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RESONANCEIONIZADTEITOENCSTPIEOCNTORFOSMCEORPCYUFROYRTHEULTRATRACE By WENDYLEIGHCLEVENGER OAFDTIHSESOEUFRNTITAVHTEEIRROSENIDQTPOUYRCIOETRSFOEEFRMNLEOTONFERTDIPSDTHAFIOOLITRONHSTPEOHAPGREHRTYDIAEADGLURFAEUTELEFOSIFCLHLMOEONLT UNIVERSITYOFFLORIDA 1997 ClevengeTrh,isadnidssmerytagtriaonndimsodtehdeirc.atAegdnteostChreemaesmmoarnyWoofotmeyngGraanmdefra.ther.CharlesAnderson ACKNOWLEDGMENTS Ihaveoftenthoughtaboutallofthethings1couldhavedonewiththepastfour syfmuelaelrlysliroenafglimtzhyeearlnoisdfee:sa.pptrNreaocviwealtitenhgat,thesIpseexenpedetirhineegnltcigeihsmteIathwaitvtheheehfnaaddmioalsfytaahgenrdgardfaurdaiuteaentdsset,usdtceahnkotio.nlgtuitnneeals,yIacnadn ThemainthanksforgettingmethroughanyofthisgotoDr.JamesWinefordner. Hisawe-inspiringenthusiasm,knowledge,andlaughterhavesetanexamplethatIhope tocarrywithmealways.Hisunderstandingandrespectforhisstudentsaresomethingto becherishedandhasmademerealizehowluckyIamtohavebeeninhisgroup. EqualthanksgotoDr.BenjaminSmithforhisfriendshipandconstantsupport. Hwaissnv'itssiuonreoIfcwohualdt.goodscienceishasalwaysinspiredmetoexcelandshineinwaysI whomIFhuratvheerbegernatfiotrutduenaisteexetneonudgehdttoobDersa.ssOolcieagteMdawtivtehevforantdheNpiacsotlotwOomcyemaerts.to.Olweigt'hs emMnoetrhdwuohsahitaRsicmtheaarrn,adcStucersreaiansttaiivcCisatyb1raewndodouNliadcnodl’iQskielnogtvoeSohuafnvhfeiosrawtsoheraikrsacasinesdnitstitshaton.sceesIinhmaturhisinstgwaoilnrskio.thtahvaenkshLoewahn andforIgniavdidnigtimoen.aInwoeuxladmplliekeotfothhoawnkhaDrr.dKwaotrhkryfnorWisltludieanmtssfcoarnheprasyuopfpfo.rtIamnudsatdvailcseo thankDr,RobertKennedy.Dr.JosephDclfino.Dr.JimDeyrupandDr.RickYostfor theirhelpandsupport,aswellastheUSNationalInstitutesofHealth,theUSDepartment ofEnergy,andespeciallytheUSEnvironmentalProtectionAgencyfortheirhelpin fundingthiswork. Mostimportantly,Imustthankmyparents,JerryandLindaClevenger,forthe love,support,andencouragementIhavebeenluckyenoughtoreceivemywholelife. today-IamalsogratefultomybrotherChuckandsisterChristyaswellastherestofmy family.Ifeelmostblessedtohaveallofthemandtheknowledgethattheyarealways thereforme. supportIovmeurstthaelpsaostthfaonukrtyheaersf.rieTnhdesstehaitncIlhudaeveJDmaWdeg,rofurpommewmhbeormsIRhoabveGugeanianredd,mDuacvhe Rusak,ArthurBestcman,ScottBaker,AndreaCroslyn,BryanCastle,andBeckyLitteral. EquallyimportantareTradeWilliams.EveHunovice,SundayBrooks.BrendanBoyd, MikeBruner,AaronWilliams,ScottGordon,andYannisKarayannis.Ialsogivemany ThankyouGodforallofthewonderfulopportunitiesandexperiencesyouhave TABLEOFCONTENTS lIF-nuadrsunccartciIevnedAlutycoeCmdoiucBprlNeneandk-dPTlhoaewisnrmSospaeMlcaEtaxrscoimStepatetrciyotnroSmpeetcrtyrom SpecianuuCoupledwithlnd; CHASSRPeuPsTmEoPRmErCneaiRasTnrnocRyc3niOepaolnSfleAcosCTNeo-Oe—iAlczPLoahYimnYiziToaqniIuieSCopsnAecLStpreTocLstcMrooEpsyRcoEpSyOolf.MVerEcDurRyE.SONANCEIONIZATION....33335696 CHARPYTDEBRE4RGRSETSAOTNEASNCEIONIZATIONSPECTROSCOPYOfMERCURY 69 SBAtusafsrfikegrnEifGnfaegscStPpsreecstsrualrelaShniefstsandBroaden ,...7777266* CHASIPINTGERENTARLA5:TMROESSPOHNEARNECEWIITOHNIAZVATAILOANNOCFHMEEARMCPUURFYIACTAOHMOSNIONFADNIE $1 ResultsandDiscussion CHACPOTNESRID6:ERMAETTIHONOSDOPTIMIZATIONANDANALYTICAL ERexspueAPPlrneetairr!lmffyeaootnnrritdmmcaaaaDllnniccsCeecuuoorsffvte-EEtlxoeoccntartotnonC-oSucnIhtee”rme’ CHAPTER7FUTUREWORK USTOFREFERENCES BIOGRAPHICALSKETCH 3- LISTOFTABLES 4- 5-11.:EE(lxxeRccvyeiidltt)baa,tetiiaroosgnntlttaerrbvaauennllss)aii,ttteaiidsoonnbtssyafbfMouorrloaHoHtrggedeffboofyrrorilMnaaosso=cerrr6e--,c,co7o,Bnnann9iee-gcc2t,t6ceaddnlldeevvieenlltsshi11s,A2w,3o3,raaknndfdo4r4n(=Ry6d,b7e,rg.45 10-48 73-5 1.lEexvceilt),ataisontatbrualnastietdiobnysfMooroHrgeffoorrlnas=er6,-c7o,n9n-ec1t3e.dlevels1,2,3and4(Rydberg 95 AbosRfletrqhaueciiUrnoeifmveeDnritsssisetfryotroatftihFoelnoDPrerigedrsaeeienntoPefadrDttoioactlthoFeurlGofrfialdPluhmaietlneotsSoocfphhtoyhoel RESONANCEIONIZADTEITOENCSTPIEOCNTORFOSMCEORPCYUFROYRTHEULTRATRACE By August1997 MajorDepartment:Chemistry Resonanceionizationspectroscopy(RIS)hasbeenproventobeoneofthemost method(i.e„astreamofineitgas)insteadofaflameorfiimace.Forthesereasons,itis thewell-establishedmetl RISinvolvesthe s.The 0 novelelectroncounterintowhichthemercuryatomsweresweptbyastreamofbuffer gas.Ahighvoltage(0-3.5kV)wasappliedbetweentwoelectrodestoallowcollection oftheelectrons.Thesignalwasamplifiedandrecordedonadigitizingoscilloscopeand laptopcomputer. FundamentalstudiesofmercuryRydbergstateswerecarriedoutinordertofind theoptimalconditionsforultratracedetection.Thesestudiesincludedtheeffectofthe choiceofgaspressureandappliedhighvoltageonthespectrallines.Inaddition,theuse ogifvaevaalsaingcnahle6a.m6plxif1icsattiiomnesofhitghheereltehcatnrictahlessiiggnnaallowbasserivnevdeswtiitghattehdeannodtmdaelteRr1mSinseedtupt.o detectionexperimentallydeterminedis1.9X10satomsinthemeasurementvolume. whichwaslimitedbypoorionizationefficiency.Apreliminarystudyinvolvingthe generationofmercurybythecoldvapormethodhornaqueousstandards,usingan unoptimizedRISdetectionschemeandsampleintroductionapparatus,showedlinearity