be associated with ozone in the lower has smaller mixing ratios, approachingthose seenat the surface which are almostalwaysquite small (<15 ppbv)in this season. An earlier set of profiles obtainedat Samoafrom August 1986 to January1990 (Figure 5) show similar characteristics to those seen in the more recent 5-year data set. For March-May the diminishes earlier as well (see Plate 3). Near the surface the seasonal variation is smaller. The most noticeable difference is the lack of very low mixing ratios in the middle and upper troposphere especiallyduringtheJanuary-May time of year.This is consistent with the fact that the western Pacific is a more OLTMANS ET AL.' OZONE IN THE PACIFIC TROPICAL 60ON•, o TROPOSPHERE . ..,• 32,511 •,. 30ON - '• 00 -- • 4 30os_ 60os - 0o 30OE 60øE 90øE 120øE 150øE 180Wø 150øW 120øW Longitude 60øN 0ON 0o 3005 60os - 0o 30OE 60øE 90øE 120øE 150øE 180Wø 150øW 120øW Longitude Figure8. Clustersof trajectories arrivingat Tahitiat 6 km for (a) March-Mayand(b) September-November for 1990-1999. greatestinfluenceon this site. The following analysisshowsthat while the airflow patternsat the westernPacific sites are quite similar, they are much different from those in the Galapagos. similar to the differences between the eastern and western The differences in airflow direction with seasonare greatestin Pacific. It is also clear that in the Galapagosozone amountsare the boundary layer. Wind shear at all altitudes is somewhat greater than in the western Pacific above 4 km in September- greaterin the Galapagosthan in the westernPacific. To carry out this analysis,a 10-year climatology of 10-day back trajectories November and above 5 km in March-May. wascomputedat threelevels(1, 6, and 13 km) for all four of the sitestbr each of four seasons. These trajectorieswere grouped 5. Flow Characteristics convectiveregionwhereboundarylayer air can be mixed into the uppertroposphere.Other than this noticeablelack of low ozone amounts the differences among the western Pacific sites are into six clusters at each site for each altitude. The choice of six Although the seasonalozone behavior at all of the sites has clusterswas somewhatarbitrary, but it has been found that six some common featuressuch as the maximum during the austral clusters usually gives sufficient transport detail while not spring(September-November),this doesnot by itself imply that producing a cluttered figure or redundant transport types. of variousregimesare discussedhere the sourcesand sinksinfluencingthe measuredozone at the sites Examplesrepresentative are the same. For example, the proximity of the Galapagosto (Figures7-12). Becauseof the similarityin flow patternsat the westernPacific South America suggeststhat this continentis likely to have the 32,512 OLTMANS ET AL.' OZONE IN THE PACIFIC TROPICAL TROPOSPHERE 60øN -• 30ON - 00 -- 3005 - 60os - 0o 30OE 60øE 90øE 120øE 150øE 180Wø 150øW Longitude Figure9. Clusters oftrajectories arriving atTahitiat13kmforallseasons for1990-1999. comingfromthe southandwestduringJunesitesthe description of the behaviorat Tahiti is usedto indicate 65% of trajectories the westernpatternwith some differencest¾omthe other sites August,while at Tahiti andSamoathe percentage of southerly noted. At 1 km, a level in the marine boundarylayer, the largest flow is closerto 30% (Figure7b). At 6 km above Tahiti airflow (Figure 8) is more uniformly seasonalcontrastis betweenDecember-February(Figure7a) and t¾om the westcomparedwith low altitudeflow, with only-20% June-August (Figure7b). Thesearetheseasons of minimumand maximum surfaceozone at Samoa [Harris and Oltmans, 1998]. comingfrom the easton an annualbasis. Thereis a southerly During the australsummer(December-February) flow at the 1-km level is predominantly from the tropicalPacificfor all of the sites in the western Pacific. In the other seasons, 15-65% of the flow is from the west and more southerlylatitudeswith the component to the airflow,butit usuallydoesnotextendsouthof 40øSwithin 10 days,in contrastto the low-levelflow thatreaches muchhigherlatitudes.Throughout the australwinterandspring (June-November),at least 25% of the trajectoriesarriving at largestpercentage of flow from the southoccurringin austral Tahiti come from as far west as the mid Indian Ocean and -10% winter. At Fiji (not shown)this featureis mostprominentwith reachsouthernAfrica (Figure 8b) within 10 days. To Fiji the 40øN -I 20ON - ,_--T/2 25%\ 10o5 - ) 2,•k 4005 l:.IOoW 100øW 70øW 40øW 10øW Longitude Figure 10. Clustersof trajectories arrivingat theGalapagos at 1 km for all seasons for 1990-1999. OLTMANS ET AL.' OZONE IN THE PACIFIC TROPICAL TROPOSPHERE 32,513 60ON - 30ON - 0o - 30o5 - 60o5 - 16001:: 170ow 140øW 110øW 80øW 50øW 20W ø Longitude 30øN • 0ø 3005 60os 160øE 170øW 140øW 110øW 80øW 50øW 20W ø Longitude Figure11. Clusters of trajectories arrivingat theGalapagos at 6 km for (a) December-February and(b) JuneAugustfor 1990-1999. flow is even more vigorous from the west and -5% of the seasons. There is some variation with season(not shown) with trajectories comefromSouthAmerica.A numberof trajectories December-Mayshowing10-15% of the trajectoriescomingfrom also have their 10-day originsover northernAustralia. In the summer,flow is less vigorousand some trajectorieshave a northerlycomponent. In theuppertroposphere (13 kin), flow is from the west,but a the Atlantic. In June-Novemberthe flow is exclusivelyfrom the south,often paralleling the South American coast. The flow at 6 km is in strong contrastto that in the boundarylayer. On an annualbasis,75% of the trajectoriesarrive at San Cristobalfrom majorityof the trajectories also have a northerlycomponent the east and have passedover the South American continentin (Figure9). This northerlyflow bringsair fromnearor evennorth the previous10 days. In December-February (Figure 1l a), -10% of the equatorand is strongest in September-November but is of trajectoriesarrive from the tropical northPacific, another10% presentin otherseasons as well. As in the midtroposphere, a from the tropical south Pacific, and the remainder from the east significantnumber of the trajectoriescome from the Indian off continentalSouthAmerica. During June-August(Figure 1lb) Ocean and Africa. and continuingthrough November (not shown), -10-15% of the The flow patterns in the Galapagos differsignificantly from flow is from the tropical south Pacific with the remainderfrom thosein thewestern Pacific.At thelowestlevel(Figure10)the the eastor with little movement(cluster3 in Figure 1lb). At 13 flow is overwhelminglyt¾omthe southand over the oceanin all km (Figure 12) the flow is about equally divided betweenweak 32,514 OLTMANS ET AL.' OZONE IN THE PACIFIC TROPICAL TROPOSPHERE 60oS - 90øE 120øE 150øE 180ø 150øW 120øW 90Wø 60øW 30øW Longitude Figure12. Clusters oftrajectories arriving attheGalapagos at 13kmforallseasons for1990-1999. flow from the eastor northeastand vigorousflow from the west. mixingratioof 105 ppbvat 5-6 km hasa trajectory(Figure14) There is a fairly strong seasonalitywith December-May that reaches back to southern Africa 10 days prior to the in thetropicalPacific,thelayer dominated by trajectories arrivingfromthe west,but abouthalf sounding.As with all soundings between the trajectories duringJune-November comefrom the eastand of enhancedozoneis alsomarkedby a large depression thefrostpointandambientair temperatures, indicative of dryair. northeast. 6. Discussion TEMPERATURE & FROST POINT (C) In the previoussectionsthe short-termand seasonalvariations -100 -80 -60 -40 -20 0 20 40 have been describedas well as the major air flow characteristics affectingthe ozonesondesitesin the westernand easterntropical Pacific. In this section,important featuresof the ozone profile 16 are linked to the trajectoriesto show how important sourceand sink regions for ozone may contribute to both the shorter-term 14 and seasonalvariations. Since the tropics are known to be a significantarea of biomassburning (see TRACE-A and SAFARI special sectionsof the Journal of GeophysicalResearch, 101, 1996), particular attentionis paid to characterizingthe possible influenceof burning on ozone at thesesitesby linking enhanced ozone layers with flow from potential sourceregions.It appears that several burning regions contribute to what is seen at these sites.The low ozonemixing ratios seenin the uppertroposphere at the westernPacific sitesalso are discussedbriefly. It is clearly seen in Plate 3 that there is a persistentlayer of enhancedozone in the midtropospherein the June-November season.The climatological trajectory analysis also shows this seasonto be one of regular occurrencesof flow from potential burning related sourceregions in southernAfrica and Australia for the westernlocationsand South America for the Galapagos. Several individual profiles are examined that contain enhanced 0 20 40 60 80 100 120 140 160 midtropospheric ozone along with the trajectoriescalculatedfor OZONE (ppbv) thesecases.An event of very high ozone seenat Fiji and Samoa Figure13. Ozonemixingratioprofileat Samoa onOctober 30, in November1997 is investigatedbecausethe flow path suggests 1998. The thicker solid line is the ozone mixing ratio. The an Indonesian source for the enhanced ozone. A profile with an enhanced midtropospheric layer characteristicof those seen during the Septemberand October periodin the westernPacific is shownin Figure 13 for a sounding done at Samoaon October30, 1998. The peak in the ozone dashedline is the air temperature andthe thinnersolidline the dew/frostpointtemperature.At temperatures above0øCthe moisture profileis withrespect to theliquidphaseof water(dew point)andbelowfreezingprofileis for the solidphase(frost point). OLTMANS ET AL.' OZONE IN THE PACIFIC 0o 30øE TROPICAL TROPOSPHERE 32,515 30ON - 00• 30os - 60os - Ef UJ 0 60øE 90øE 120øE 150øE 1800 Longitude 1 2 3 4 5 6 7 8 9 10 Days to Samoa Figure 14. Ten-day back trajectoryarriving at Samoaat 5 km at 0000 GMT on October30, 1998. The numbers alongthe trajectorypathmark the numberof daysbackin time from the endpointthat the air parcelwaslocated. The elevationchangeof the air parcelis shownin the bottom. This suggeststhat air with large ozone amounts is not simply litied from the surface at the source region and transportedto Samoa. The changein the temperaturelapse rate near 4 km at the bottomof the layer with enhancedozone suggeststhat the air has subsided and warmed in its transit to Samoa. A significant subsidenceof-3 km can be seen in the air parcel basedon the calculatedtrajectory(Figure 14). In orderfor a layer with sucha prominent ozone peak to be transported over the distances suggested by the trajectorycalculationit would likely have to remainrelativelyunmixed,both verticallyand horizontally,with air from surroundinglayers. The preservationof the layer as well as the validity of the trajectorycalculationis dependenton the air parcelnot passing througha region of strongconvection. Inspectionof the OLR TEMPERATURE& FROSTPOINT(C) TEMPERATURE& FROSTPOINT(C) -100 0 20 -80 40 -60 -40 -20 0 20 60 80 100 120 140 OZONE(ppbv) -100 40 160 0 20 -80 40 -60 -40 -20 0 20 60 80 100 120 140 40 160 OZONE(ppbv) Figure15. Ozonemixingratioprofilesat Samoaon (a) October2, 1997at 0000GMT and(b) October30, 1997,at 0000 and 1200 GMT. 32,516 OLTMANSET AL.:OZONEIN THEPACIFICTROPICAL TROPOSPHERE • 20os- 50os I 80øE I I 110øE I 170øE 140øE 160øW Longitude • 0 1 2 , , 4 5 6 l:)0øW ...• 7 8 9 10 Daysto Samoa 30ON o• lOON - 20oS - 50os I 120oE I 150oE I 180oE 150oW , 0 1 2 3 4 5 6 7 , 8 9 10 Days to Samoa Figure 16. Trajectories to Samoaat 5 km on (a) October2, 1997,at 0000GMT (solid)and12 GMT (dashed) and (b) October30, 1997, at 0000 GMT. maps for October20-30, 1998, showsthat indeedfor the period.Soundingsfrom Irene, SouthAfrica (25.9øS,28.2øE)were computed trajectory paththeair parcelis notlikelyto havebeen begunlate in November1998 so do not includethe periodof the stronglyinfluenced by convection.The otherneededingredient Samoasounding.Profilesfrom Irene in 1999 and 2000 from late in additionto a transport pathfor theappearance of theenhanced Octoberdo showozonelevelsof- 100 ppbv at altitudesbelow 10 ozone layer over Samoa is a sourceof such large ozone km (Thompsonand Witte 11999], and the SHADOZ archive at http://code916.gsfc.nasa. gov/Data_services/shadoz/). At La Reunion, Madagascar (21.1øS, 55.5øE) there is a profile earlier in Africa (the sourceregionsuggested by the trajectory)duringthis concentrations. No ozonesonde data are available from southern OLTMANS ET AL.' OZONE IN THE PACIFIC TROPICAL TEMPERATURE & FROST POINT (C) -100 -80 -60 -40 -20 0 20 TROPOSPHERE 32,517 derivedfrom TOMS total ozonemeasurements [Thompson and Hudson [1999] and the Web site http://metosrv2.umd.edu/ --tropo/)aroundOctober20, 1997,showhighlyelevatedozonein the regionto the north(0ø-15øS) of the areaindicated by the calculated trajectory.This techniquedoesnot producereliable troposphericdata at more southerlylatitudes. Given the somewhat uncertainnatureof the trajectorycalculationafter 10 40 18 days and the indication of enhancedozone amountsover southern Africa at this time year, it is reasonablethat Africa was the sourceof the layer of high ozoneconcentrations over Samoaseen in theOctober30, 1998, profile. Ozoneprofileswithpeaksgreaterthan-70 ppbv(Figure15) do not alwayshavetrajectories(Figure16) that extendbackto Africain 10 days,buttheyalwayshavepathsthathavea strong westerlycomponentso that 10-dayoriginsare to the west of Australiainto the Indian Ocean. On many occasions the trajectories passover Australia,usuallythroughthe middleor southernpart of the continent.The marked contrastthat can occur 0 20 40 60 80 100 120 140 160 OZONE (ppbv) Figure 17. Ozonemixingratio profileat Tahiti on October3l, 1995. duringa month(seeFigure 15) illustratesthe dominantrole that the airflow (Figure 16) to a site plays in the ozone profile, particularly during this season. For the profile obtained on October30, 1997 (Figure 15b), the 10-daytrajectory(Figure 16b) in the midtroposphere showslittle air movementfrom the vicinity of Samoaand mixing ratiosare 20-25 ppbv or lessthroughoutthe troposphere.This is in contrastto the near 80 ppbv mixing ratio seen at 5 km on October 2 (Figure 15a) when the flow was westerly(Figure 16a). the month with midtroposphericmixing ratios near 100 ppbv. This is somewhatearlier, however, than when the trajectory for the Samoa profile indicatesthat the air parcel would have been over southernAfrica. It is not unusualtbr La Reunion to see very large ozone enhancementsduring this time of the year that are often associatedwith biomass burning [Randriambelo et al., 1999, 2000]. Maps of tropicaltroposphericcolumnozone(TTO) FromFigure8 it is clearthata largefractionof the air parcels rcachingTahiti (and also Samoaand Fiji) passover Australia. From the data that are available from the ozonesondes and trajectories it is difficultto determine if trajectories thatpassover Australiaare influencedby burningin Australiaratherthanby burningin southernAfrica [Olson et al., 1999]. In somecases thetrajectories showthattheair movesmoreslowly(for example 30ON 10ON • 20øS - 50os • E I 140oE I 110oE I 140oE I 160oW 170oE ::': 4 Lu 0 1 2 5 4 5 6 7 8 9 Daysto Tahiti Figure 18. Trajectoryto Tahiti at 5 km on Novemberl, 1995, at 00 and 12 GMT. 10 32,518 OLTMANS ET AL.' OZONEIN THE PACIFICTROPICALTROPOSPHERE TEMPERATURE &FROST POINT (C) -100 -80 -60 -40 -20 0 TEMPERATURE &FRO•T POINT (C) 20 40 -100 -80 -60 -40 -20 0 18 20 40 16 14 12 • •o 6 4 2 0 0 20 40 60 80 100 120 140 160 0 20 40 OZONE(ppbv) 60 80 100 120 140 160 OZONE (ppbv) Figure 19.Ozone mixing ratio profile at(a)FijionNovember 19,1997, and(b)Samoa onNovember 20,1997. 30oN - 30ON - Samoa 10oN - lOoN - <t?' /'g 6 km ..• 20øS - .• 20øS- 50oS-- Nov. 20,1997 I 80oE 8 km I 110oE 140oE • ' Nov. 20,1997 50oS- I I I 170oE 160oW 130oW I 80OE I 110oE Longitude 140oE I I 170oE 160oW Longitude 30ON - 30ON - ß S'moa lOoN - lOoN , • 8km 10 km 20oS - :m 20os - 50os - Nov. 23,1997 • Nov. 21, 1997 I 80OE 110oE • . 50oS- I 140oE I 170oE I 160oW I 130oW Longitude 800E 110oE I 140OE I I 170oE 160oW Longitude Figure20. Trajectories to Samoa at6 kmonNovember 20, 1997,andat 10kmonNovember 21,1997,andtoFiji at 8 km on November 20, 1997, and November 23, 1997. OLTMANS ET AL.: OZONE IN THE PACIFIC •0 -60 -40 -20 0 20 TROPOSPHERE 32,519 ratherthansouthernAfrica). Althoughburningis knownto take placeduringthis time of year in northernAustralia[Olsonet al., 1999] there is not informationfrom ozone profilesfrom this regionto confirmthathighozoneis produced in theregionandin particularwhetherthe high ozoneamountsseenin the layer at TEMPERATURE & FROST POINT (C) -100 TROPICAL 40 Tahiti came from this source. In 1997, extensiveburningtook placein Indonesiaassociated withdroughtconditions thatwerea consequence of thestrongE1 Nifio. Ozoneprofile measurements [Fujiwara et al., 1999] and analysis of satellitedata[Thompson et al., 2001]foundveryhigh ozoneamountsin Indonesiaand Malaysiain connectionwith the burningin theregio_n_ On November19 and20 at Fiji andSamoa (Figure19) someof the highesttropospheric ozoneamountswere seenfor any event recordedat thesesites. These enhancements, which encompassed the entire troposphere abovethe two sites, increasedthe total tropospheric columnby -20 DU, or morethan 70% over averagevaluesfor the month. The trajectoriesshow thatat bothsitesair wascomingfromIndonesia(Figure20a-20d) 0 20 40 60 80 100 120 140 throughout thedepthof thetropospheric column.Althoughthese profiles were the only ones measuredduring the event, trajectories showthat a flow patternnearlyidenticalwith the one duringthislargeozoneenhancement persisted for -5 daysaround thetimethatthe profileswereobtained(Figure20d). Although Novemberwas not the peak in the burningover the Maritime 160 OZONE (ppbv) Continent,the presenceof large ozonecolumnamountsover the regioncanbe seenfrom the TI'O mapsfrom the period(Plate4) thatthetrajectories showair movingfromthisregiontowardFiji and Samoa. Given the large vertical extent of the ozone enhancement seenin the profile measurements andthe coherence of thetrajectorypathwith altitude,it appearsthata largeplume Figure21. Ozonemixingratioprofileat SamoaonFebruary 20, 1999. cluster3 in Figure 8b). An exampleof sucha caseis shownin the profile of October 31, 1995, at Tahiti (Figure 17). The correspondingtrajectory just reaches the York Peninsula of Australia (Figure 18) in 10 days. The indication of relatively slow transport,the large peak mixing ratio, and the thin vertical extent of the layer suggestthat the sourceof the elevated ozone seen at Tahiti may have been relatively nearby (i.e., Australia 20øN - / an area of enhanced column ozone amounts of-50 DU near the datelineandextendingfrom -7øS to15øSthatlasted-10 days. c• lOON' • of air with high ozone concentrationslid southeastward from the MaritimeContinent regionoverFiji andSamoa.TheTTO maps at thetimeof theprofilesfromSamoaandFiji showveryclearly ••,• 20os - 50os I [:::: 80øE 0 I 110øE 1 2 3 I 140øE 4 5 170øE 6 7 8 160øW 9 10 Days to Samoa Figure22. Trajectory to Samoaat 13kmonFebruary 20, 1999,at0000GMT (solid)and1002GMT (dashed). 32,520 OLTMANS ETAL.:OZONE IN THEPACIFIC TROPICAL TROPOSPHERE showsthatair originated10 daysearlierin northeastern Australia in a regionassociated with extensiveconvection duringthistime of year. The OLR map (Plate 5) for the periodprior to the soundingshowsthat convection(evidencedby the very low OLR) was widespreadin the region along the South Pacific Convergence Zone(SPCZ)throughwhichthe air parceltraveled basedon thetrajectorycalculation.The validityof thetrajectory TEMPERATURE & FROST POINT (C) -100 •0 -60 -40 -20 0 20 40 16 14 calculationunderthesevery convectivecircumstances is opento question, but sincethe calculation is for an altitudeof 13 km, thereis somereasonableexpectationthat the air parcelpath is abovethelayerwith the strongest verticalmotions.At anyrateit is clearthat air reachingSamoaduringthis periodis likely to havepassed througha regioninfluenced by convection. Thelow ozonemixingratiosare not usuallya resultof mixingdirectly from the surfacenearthe site,althoughsurfacemixingratiosare 6 low. This can be seen in Plate 3a, 3c, and 3d where the minima in theuppertroposphere arenotconnected to thelow valuesat the surfaceas illustratedby the individualprofile shownin Figure 21. Instead,there is normally a relative maximum in the mixing ratio in the midtroposphere.It is more likely that air with very low ozone is mixed vertically by convection in the region of o northernAustraliaand easternIndonesiaand transportedto these o 20 40 60 80 lOO 12o 14o 1 io sitesin the uppertroposphere[Kley et al., 1997]. OZONE (ppbv) In the Galapagosmany of the profiles during August-October Figure23. Ozonemixingratioprofileat theGalapagos on alsoshowpronouncedmidtroposphericpeaksas seenon October October 9, 1999.Thethickersolidlineistheozonemixingratio. 9, 1999 (Figure 23). The trajectory for this event (Figure 24) Thedashed lineis theair temperature, andthethinnersolidline crossesBrazil in less than 10 days over a region that is heavily is the dew/frostpoint temperature. influenced by biomass burning during this time of the year [Fishman et al., 1996]. Clear evidence for the enhancementof This is consistentwith the column amountsmeasuredin the ozone over Brazil is seen in two profiles from Natal, Brazil (5.4øS,35.4øW), on September29 and October6, 1999 (Figure profiles. As wasnotedearlier,duringtheaustralsummer, ozonemixing 25), where ozone mixing ratios exceed 100 ppbv. Althoughthe ratiosare generallysmallthroughout the troposphere in the air parceltrajectorypassesalmostdirectly over Natal, it may be westernPacific. Values less than 10 ppbv are seenas in the that both Natal and the Galapagosare influencedby the area to profile forFebruary 20,1999,atSamoa (Figure 21),where inthe the west and south of Natal, where the burning actually takes 13-15kmlayerozoneis -5 ppbvsimilarto theverylowvalues place [Kirchhoff et al., 1996]. This is stronglyindicatedby the seenbyKleyet al. [1996].Thetrajectory at 13km(Figure22) TTO map for October 4-6, 1999 (Plate 6), that identifies the 20ON - 0 O -- 30os - 90ow 120øW E 60øW Longitude 8[ , ....w 0 o 30øW 1 2 3 , , , , 4 5 6 7 8 9 Daysto Samoa Figure 24.Trajectory totheGalapagos at6 kmonOctober 9, 1999,at0000GMT. lO OLTMANS ET AL.' OZONE IN THE PACIFIC TROPICAL TROPOSPHERE 32,521 10 • t -5 -1o 80 1O0 120 140 160 180 Longitude ! Modified-Residual Tropospheric Ozone 03ohson Units) Plate 4. Map of the averagetropical troposphericozone residualcomputedfrom the Total Ozone Mapping Spectrometer (TOMS) totalcolumnozonefor the periodNovember10-12, 1997. 20ON -- 0 m ! I 90OE 180 ø Longitude 180 200 220 240 260 280 300 Plate 5. Map of the averageoutgoinglongwaveradiation(OLR) for the periodFebruary12-20, 1999. Plot from the NOAA-CIRES Climate DiagnosticsCenter. 32,522 OLTMANS ET AL.: OZONE IN THE PACIFIC TROPICAL TROPOSPHERE lO l -5 .1o -80 -lOO -60 -20 -40 Longitude o oo ,.-, o Ig • ..• ,,.,,1 Modified-Residual Tropospheric Ozone (Dobson Units) Plate6. Map of theaveragetropicaltropospheric ozoneresidualcomputed fromtheTOMS totalcolumnozonefor the periodOctober4-6, 1999. 15ON -- 90oW 60øW 30ow Longitude 180 2.00 220 240 260 280 300 Plate 7. Map of the averageOLR for the periodMarch 31, 1998. Plot from the NOAA-CIRES Climate DiagnosticsCenter. OLTMANS ET AL.' OZONE IN THE PACIFIC TROPICAL TEMPERATURE& FROSTPOINT(C) • - 100 -80 20 40 TROPOSPHERE 32,523 TEMPERATURE& FROSTPOINT(C) -60 -40 -20 0 20 60 80 100 120 140 40 - 100 -80 -60 -40 -20 0 20 20 40 60 80 100 120 140 40 10 U.I 1:3 ::3 !::: 8 0 160 0 OZONE(ppbv) 160 OZONE(ppbv) Figure 25. Ozonemixingratioprofilesat Natalon (a) September 29, 1999,and(b) October6, 1999. region of highest troposphericcolumn ozone as being over centralBrazil. From the Galapagosand Natal soundingsit is clear that enhancedozone amounts resulting from biomass burningare transportedboth to the east [Kirchhoff et al., 1996] wherethey appearat Natal andto the westreachingat leastas far as the Galapagos. It is possiblebasedon the case studiedhere that air reachingNatal from the region of burning may be recirculatedback to the west toward the Galapagosor may be transported directlyfrom the burningregionto the Galapagos. Investigationof eachprofile with an enhancedozonelayer in the midtroposphere during the August-Octoberperiod showeda trajectorythat passedover Brazil. At times of the year when burningis not occurringin Brazil, profiles at the Galapagosdo not show pronouncedtroposphericpeaks (Figure 26). Profiles with mixing ratios near 50 ppbv in the midtroposphereare occasionallyseen (Figure 26a). These higher amounts are generally associatedwith flow from continental South America (Figure 27a). However, flow from the continentmay also have TEMPERATURE& FROSTPOINT(C) TEMPERATURE & FROSTPOINT(C) -100 • -80 -60 -40 -20 0 20 100 120 140 - 100 40 -80 -60 -40 -20 0 20 100 120 140 40 10 u.I 1:3 ::3 I-- F-- 8 0 20 40 60 80 OZONE (ppbv) 160 0 20 40 60 80 OZONE (ppbv) Figure26. OzonemixingratioprofilesattheGalapagos on(a) March25, 1999,and(b) April4, 1998. 160 32,524 OLTMANS ET AL.: OZONE IN THE PACIFIC TROPICAL TROPOSPHERE 20ON -. 0 0 -- 30os 120øW 90ow 60ow 30ow Longitude 0 1 2 3 4 5 6 7 8 9 10 Days to Samoa 20ON - 0o - • 3005 - I 120oW iTi 0 0 I 90øW 1 2 3 60øW 4 .5 6 7 30øW 8 9 10 Daysto the Galapagos Figure27. Trajectories totheGalapagos at6 kmon(a)March25,1999,at1200GMTand(b)April4, 1998at120 GMT. relativelylow ozoneamounts(Figures26b and 27b). It appears that even thoughtransportto the site is similar,that unlessthis flow taps a sourceregion with higher ozone,the passageof air parcelsover a continentis not sufficient(althoughit doesappear necessary) to give enhancements in the ozoneamount.The April 4, 1998, example(Figure26b) wasalsonearthe endof the 19971998 E1 Nifio-southernoscillation(ENSO) warm phasewith well abovenormalprecipitationboth in the Galapagosand western equatorialSouthAmerica. The profile of April 4 suggests that convectionhasinfluencedthe profile sincehumidityis high up to -9 km (the depressionbetweenthe air temperatureand frostpointtemperature shownin Figure26b is small). The convection thatis responsible for thecharacteristics of thisprofileis likelyto have occurred over equatorial South America where the trajectory(Figure27b) showsthe air parcelintersecting an area of very strongconvection (Plate7). Convection nearerto the OLTMANS ET AL.: OZONE IN THE PACIFIC TROPICAL TROPOSPHERE Galapagosmay have influencedthe characteristics of the ozone profile at lower levels (below -6 km), but this cannotbe discernedfrom the profile information. 7. Conclusions 32,525 ExploratoryMission in the tropical Pacific: PEM-Tropics A, AugustSeptember1996,J. Geophys.Res.,104, 5567-5583, 1999. Kirchhoff, V.W.J.H., J.R. Alves, and F.R. da Silva, Observations of ozone concentrationsin the Brazilian cerrado during the TRACE A field expedition,J. Geophys.Res., 101, 24,029-24,042, 1996. Kley, D., P.J. Crutzen, H.G.J. Smit, H. Vomel, S.J. Oltmans,H. Grassel, and V. Ramanathan, Observations of near-zero ozone concentrations From an extensiveset of ozone profiles obtainedover the past several years in the tropical Pacific, the picture emergesof a regionof both very low troposphericozone amounts(-10 ppbv) and surprisinglylarge (-100 ppbv) mixing ratiosat all of the sites studied. The low concentrationsare expected in light of the strongphotochemicalsink in this region [Kley et al., 1997], and the importantrole of convection,particularlyduring the austral summer. On the other hand, the ubiquitous presence of midtroposphericlayers of enhancedozone demonstratesthat the influence of biomass burning is widespread throughout the tropical zone during August-November.In several examplesa strong connectioncould be made between enhancedozone amountsin the burning sourceregion and layers of large ozone concentrationin both the eastern and western tropical Pacific. On average,ozone at the equatorialGalapagossite in the eastern Pacific is greater than at the three western tropical Pacific sites. However, for individual profiles the midtropospheric enhancementsseen in the western Pacific attain larger mixing ratios than those seen in the Galapagos. This is in spite of the fact that the Galapagosare located much closer to a potential sourceof biomassburning (Brazil) than are the westernPacific sites (southern Africa). The proximity of other sources in Australia and Indonesia may partially account for this by providing closer source regions for the western Pacific sites. Alternatively, the much greater amount of biomassburned in southernAfrica may producelarger ozone enhancements[Olson et al., 1999]. The extensiveburningthat took place in Indonesia and Malaysia during the latter half of 1997 appearsto have been the sourceof very large ozoneamountsseenin Samoaand Fiji in November 1997. over the convectivePacific: Effects on air chemistry, Science,274, 230-233, 1996. Kley, D., H.G.J. Smit, H. V6mel, H. Grassl,V. Ramanathan,P.J. Crutzen, S. Williams, J. Meywerk and S.J. Oltmans, Troposphericwatervapour and ozone cross-sectionsin a zonal plane over the central equatorialPacific, Q. J. R. Meteorol. Soc.,123, 2009-2040, 1997. Komhyr, W.D., R.A. Barnes, G.B. Brothers, J.A. Lathrop, and D.P. Opperman, Electrochemical concentration cell ozonesonde performanceevaluationduring STOIC 1989, J. Geophys.Res., 100, 9231-9244, 1995. Merrill, J.T., Trajectory results and interpretationfor PEM-West A, J. Geophys.Res., 101, 1679-1690, 1996. Moody, J. L., The influenceof meteorologyon precipitationchemistryat selectedsitesin the easternUnited States,Ph.D. thesis,176 pp., Univ. of Mich., Ann Arbor, Michigan, 1986. Olson,J.R., B.A. Baum,D.R. Cahoon,andJ.H. Crawford,Frequencyand distributionof forest, savannaand crop fires over tropical regions duringPEM TropicsA, J. Geophys.Res., 104, 5865-5876, 1999. Randriambelo,T., J.L. Baray, S. Baldy, and P. Bremaud,A casestudyof extremetroposphericozonecontaminationin the tropicsusingin-situ, satelliteand meteorologicaldata, Geophys.Res. Lett., 26, 1287-1290, 1999. Randriambelo,T., J.-L. Baray, and S. Baldy, Effect of biomassburning, convective venting, and transport on troposphericozone over the Indian Ocean: Reunion Island field observations,J. Geophys.Res, 105, 11,813-11,832, 2000. Singh,H.B., et al., Biomassburninginfluenceson the compositionof the remote South Pacific troposphere:Analysis based on observations from PEM-TropicsA, Atmos.Environ.,34, 635-644, 2000. Stoller, P., et al., Measurementof atmosphericlayers from the NASA DC-8 and P3-B aircraftduringPEM-TropicsA, J. Geophys.Res.,104, 5745-5764, 1999. Thompson,A.M., and R.D. Hudson,Tropical troposphericozone(TTO) mapsfrom Nimbus 7 and Earth-ProbeTOMS by the modifiedresidual method: Evaluation with sondes, ENSO signals and trends from Atlantic regional time series,J. Geophys.Res., 104, 26,961-26,975, 1999. Thmnpson, A.M., and J.C. Witte, SHADOZ (Southern Hemisphere Acknowledgments. The authorsacknowledgethe helpful remarks of two reviewers whose commentsstrengthenedthe paper and improved the discussionof the connection between ozone source regions and featuresin the ozone profiles. The assistanceof R. Rossonin editing the manuscript and Jacquelyn Witte and Alexander Frolov in preparingthe TTO mapsis also acknowledged. Additional Ozonesondes: A new ozonesonde data set for the Earth sciencecommunity,Earth Obs., 11, 27-30, 1999. Thompson,A.M., J.C. Witte, R.D. Hudson,H. Guo, J.R. Herman,andM. Fujiwara, Tropical troposphericozoneand biomassburning,Science, in press,2001. M. Agama, J. Cornejo,and F. Paredes,INAMHI, San Cristobal, Galapagos,Ecuador. R.J. Bendura,Mail Stop483, NASA LangleyResearchCenter, Fishman, J., J.M. Hoell Jr., R.D. Bendura, R.J. McNeal, and V.W.J.H. Kirchhoff, NASA GTE TRACE A Experiment(September-October Hampton, VA 23681. H. Enriquez, INAMHI, Quito, Ecuador. 1992):Overview,J. Geophys.Res.,101, 23,865-23,879, 1996. J. M. Harris, B. J. Johnson,S. J. Oltmans,and H. V6mel, Climate Fujiwara, M., K. Kita, S. Kawakami, T. Ogawa, N. Komala, S. Saraspriya,and A. Suripto,Troposphericozoneenhancements during MonitoringandDiagnosticsLaboratory,NOAA, Boulder,CO 80305. (soltmans @cmdl.noaa.gov) the Indonesianforest fire events in 1994 and 1997 as revealed by F. Hasebe,IbarakiUniversity,Mito, Japan310-0056. ground-based observations, Geophys.Res.Lett., 26, 2417-2420, 1999. V. W. J. H. Kirchhoff, INPE, Caixa Postal 515, 12201-970 Sao Josedo Gregory,G.L., et al., Chemicalcharacteristics of Pacific tropospheric air in the regionof the IntertropicalConvergenceZone and SouthPacific Campos,Brazil. K. Koshy,M. Maata, A. Samad,G. Sami, and T. Tabuadravu, Convergence Zone,J. Geophys.Res.,104, 6577-5696, 1999. Harris, J.M, and J.D. Kahl, A descriptive atmospherictransport Universityof the SouthPacific,P.O. Box 1168,Suva,Fiji. J.A. Logan,Dept. of Earth andPlanetarySciences,Harvard climatology for the Mauna Loa Observatory, using clustered University,Cambridge,MA 02138. trajectories,J. Geophys.Res.,99, 13,651-13,667, 1990. M. Shiotani,HokkaidoUniversity,Sapporo,Japan060. Hams, J.M., and J.D. Kahl, Analysisof 10-day isentropicflow patterns P. Simon,MeteoFrance,Papeete,Tahiti, FrenchPolynesia. for Barrow,Alaska: 1985-1992,J. Geophys.Res., 99, 25,845-25,855, References 1994. Harris,J.M., andS.J.Oltmans,Variationsin tropospheric ozonerelatedto transportat American Samoa, J. Geophys.Res., 102, 8781-8791, A.M. Thompson,Code916, NASA GoddardSpaceFlightCenter, Greenbelt, MD 20771. 1998. Hoell, J.M, D.D. Davis, D.J. Jacob, M.O. Rogers, R.E. Newell, H.E. Fuelberg, R.J. McNeal, J.L. Raper, and R.J. Bendura, Pacific (ReceivedSeptember20, 2000; revisedDecember19, 2000; acceptedDecember21, 2000.)
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