JOURNAL OF GEOPHYSICAL RESEARCH, VOL. 96, NO. A11, PAGES 19,321-19,330, NOVEMBER 1, 1991 Compositionof Solar Flare Noble GasesPreservedin MeteoriteParentBody Regolith M. N. RAO• D. H. GARRISON? D. D. BOOARD G. BADHWAR, ANDA. V. MURALI 3 NASA JohnsonSpaceCenter, Houston,Texas The isotopiccomposition(long-termaverage)of solar flare (SF) Ne has been determinedby three isotope correlation techniques applied to datameasured onchemically etched pyroxene separates •repared fromtheKapoeta meteorite, whichis known to contain implanted solargases.TheSF 2øNe/2"Ne ratio obtainedis 11.6+ 0.2 and confinns previousdeterminations of this SF ratio in lunar and meteoritic samples.The sameSF Ne composition is alsoobtainedby applyingan ordinateintercepttechniqueto the samedataset. The ordinateintercepttechnique wasalsoappliedto theAr and He data,on whichthe threeisotopecorrelation technique cannotbe applied.The isotopiccomposition of SF Ar andSF He so obtained areSF36Ar/•Ar=4.9 +0.1andSF4He/3He =3800_+200,whicharesignificantly different fromthesolar wind(SW)ArandSWHevalues of-5.35and-2500,re.spectively. Correlation between 2øNe/22Ne and 36Ar/38Ar forthesame datasetalsogivesa similar SF 36Ar/XAr ratioof 4.8+ 0.2. Thedetermined SF He, NeandAr isotopicratiosdiffer from thosein SW by 52%, 17% and 9%, respectively,but the elemental compositions of 4Hed36Ar and2øNe/36Ar do notshowobvious differences between SF andSW. The concentration of the SF component in Kapoetapyroxenesis -20% that of the SW component,which is ordersof magnitudehigher than expectedfrom SW and SF protonflux measurements.Variationsin elementalandisotopiccomposition of He, Ne andAr in SF relativeto SW arefoundto correlatewell with a (Z/A)2 dependence, indicating a rigidity-dependent particle spectrum in solarflares. INTRODUCEION meteoritesKapoeta and Fayetteville using stepwiseheating methods have better definedthe SF 2øNe•2Nevalue to be in the Information about the composition of charged particle emissionsfrom the ancientSun can be obtainedfrom analysis range of 11.3 to 11.6 for both the ancientSun and the recent of helium, neon and argonimplantedinto fine-grainedregolith Sun [Venkatesanet al., 1981; Nautiyal et al., 1981, 1986; (or soils) of small planetary bodies such as the Moon and Wider et al., 1983, 1986; Padia and Rao, 1989]. However, it meteorite parent objects. Surface-implantednoble gases in hasnot beenclear whetheronly Ne showsisotopicdifferences silicategrainsfrom theseregolithsare a mixture of low-energy between$W and $F composition,or if similar and possibly existin He andAr isotopes aswell. solarwind (SW) and solarenergeticparticles,or solarflare (SF) relatedisotopicdifferences Complete analytical decompositionof a four-component gases,which reside in the outer micrometer and outer tens of and cosmogenic micrometers,respectively,of individualgrainsand are referred systemof implantedSW and SF components to as implantedor surface-correlated components.Noble gases GCR and SCR componentsthrough stepwisesampleheating producedby in situ spallationreactionsfrom galactic cosmic aloneis not possiblewith the Ne, Ar and He isotopicsystems. rays (GCR) and solar cosmicrays (SCR) residethroughoutthe However, chemical etching of the surfaces of grain-size interior of grains in abundancesgoverned by the exposure separatesof selected minerals, using techniquesdeveloped history, mineral-dependentproduction rates, and shielding earlier for lunar soils [Rao et al., 1979;Nautiyal et al., 1981], SW gases(mostlypresentin conditionsof the grains and are referredto as cosmogenicor can removethe surface-correlated volume-correlatedcomponents. Meteorites such as Kapoeta, the outer micrometer of grains), thereby permitting relatively rich in such solar gases, are ideally suited for decompositionof the SF, GCR and SCR componentsin the mineral residues. studyingthe preservedrecord of the isotopic abundancesof We have made mass spectrometricanalysesof noble gas solar noble gas componentsfrom the early solar system, whereasstudiesof grains from lunar soils and rocks usually componentsin acid-etchedpyroxene mineral separatesfrom Kapoeta, a brecciatedmeteorite consistingof both light and characterize more recent SW and SF irradiations. Therecentsolarwindis represented by a 2øNe/22Ne ratioof dark phases. The light phasehas been shieldedfrom relatively 13.6 + 0.1 [Geiss et al., 1972], as measuredon the Moon. A low energySW and SF particleirradiation,with its noblegases different Ne isotopic component (called Ne-C) having a being predominantly spallation products from deeply 2øNe/22Ne ratio of 10.6 was first identifiedby Black [1972] penetratingGCR. The dark phaseconsistsof SW- and SF- grainswhichcontainthevestigialrecordof ancient from stepwiseheatingof bulk samplesof gas-richmeteorites irradiated SW and SF implantedions,aswell asGCR and$CR spallation. and was attributedto SF Ne implantation. Further detailed measurements of Ne in lunar soilsandrocksand in the gas-rich Using three-isotopecorrelationsand•ordinateintercept techniques, we confirmpreviousresultsof otherlaboratories thattheisotopic composition of SFNe is different fromthat 1Also atPhysical Research Labaratory, Ahmedabad, India. in SW. Themajorpurpose of thepresent study, however, 2Alsoat Lockheed Engineering & Sciences Company, Houston, found Texas. 3AlsoatLunarandPlanetary Institute, Houston, Texas. is to extendthe techniques usedto determine the SF Ne composition to determine the SF Ar andSF He isotopic Paper number91JA01948. compositions[Rao et al., 1990]. Additionally, we discussa rigidity-dependentsolar flare particle spectrumas a possible explanationfor the observedisotopic and elementalSF SW 0148-0227/91/91JA-01948505.00 correlations. Copyright1991by the AmericanGeophysical Union. 19,321 19,322 RAO ET AL.: SOLARFLARENOBLEGASES EXPERIMENTAL METHODS Sampleswere taken from a large piece of Kapoetawherethe contact surface between light and dark portions was clearly distinguishable.The light sample(gas-poor)was takenfrom a clearwhite portion,while the dark sample(gas-rich)was taken from a portion which appeareduniformly grey. Extra dark grainsfound in the dark matrix were removedby hand-picking undera microscope.The light anddark sampleswere separately disaggregated by gentle crushing followed by mild ultasonication of remaining large aggregates. Mineral fractionsenrichedin pyroxeneand feldsparwere then prepared by repeatedheavy liquid separationfollowed by dry-sieving into 10-35 !.tm, 35-125 !.tm and 125-200 !.tm grain-size fractionsusing nylon sieves. Using energy dispersiveX-ray measurementson a scanningelectronmicroprobe,purity was determinedfor pyroxene separatesto be 98% for the 125-200 I.tm size fractionand 93% to 96% for both 10-35 I.tm and 35125 I.tm size fractions. The minor elemental composition was determined in aliquants of Kapoeta pyroxenes and feldspars by neutron activationanalysis,and the major elementalcompositionwas determined by microprobe measurements (by alternately scanningsamplesand standardsunder similar conditions). For the pyroxenes, we have found the following average compositions(over different size fractions):SiO2= 51.89%; A1203= 0.18%; MgO = 19.69%; CaO = 1.75%; FeO = 24.36%; MnO = 0.81%; Ba = 36 ppm. The averagecompositions from feldsparsize fractionsare SiO2= 45.02%; A1203= 35.39%; MgO = 0.4%; CaO = 18.6%;FeO = 0.52%;Ba = 68 ppm;U = 52 ppm;La = 1.52 ppm. Uncertainties in thesedeterminations are 8 to 10%. To remove the SW gasesfrom the surfaceof the silicate grains, aliquants of these mineral separateswere selectively etchedby stirring an acid mixture of HF+H2SO,•+H20 (1:1:4) underan infraredlamp for 30 to 60 s for the light etchandabout 2 to 2.5 min for the heavy etch. The chemicalreactionis suddenlyfrozen after the stipulatedperiod by heavily diluting the mixture with ultrapurewater. The etchedpyroxeneresidue is then washed in ethyl alcohol and dried. This procedure resultedin lightly etched(LE) andheavily etched(HE) samples for each pyroxene size fraction. Two chemical etching procedures were considered,weak acid/longexposureor strong acid/shortexposure. Long exposureis likely to enhancethe effects of acid creeping into the crevices of the pyroxene grains,dissolvingdeeperlayers and increasingthe amountof etchant.This effect results in distortionof the etchingdepth from the sieved fractions, while generally irregular in shape, were determined by estimating the approximatesizes of nonaggregate grainsundera microscope (about200 grainsper sample)[Eberhardtet al., 1965;Rao et al., 1979]. The average grainsizesare then--62 !.tmfor the 35-125 !.tmsize fractions and~146 grn for the 125-200!.tinsize fractions.The thickness of the surfacelayer removed from the pyroxenegrains was estimated usingthe amountof Fe, Si, andMg determined in the acidleachsolutionby atomicabsorption spectrometry (AAS) usingstandard procedures, andthedetermined average chemical composition of pyroxenes. For the LE 35-125 !.tmand LE 125-200 I.tm size fractions,the weight loss of the original samples was~8%. For theHE 35-125I.tm and125-200!.tmsize fractions, the weightlosswas~25% and20%, respectively.In the caseof the 10-35!.tmfraction,the weightlosswasfoundto be ~25%. For purposesof calculation,we assumedthat the grainshapesare approximately sphericalandthe materialwas removeduniformly from the surface. The averageetching depthsthusdetermined by procedures givenby Eberhardtet al. [1965] and Rao et al. [1979] for both pyroxenesize fractions are 1-2 I.tm for thelightly etchedsamplesand8-10 I.tm for the heavily etchedsamples. These representaverageetching depthsand may vary amongindividualgrainsdependingon graingeometryandetchingalongstructural defects.Finally, basedon the range-energyrelationshipgiven by Lal [1972] and using the determined average etching depths, the upper limit for the kinetic energyper nucleonof the implantedsolar flare particleswas estimatedfor each sample. Lightly etched sampleswith 1-2 !.tm removed containSF particlesof energy >0.4 MeV/amu (plus cosmogenicgases). Heavily etched sampleswith 8-10 !.tmremovedcontain SF particlesof energy >1.2 MeV/amu (plus cosmogenicgases). The uncertaintyin individual grain etching depths of 1-2 I.tm correspondsto variationsin energyof 0.1-0.2 MeV/amu. The noble gas compositionof the unetched(UE) samples from eachsize fractionis dominatedby solarwind gaseswith moderatecontributionsfrom SF and cosmogenicgases. While not treatedwith acid, these sampleshave probably lost some amount of surface material as a result of sample handling, crushing,ultrasonictreatmentand mineral separationsusing corrosivebromoformand acetyl bromide. The material lost is estimatedto correspondto SF particleswith energy<0.005 MeV/amu. Noble gas analyseswere made with a 6"-60ø sectormass spectrometerequipped with a Nier source and an electron multiplier. Gas extractionof ~100-mg sampleswas made by radio frequencyinductionheatingin a low blank, differentially information derived from mass balance. To minimize this pumped,Ta-tube furnace. Standarc'Zr/A1 gettersand charcoal effect, we have adopted the strong acid/short exposure fingers were used for gas clean-up and noble gas separation. approach. This permits the attack of the grain surfacesby Noble gas isotopicmeasurements were then made by standard strongacid for a shortperiodof time at an elevatedtemperature massspectrometrictechniquesin three temperatureextractions (60øC)to etchaway the requiredamountof the surfacematerial. of 600øC, 1200øC and 1600øC. All data were corrected for The HF + H2SOn+ H20 mixture chosenis commonlyused for blanksandmassdiscrimination.Typical 1600ø blanksfor the etching of pyroxenes [Crozaz et al., 1970]. The pyroxene systemare 3He, 0.2; 4He, 160;2øNe,0.25;4øAt,7.5 (x10'lø etching by HF + H2SO,• mixture is different from that by cm3STP). concentrated HNO3 [Wieler et al., 1986]. The etching of pyroxene grains by HNO3 seemsto take place along some SOLARFLARENEON,ARGON, AND HELIUM ISOTOPIC COMPOSITIONS crystalplaneswhile otherplanesseemto remainunattackedby the etchant[Haack, 1972]. Similar inferenceswere made earlier Solar Flare Neon in the case of olivine etching by HNO3 (D. Lal, private communication,1989). The use of HF + H2SOnseemsto result In this investigation we first show that three-isotope in a relativelyuniformchemicalattackof pyroxenes. correlationplots and the ordinate intercept technique,when The averagegrain sizesof the individualpyroxenegrains appliedto stepwise-released Ne data from etchedpyroxenesize RAO ET AL.' SOLARFLARENOBLEGASES 19,323 16 14 I SW 12• Lunar 12 lO z [] 6000 A 12000 o 1600C 0.0 SCR 2 2.O1 GCR lOO 0.0 0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1 21Ne / 22Ne Fig.1. Three-isotope correlation plotforNe fromstepwise heating of etched grainsizeseparates of Kapoeta pyroxene.SW, solarwindcomposition experiment [Geisset al., 1972]'Lunar, typicallunarfines;Air, terrestrial atmosphere; C.Ch, carbonaceous chondrites (meteorites); GCR, produced by galactic cosmic rayspaRation; SCR, produced by solarcosmicray reacttons. CompOSitional Nechanges duetoshielding variations of0-100 gcm '2and0-2g'cm-2 were calculated from Hohenberg et al. [1978] and are shownfor the GCR and SCR components, respectively.The GCR value plotted (2øNe/22Ne=0.92, 21Ne/22Ne=0.86) represents -15gcm '2shielding determined from track data calculations ofpreatmospheric radiiby Bhandari etal. [1980]. The Kapoeta datadefinea lineartrendproduced by mixingof two components. SF Ne is represented bytheintersection of thetwotrendlines.Theinsertshows thepossibility of upto 2%residual STMin the 600øC extractions.Uncertainties in isotopicratiosare within the symbols. likelytocontain residual SW,yields a SF2øNe/22Ne ratioof separates,yield similar and expectedcompositionsfor the less surface-correlatedSF Ne component. We then apply the 11.5q-0.2. This SF valueof 11.5 wouldallow for up to 2% SW ordinateintercept techniqueto He and Ar to determinethe to remain in the 600øC releases. Either value is consistent with surface-correlated SF Ar and SF He composition. Until now, previousdeterminationsof 11.3 to 11.6 for the SF Ne three-isotope correlationdiagrams(e.g., 2øNe/22Neversus compositionof both the ancientSun and the contemporarySun 21Ne/22Ne) havebeen theonlymethod used todetermine thesF [Venkatesanet al., 1981;Nautiyal et al., 1981,1986;Wieler et Ne isotopiccompositionin irradiated samples. In a three- al., 1983, 1986],indicating thatthe long-termaverageSF Ne isotope'plot for a systemconsistingof two distinct composition hasnot changed appreciably overthe last4,5 component in Kapoetapyroxene is components,generally surface-correlatedand volume- Gyr. The cosmogenic consistent with either SCR Ne produced at an average depth of correlated, thedatafromdifferent temperature releases lie on• at an averageshieldingdepth straight line joining the two end members. The relative ~0.3 gcm-2,or GCR Ne produced proportionof these componentsin a given gas fraction of ~15 gcm'2 (Figure1). An equivalent SF Ne composition is found using the determines where along the line the data point falls. Extrapolation of the data alongthe mixing line until it crosses ordinateintercepttechniqueapplied to the samepyroxeneNe theSW-air-planetary mixinglinethendetermines thesurface-databy plotting2øNe/22Ne versus thereciprocal of the22Ne concentration(Figure 2a). The ordinate intercept technique correlatedcomponentcomposition. Our Ne isotopicdatafrom step-wisetemperature extractions [Eberhardt et al., 1970] has been widely applied to lunar to determine the isotopiccomposition of (600ø, 1200ø,and1600øC)of etchedpyroxeneseparates of the regolithmaterials 10-35•tm, 35-125 •tm and 125-200•tm grain-sizefractionsfor two mixed gas components,a surface-co,elated(imp!anteed anda volume-col'related (cosmic bothdarkandlight Kapoetaphasesareplo,ttedin Figure1. The solarwindor flare)component component. For a suiteof grainsizes,a plotof pronounced lineartrenddefinedby theNe data(R2=0.991) rayproduced) of indicates mixingof a SF component alongtheupperleft of this an isotopicratio versusthe reciprocalof the concentration line and a cosmogenic componentat the lower right. an elementdominatedby the variable (surface)component results in a lineartrend.Theintercept of thistrend Extrapolation of thislineartrendintersects the SW-lunar-air tie generally to infiniteconcentration of thesurface-correlated line at 2øNe/22Ne= 11.6 q- 0.2 and 2aNe/22Ne= 0.030 q- 0.001 extrapolated definesthe isotopicratiø of that surface andder'roes theSFNe composition. TheFigure1 insertshows component that at low-temperatureextractionsthere is a very slight component.Sampleswith differentdegreesof etchh•goughtto to the ordinateintercepttechnique, because like deviationof the 600øCdatafrom the mixing line, possiblydue be amenable to thepresence of verysmallamounts of SW Ne. A best-fitline samples of different grain sizes, etched samples vary in of the surface-correlated gasper unit volumeof through onlythe 1200øCand1600øCdatapoints,whichare concentration 19,324 RAo ETAL.' SOLAR FLARENOBLEGASES 14 0.8 (a) 0.6 ß 10 z •. 8 z c• TEMP. 6 r• 600 0.2 .46 1600 r• 600 0.036 /• 1200 0.030 o '1600 - ß SUM ß SUM .52 I 2 TEMP, 21/22 .71 A 1200 o .... 20/22 0 0.027 . I I I I 0.2 0.3 0.4 0.5 0 0 0.6 I I I I I 0.1 0.2 0.3 0.4 0.5 -8 0.6 1 / [22Nex 10'sccSTP/g] / [22Ne x 10 ccSTP/g] 5.5 4,000 (c) 5.0 i i-i (d) i TEMP. [] 600 /• 1200 ß SUM 3,000 4.5 TEMP. 36/38 • 600 • 1200 o 1600 ß SUM SW 2.5 2.0 0 -• 2,000 4.82 ..!- 5.06 4.87 4.94 5.35 i i I i 2 4 6 8 4/3 3770 --3990 1,000 0 10 I 0 5 10 15 , I , 20 I , 25 3O 1/ [3He x10'SccSTP/g] 1 / [38Arx 10'eccSTP/g] Fig.2. Ordinate intercept plotsfor(a)2øNe/22Ne, (b)21Ne/22Ne, (c)•Ar/38Ar, and(d)4He/3He. Dataarefrom600øC, 1200øC, and1600øCtemperature extractions of five etchedKapoeta pyroxenes (threegrain-size separates andtwodegrees of etching). Wholedata,reconstructed fromthe sumof the temperature data,are alsoshown(twodatapointsoverlapin someplots). Uncertainties are contained withinthe symbols,exceptwhereindicatedfor a few concentrations. the samplebut not in the concentration of volume-correlatedextrapolation. Since bulk analysesof grain-sizeseparates gas. Additionally,increasingtemperatureextractionsare ratherthanstepwise temperature releases are thepreferreddata datafor all expectedto preferentiallyreleasesurface-correlated gas first to usewith theordinateinterceptplot,thecombined and volume correlated gas later. The 600øC and 1200øC extractions of eachetchedpyroxenegrain-sizeseparateare also extractions (each as a data subset) release predominantly surface-correlatedgas. To the extent that both of these extractionsof individualsamplesshowa spreadon the ordinate intercept plot because of variations among samples in concentrationof surface-correlatedgas (and not becauseof variations in relative proportions released of surface- and volume-correlated gas), these temperature data sets independentlyqualify for the ordinateintercepttechnique. The distributionof Ne data for each temperatureextractionthen indicatesa mixture of surface-correlated(solar) and volumecorrelated(cosmogenic)components. The 600øCextractionsall havemeasured2øNe/22Nelessthan or equal to 11.7, much lower than the SW value of 13.6. plottedin Figure2a. Thesedatadefinea line (R2= 0.943) whichyieldsan intercept valueof 11.52for the2øNe/22Ne SF composition.An analogousplot, shownin Figure 2b, of 2XNe/22Ne versus1/[22]is wellbehaved andyields2XNe/22Ne SF TABLE 1. KapoetaPyroxene SolarFlare(SF)Isotopic Compositions Determined by the OrdinateIntercept(OI) Three-Isotope Correlation, andTwo-ElementCorrelationTechniques Method 4Hed3Fe 2øNed22Ne21Ned221• 3990+100 3770+200 11.52+0.1 11.71+0.1 11.46+0.2 0.027+.001 0.036+.003 0.030+0.002 component, yieldsa 2øNe/22Ne valueof 11.7. The 1200øC Three-isotope 3150+150 temperature data(R2 =0.921)definean intercept valueof 11.46. Two-element 11.60+0.1 0.030+0.001 Furthermore,they define a line (R2= extrapolatedto infinite concentration of OI; 600øC 0.969) which, when OI; 1200ø C the surface-correlatedOI; 1600øC Both of these values are within errors of the SF 2øNe/22Ne composition of 11.6 + 0.2 determined by the three-isotope Ne correlation technique usingall of thedata.The 1600øCdataare 36Ar/38Ar 4.94+.1 4.82+.2 5.06+0.2 4.87+.2 SF value a 3800__+200 11.6+0.2 0.030+0.001 4.80+.2 4.90+0.1 SW value•' 2500+100 0.029+0.001 5.35+0.02 13.6+0.2 a AverageSF valueobtainedfrom all methods. SW valuesfrom Geisset al. [ 1972]andEberhardt etal. dominatedby the volume-correlatedcosmogeniccomponent bMeasured and have a lever arm too long to permit meaningful [1972]. RAO ET AL.: SOLARFLARENOBLEGASES values similar to those obtained in the three-isotope correlationplot. A summaryof SF Ne values obtainedby differentmethodsis given in Table 1. 19,325 contain small amountsof residual SW. An 3eAr/38Arvalue of 4.9 + 0.1 is obtained by averaging the four independently derived values, giving greater weight to the more precise summedtotal data, and is taken to representthe compositionof the surface-correlated SF Ar component. Yet anothermethodfor deducingthe isotopiccomposition of a surface-correlated component is to utilize elemental correlationsand determine one surface-correlatedcomposition knowing the other. Figures 3a and 3b show the correlation The solar flare 2øNe/22Necompositionwas previously determinedto be 11.6 :k 0.2 by Nautiyal et al. [1981, 1986] and Padia and Rao [1989] from stepwisepyrolysisof acid-etched pyroxeneand plagioclasemineral separatesfrom both lunar samplesand the Kapoeta and Fayetteville meteorites. A slightly lower value (though within errors) of 11.3 :k 0.3 was 2øNe/22Ne and36Ar]38Ar and4He/3He, respectively. In reportedby Wieler et al. [1986, 1989] for lunar samplesusinga between closedsystemstepwiseetching (CSSE) technique. The reason such a plot the summeddata def'memixing lines between a solar component,variable by grain size and for the small difference in the value determined in Ahmedabad, surface-correlated India, and in this Kapoeta investigation versus the value degree of etching, and a volume-correlated cosmogenic determinedby Wider et al. [1986, 1989] is not clear and may component(which in the case of nHe/3He also contains be analyticalor procedural. Subtle fractionationeffects in SF radiogenic 4He). The intersectionof the SF 2øNe/22Ne Ne may exist amongsamples,as Wieler et al. [1986] found the compositionwith the trend line definedby the summeddata in for 36Ar/3SAr and 2øNe/22Ne ratio in five plagioclase samplesfrom Apollo 16 eachfigurei• usedto infertheSFcomposition in theseSF soilsto vary from 10.9 + 0.1 to 11.6 + 0.2, with an averageof nHe/•He(seeFigures3a and3b). The uncertainties compositions are shownby the width of the shadedbarsand are assignedfrom a projectionof the uncertaintyin the derivedSF 2øNe/22Neratio onto the correlation of the summeddata. A direct "straight-line" correlation between Ne and Ar and especiallybetweenNe and He releasedat specifictemperatures generallygood agreementon data for solar-derivedgases is not expectedon theseplots becauseof different diffusion between their CSSE experiment and single-stage i•tching rams of both the solar and cosmogeniccomponentsof the followedby total samplefusion. It is conceivablethat a small noble gas elements. This is particularlypronouncedin Figure amount of SW Ne remained in all samples analyzed in Ahmedabadand in this investigation,but we would not expect the five of 11.3 + 0.3. A small mineral-dependent effect may alsoexistfor the SF Ne composition,as feldsparandpyroxene are knownto differ in their retentionpropertiesof SW Ne. We have no reasonto expect different resultsfrom the CSSE and single-stageetching techniques,as Wieler et al. [1986] found the amount of SW Ne to remain so constant between lunar and meteoritic samples and different etching experiments. The CSSE experimentsof Wieler et al. [1986] releasedsubstantial quantitiesof SW Ne in the earlieretchingsteps;the specificSF Ne compositionderived thus subtly dependson the fact that specificdata representinggreateretchingdepthswere selected for extrapolation. There is no real evidencein the collective data of a temporalvariation in the SF Ne composition. It is established,however,that this energeticsolarNe composition is quite distinctfrom the solar wind Ne compositionwhich has a 2øNe/22Ne ratio of 13.6 + 0.1. (a) SF 36Ar/38Ar = 4.8 +- 0.2 f o • ß ',:::::::: 3 - a,• SolarFlareArgon With the conclusionthat the isotopic compositionsof SF Ne and SW Ne are substantiallydifferent, we now examine whetherany differencesexist in the isotopiccompositionof Ar li.•:-.-'::.: Cosmog, I • • o o 2 $F 20Ne/22Ne = 11,6 -20,2iiiiiii!i • I • I • I , ,"-'",• , I 4 6 8 lO 12 14 20Ne / 22Ne and He in solar flares comparedto solar wind. BecauseAr has onlytwo isotopes (masses 36 and38) withpredominantly 4,000 (b) _ solar contributions(mass40 is dominatedby the decay product ß OF 4Ho/3Ho = 3150 + 150 of 4øK), a three-isotope correlationplot cannotbe usedto determine the Ar composition. Having established the consistency betweenthe three-isotopecorrelationand ordinate intercepttechniquesin determiningthe SF Ne composition,we now apply the ordinateintercepttechniqueto the Ar data from 3,000 ß :i:i:i:i:i:i:i:i:i:i.•!:!:i:!:i:i:i :::::::::::::::::::::::::::::::::::::::: :::::::::::::::::::::::::::::::::: '•' 2,000 ................... .................... /• the sameetchedpyroxenegrain-sizefractionswith a view to deducingthe surface-correlated SF Ar composition(see Figure 2c). Best-fit lines throughtemperaturedata setsof 1200øC, 1600øCandthesummed totaldata(R2= 0.993)yield36Ar/38Ar -:.:-:-:.:-:.:.:.:.:.:-:.:.:-:-:.:-:.:. .................... ::::::::::::::::::::::::::::::::::::::: 1,000 -- /• • 0 9 I , I ':':':':"::':':':':':':':':':':':':':' SF 20Ne/22Ne = 11.6 + 0.2 • I • I - , :::::¾::::::::::::::::::::::::::: 10.5 11 11.5 12 intercept values of 5.06, 4.87 and 4.94, respectively. Data 20Ne / 22Ne obtainedin the 600øC extractionsfit to a line with essentially zero slope. This indicatesthat variable concentrations of the 36 38 Two-element,isotopecorrelationplotsfor (a) Ar/ Ar versus SF componentwere released in the 600øC extraction with Fig. 3. 22 4 3 22 2øNedNe and(b) He/ He versus2øNe/Ne. Stepwise temperature virtually no cosmogeniccomponentreleased. An averageof extractions(open symbols)of five etched Kapoetapyroxenesand the 600øCdata yields a SF value of 36Ar/3SAr= 4.82. As mentionedfor the 600øCNe, theseextractionsmay or may not 9.5 /X 10 whole sampledata (solid symbols)reconstructed from the sumof the temperature dataareplotted. 19,326 lL•o ET AL.: SOLARFLARENOBLEGASES 3b, Wheresignificant amounts of nonsolar He wasreleased in Figure3b is a two-element, isotoperatioplot of '•He/3He the 600øCextraction, andall He wastotallyextracted by versus 2øNe/e2Ne similarto the36Ar/38Ar versus 2øNe/eZNe plot. 1200øC. Intersectionof the SF 2øNe/22Nefield of 11.6 + 0.2 with the TheSFComposition of2øNeffZNe = 11.6+ 0.2intersects the trendlinedefined bythesummed temperature datayieldsa SF trendlinedefined by thesummed etched pyroxene dataandthe '•He/3He composition of 3150+ 150,considerably lowerthan GCRc0smogenic endpoint in Figure 3aata sF36Ar/3SAr value thatobtained bytheordinate intercept method. Thistrendline of 4.8 + 0.2, which is within the limits of the SF 3•Ar/38Ar is not anchoredto the cosmogenic He composition because of value of4.9+ 0.1derived fromtheordinate intercept plot.The thedominance ofradiogenic '•He.Also,thefivesummed data are 600,øC and1200øC datapointsplotneartheregionwherethese pointsusedin Figure3b to derivethis4He/aHecomposition trendlinesintersect, indicating a minorcontribution fromthe not highly linear, and the uncertaintyon this ratio is probably cosmogenicComponent,whereasthe 1600øCpoints indicate considerablygreater than the shaded'•He/3He field would significant contributions from the cosmogenic component.indicate. In addition,He and Ne differ considerablyin the rate Consistentresults from the two techniquesindicate that the of releaseof their surface- and volume-correlatedcomponents long-term average SF Ar compositionimplanted in etched with increasingtemperature,as evidencedby the apparently releasesof Kapoeta pyroxene grains is significantly lower than that of curvedmixing line definedby individualtemperature othertrapped argon reservoirs suchasSW(3•Ar/38Ar = 5.35)or the etchedsize separatesin Figure 3b. Becauseof the greater terrestrial "air"andis bestrepresented by a 3eAr/38Ar ratioof tendencyfor He to be diffusivelylost from the samples,it is 4.9 + 0.1. possible thattheHe/Neratiosvaryevenamongthesummed A fewattempts havebeenmade earlier todetermine theSF data,which might explainthe differentSF '•He/3He value Ar compositio n usinglunarandmeteorite samples. Usingthe derivedfrom Figure3b comparedto Figure2d. We placemore ontheordinate intercept technique andpreferthelohgCSSE techniqu e on mineralseparates from lunarfines71501, reliance term average SF '•He?He ratio of 3800 + 200 for etchedKapoeta Wieleretal. [1986]reported nodifference in the3eAr/38Ar ratio pyroxene grains, although it is clear that a considerable uncertaintyexists in this value. Earlier,Benkertet al. [ 1988]reporteda valueof greaterthan reporteda valueof 4.94 + 0.1 for the36Ar/38Ar ratioby fitting 4200 for the'•He/3Heratioin SF He by fittingcurvedmixing curvedmixing lines to selectedtemperaturefractions. Earlier, Rao and Mathew[1987] reporteda valueof 5.2 for the same linesto selectedtemperaturefractiondata from the CSSE study from lunar fines 71501. In ratio basedon the 600øC gas releasefrom two orientedrocks of pyroxeneand ilmeniteseparates from the lunar Surface. anothercontext,Nier and Schlutter[1990] observedan average betweenSW, SF and air. While using the sametechniqueon mineral separatesfrom the same soil, Benkert et al. [1988] Solar Flare Helium The isotopic compositionof He measuredin solar flares '•He?Heratioof 4160+ 520 whilestudying He andNe isotopic ratios in interplanetary dust particles (IDPs). Thus there appearsto be significantevidencethat the '•He/3Heratio in variesfromonetypeof flareto another.I n 3He-richflares, solar flares is substantially greater than the SW value of generally smallevents, the4He/3He ratioranges from1 to 100, -2500. and in larger, "normal"flares the sameratio is 1000 or greater Summarizing,new data presentedin this studyindicatethat at energiesof about 10 MeV/amu [Webberet al., 1975]. As the long-termaverageNe, Ar and He isotopiccompositionsin this '•He/3He ratio in solar flares is known to be energy solarflaresare 11.6 + 0.2 for •Ne?ZNe, 4.9 + 0.1 for 3aAr/3SAr, dependent, the'•He/aHeratioaveraged overmanylargeevents and3800 + 200 for '•He/3He. TheseSF compositions are canbe ashigh as a few thousandat low energiesof ~1 MeV/amu significantly differentfromtheSW ratiosof 13.6for •øNe/ZeNe; [Black, 1983; Hurford et al., 1975]. The average isotopic 5.35 for 3•Ar?SArand 2500 for '•He?He. composition for He in a "normal"flare wouldseemto be a ELEMENTAL ABUNDANCES AND(Z/A)2DEPENDENCE bettercandidatefor comparisonwith lunar and meteoritedata. We now considerthe SF elementalcompositionof He, Ne Based on correlationsbetween trapped He and Ne isotopic compositionsin gas-richmeteorites,Black [1972] suggesteda andAr, i.e., '•He?•Arand2øNe?•Ar,usingthe samedatabase. valueof ~2500 for He-C whichwastentativelyidentifiedas SF At the outsetit may be noted that the SF componentcannotbe He at 1 MeV/amu. On the other hand, Yaniv and Marti [ 1981] derived by simple diffusive fractionation of SW into these reported a valueof ~12 for theSF'•He?Heratioin thelunarrock grainsbecausethe SF componentis enrichedin heavy isotopes 68815 at an energyof ~10 MeV/amu. relativeto the light isotopes(Table 1). If it were a diffusive Finding consistentresults between the ordinate intercept process,light isotopesshouldbe enrichedrelativeto the heavy and the two-elementisotoperatio techniquesin the caseof SF isotopes.This argumentwas madein moredetailby Wieler et Ne and SFAr leadsus to applythesetechniques to the He data. al. [1986]. Here we have studiedthree samplesets,unetched A He ordinateinterceptplot of 600øC, 1200øC and summed (UE), lightlyetched(LE) andheavilyetched(HE) fractionsfrom temperature data from each of the etched pyroxene size two pyroxenegrain size separates, 35-125 grn and 125-200gm fractionsis shownin Figure2d. The 1200øCdataare dominated (see experimentalsection). The data are given in Table 2 as by cosmogenic He, whereasvirtually no 3He remainsby the measuredtotals,i.e., summeddatafrom all temperature stepsof 1600øC extraction. The summedand the 600øC data points a given pyroxene fraction. The LE and HE samplescontain define best-fit lines (R2=0.992, 0.994) which, upon contributionsfrom SF particlescorresponding to E >0.4 and E extrapolationto infinite surface-correlated gas concentrations, >1.2 MeV/amu, respectively, and small amounts of yield surface-correlated SF '•He/3Hevaluesof 3990 and3770, cosmogenic gases. SF abundances were estimated by respectively(averagevalue: 3800 + 200). These values are subtracting thegasconcentration measured in the SF shielded muchhigherthanthe accepted SW '•He/3Heratioof ~2500 light pyroxenesamplefrom the measuredtotal abundancesin measuredin Kapoetabulk samples[Schultzand Kruse, 1989] the LE and HE dark pyroxenesamples. The UE samplesare and lunarfines [Eberhardtet al., 1970, 1972]. dominatedby SW gases of E > -0.005 MeV/amu. SW RAO ET AL.: SOLAR FLARE NOBLE GAS•ES 19,327 TABLE2. Measured Elemental Abundances in units10-scrn3STP/g Etch 3I-Ie 4I-Ie 2øNe 2•Ne 22Ne 3aAr 38Ar 2004.9 1045.6 810.1 264.1 205.1 245.2 8.26 5.32 5.49 4.26 3.92 3.99 165.3 86.2 73.5 37.7 21.7 24.7 56.53 36.23 15.60 13.87 5.06 7.15 10.72 7.71 3.51 3.19 1.37 1.83 3.9 0.89 4.2 1.6 0.06 PyroxeneDark 35-125 grn 125-200• 35-125 • 125-200• 35-125 • 125-200Wain PyroxeneLight 125-200• UE UE LE LE HE HE LE 44.39 116,900 31.01 69,600 35.26 88,000 27.33 55,600 25.74 37,500 21.91 36,700 4.11 2,804 Estimateduncertaintiesfor Ne and Ar are 5-7% and for He, 10-12%. UnetchedCLIE)samplescontainprimarilySW gaseswith moderateamountsof SF gasesand small amountsof cosmogenic gases.Unetchedsampleswerenot treatedwith the acid etchant. However,these samplesmay have lost somesurfacematerial (estimatedE <0.005 MeV/amu) as a result of sample handling,crushingand ultrasonictreatment. SW abundances comparableto literaturedata [Shultz and Kruse, 1989] are obtainedby subtracting the heavily etchedsampleconcentrations from the unetched sample concentrations. Lightlyetched(LE) samples had-1-2 prnof surfacematerialremovedby acidetching. They containSF gaseswith E >0.4 MeV/amu, plus smallamountsof cosmogenic gases. Heavilyetched(HE) samples had-8-10 [xmremovedby acid-etching.They containSF particleswith E >1.2 MeV/amu, plus smallamountsof cosmogenic gases. SF abundances were obtainedby subtracting the SF shieldedlight sampleabundances from the HE darksample. abundanceswere obtainedby subtractingthe calculatedSF still possiblethat there has been a factor of 2-3 diffusive loss of SF He, relative to At, from theseKapoetagrains. A comparison of the long-term average isotopic samples,and are shownTable 2. These SW abundances are abundancesfrom the total He, Ne and Ar measured in the UE of SF 3He/4He, 2øNe/22Ne and36Ar/3SAr ratiosto the comparable to thosefrom Kapoetaliteraturedata [Schultzand composition Kruse, 1989] except for SW He, which shows large losses corresponding SW ratios showsthat the enrichmentof heavier relative to At, possibly due to diffusion from shallow grain- isotopesover lighter isotopesis greater in SF than SW by surfaceimplantation.The observed SW 4He/36Arratiosof 626- about52%, 17% and 9%, respectively(Table 3). Theseheavy 1540 are a factorof 7 to 10 lower thanthe SW 4He/36Arratio of ion enhancements for He, Ne, and Ar fit the empiricalequation -7500 obtained from lunar fines [Eberhardt et al., 1970]. The AM/Mp = K, whereM refersto the isotopicmass, AM refersto SF 4He/36Arratiosrangefrom4300 to 10,030with an average the massdifferencebetweentwo adjacentisotopesof a given valueof 6640, whichis closeto the SW 4He/36Arratio of -7500 from lunar fines. There has apparentlybeenmuchlessdiffusive lossof SF He than SW He, relativeto At. This greaterretention of SF He is likely due to the higher-energySF particlesbeing more deeplyimplantedin the grain surfacesthan SW. The SW element,p is the enhancementfactor (SF/SW), and K -0.68 is a constant. This heavy ion enhancementbetween the two isotopesof a given elementdecreasesmonotonicallyas the mass increases from He to Ar in solar flares. Table 3 lists the isotopic and ele•nental fractionation 2øNe/36Ar ratiosrangefrom 27.5 to 35.0 with an averageof 31.7, which is similar to the "solar system average" SW 2øNe/36Arvalue of ~37 determined from meteorites and lunar sampleslandersand Ebihara,1982]. The SF 2øNe/36Ar ratios TABLE 3. IsotopicandElementalFractionation Factors,for example, 36 36 (2øNe/Z2Ne)sw/(•e/•e)sFand(2øNed Ar)sw/(2øNe/ Ar)sl• range from 29.2 to 49.6 with an averagevalue of-41, also Elemental similar to the "solar system"SW value of-37. This suggests Isotopic that therehas been no significantlossof SF Ne, relative to At. 3/36 4/36 20/36 22/36 3/4 20/22 36/38 We concludethat the4He/36Arand2øNe/36Ar ratiosin solarflares are similarto thosein SW within experimentalerrors. SW/SF a 1.52 1.17 1.09 0.4-1.5 0.7-1.7 0.8-1.3 0.5-1.0 We can alsocomparethe long-termaverageSF He/At andSF (Z/A)2b 1.79 1.21 1.10 1.80 1.00 1.00 0.80 Ne/Ar values derived here with direct satellite measurements of (l/A)2c 1.79 1.21 1.10 144 81 3.20 2.70 contemporarysolar energetic particles (SEP) summarizedby Mason [1987]. This comparisonrequiresconsideringtotal SF aSolarFlare (SF) isotopicratios are derivedfrom three-isotopeand elementalabundanceratios of (3He+4He)/(3aAr+3SAr)and (2øNe+22Ne)/(3aAr+38Ar), whicharedetermined fromTable2. SF contributions of 2XNeand4øAtarenegligible.The observed SF Ne/Ar ratiosof ~45 are in excellentagreementwith the satellite SEP Ne/Ar ratio of 42. However, the observed SF He/At values of 4-7 x 103are lowerthanthe valueof ~17 x 103givenby Mason [1987]. While SF He does not show the same order of magnitudelossesrelative to Ar as SW He, noted above, it is ordinateintercepttechniques(see Table 1); SF elemental ratios are derivedfrom heavyetchconcentrations (seeTable 2); solarwind (SW) He andNe isotopicratiosare from Geisset al. [1972]; SWAr isotopicratios are from Eberhardt et al., 1972. The SW He/Ar elemental ratios are from Geiss et al. [1972]; the SW Ne/Ar ratio is from Anders and Ebihara [1982]. Estimated elemental ratio uncertaintiesare He/At -35%; Ne/Ar -25%. t,(Z/A)2 factorrepresents rigidity dependence. c(1/A)2 factorrepresents mass dependence. 19,328 RAOET AL.: SOLARFLARENOBLEGASES factors obtained fromSw/sFratiosfor He, Ne, andAt. It It has been shown [Lal, 1972; McGuire et al., 1981] that the by an exponential shouldbe clearlyunderstood thatbecauseof thenatureof these SF particlespectrumcan be well represented rigidity,J(R)= ke-R/Ro,whereJ is thedifferential measurement techniques,theseratiosare basedon essentially in particle the same energy per nucleon and reflect rather long term flux and Ro is a characteristicrigidity. This rigidity spectrum averages of theseelements.The isotopicratiosgivenin Table can be transformedinto a spectrumin kinetic energy per 3, which are less affectedby relative diffusionrates, show a nudeonJ(E)= AE-• At very high energies(> 100 MeV/amu,Ro near-perfect correlation with (Z/A)2 and(l/A) 2. In orderto ~100 MV) theslopebecomessteepwith ¾~3,while remaining distinguish betweentheserelations,one can examinethe essentially flat at low energies (<10 MeV/amu) with •'-1 elementalfractionationfactors. It is quite clear from these [Blanfordet al., 1975]. This low-energyvalueis in agreement ratiosthata (Z/A)2 proportionality is favoredover the simpler with observationsof Lal and Rajah [1969] and Pellas et al. (l/A) 2 dependence, particularlywhenoneconsiders the higher [1969], who found¾=1.2 + 0.2 for $F Fe groupnucleiin the 1diffusion rates of He relative to At. to 10-MeV/amurange in Kapoetapyroxenes. However,there The excess22Ne over 2øNe in SF comparedto SW, as may be somecontributionto the flatteningof the observedFe discussedat the beginning of this section, can easily be group $F particle spectrum at low energies, i.e., 0.1-10 understoodif one assumesthat the SF particle spectrumis a MeV/amu, from shieldingof Kapoeta grain surfaces[Zinner, function of rigidity alone. There is significantexperimental 1979]. For Kapoeta,we can use a $F flux ratio as an indication evidence (next section) to suggest that this assumptionis of the spectral shape of the implanted $F ions in the 1valid. If we now recall that the measurements are made at the Mev/amuenergyregion. This ratio is definedto be thetotal SF samekinetic energy per nucleon,the rigidity spectrum,J(R), particleflux with E > 0.4 MeV/amu to the totalSF flux with E > can be convertedinto a kinetic energy per nucleon spectrum, 1.2 MeV/amu, i.e., (•E>0.4 MeV/amu)/(•E>l.2 MeV/amu). J(E). This transformationfor very low energyparticles(E<< The observedflux ratios and the theoreticallypredictedflux protonrestmass,m) is simplygivenby J(E) = J(R) (Z/^)2 ratios determined for both rigidity and kinetic energy ((E+m)/R). Thus the conversionfrom a rigidity to a kinetic dependentspectraare listed in Table 4. The resultsshowthat energy per nucleonbasis leads to the observed(Z/A)2 the solar flare particle flux spectrumdeterminedin Kapoeta proportionality. This is consistent with the explanation does indeed flatten out at low energy, i.e., •' approaches1 at offeredby Meyer and Casse [ 1979], in which they proposed particleenergiesof a few MeV/amu. that the particle acceleration selectively enhances the abundance of heavierisotopesdue to their greaterrigidity at the TABLE 4. Measured and Theoretical Solar Flare Flux Ratios: sameenergyper nucleon. ß (E>0.4 MeV/amu)/•(E>l.2 MeV/amu), DerivedFrom LighfiyEtehedand Heavily EtchedGas Concentrations Basedon orderingof our isotopicdataby (Z/A)2, as first suggested by Meyer and Casse[1979], one would expectsolar particle accelerationto selectively enhancethe abundanceof heavier isotopes. In a review of satellite-basedmeasurements of a largenumberof isotopesin recentsolarflares,Mewaldt et al. [1984] found no such abundanceenhancement. There are, however, three significant differences between our measurementsand these satellite-basedmeasurements: (1) our data include particleswith significantlylower kinetic energy per nucleon (<~1 MeV/n) compared to the measurements summarized by Mewaldt et al. [1984]; (2) although it is observedthat the isotopic compositionis relatively constant over a very small time interval, our measurements correspond 35-125gm 125-200 gm 3•Ar 22Ne 4He lae-a/•o 3.08 1.94 3.40 1.53 2.35 1.51 1.49a 1.49a !• '• 1.41•' 1.41•' SeeTable2 for samplegasconcentrations. "Integralflux determined from a rigidity-dependent particlespectrum; R=54.8 MV at E=0.4 MeV, R=94.9 MV at E=l.2 MeV, Ro=100 MV. •'Integral fluxdetermined froma kineticenergy dependent particle spectrum; ?--1.4for E<15 MeV and ?=3for E>15 MeV [Blanfordet al, 1975]. to an extremelylargetime averageandincludemany3He-rich flares; and (3) Mewaldt [1979] pointed out that the isotopic Up to 25% of the total trappedsolarNe and Ar in Kapoeta compositionof solar wind and solar flaresmay be significantly canbe attributedto SF (Table 2). Similarly,SF Ne observedin different. Althoughno modelsexist for thesedifferencesor for the isotopiccomposition in 3He-richflares,we simplypoint out that our measurementsof noble gasesover a very large (Z/A) 2 can mosteasilybe understood in termsof a rigiditydependentmechanism. ENERGY SPECTRUM OF SOLAR FLARE NEON AND ARGON By calculatingthe approximatedepthsto which the grain surfaces have been etched and utilizing a range-energy relationship [Lal, 1972], the grain-etchingtechniquecan be used to samplethe incident particle energy spectrumabove a given kinetic energy per nucleon. The kinetic energy per nucleonfor the trappedsolar flare particlesremainingin each sample after etching is estimated to be greater than -0.4 MeV/amu in the lightly etchedsamples,and greaterthan -1.2 MeV/amu in the heavily etched samples(see experimental section). pyroxenesfrom lunar fines accountfor -20-30% of the total retainedsolar Ne [Nautiyal et al., 1986; Wieler et al., 1986]. This resultled Wieler et al. [1986] to point out that theratio of the averageSW protonflux to the SF protonflux (E >10 MeV) is six ordersof magnitudehigherthantheir observedlunarsoil SW/SF Ne flux ratio. In order to explain this apparentlarge flux of SF ions, Wieler et al. [1986] invoked the presenceof 10- to 50-keV/amu "suprathermalions" in concentrations sufficientlyhigh to bring the SW/SF flux ratio down to ~3. KapoetaSW/SFNe andAr flux ratiosof ~10, inferredfrom the measuredabundanceratios listed in Table 5, were determinedin the acid-etchedgrain separateswhere particlesof energyless than-1.2 MeV/amu were quantitativelyremoved.This implies that the measuredSF componentin gas-richmeteorites(as well as in lunar soils)doesnot seemto be dominatedby ions from the 10- to 50-keV/amu range, althoughthe presenceof such ions at much lower concentrations cannot be ruled out. At RAG ET AL.' SOLAR FLARE NOBLE GASES 19,329 TABLE 5. Ratios of Solar Wind (SW) to Solar Flare (SF) Abundances, of trappedgasesin the meteoriteKhor Temiki, J. Geophys.Res., 70, 4375-4378, 1965. Eberhardt, P., J. Geiss, H. Graf, N. Groegler, U. Kraehenbuehl, H. Schwaller,J. Schwarzmueller,and A. 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