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Isotopic Analyses of Barium in Meteorites and in Terrestrial

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Isotopic Analyses of Barium in Meteorites and in Terrestrial •'OO•,NALO• GEO•'IIYSlCALRESXAaCX VOL. ?4, NO. IS, JULY IS, 1969 Isotopic Analysesof Barium in Meteorites and in Terrestrial Samples O. EUGSTER,F. TERA,AND G. J. WASSERBURG Charles Arms Laboratory o• the Division o• Geological Sciences Cali•Jrnia Institute o• Technology,Pasadena, California 91109 Isotopic compos•tien and concentration of barium in six stone meteorites and the silicate inclusionsof two iron meteorites and three terrestrial sampleswere measured by use of a 'double spike' isotopic dilution technique in order to correct for laboratory fractionation. Any differencesbetween the abundancesof the isotopesin meteoritic and terrestrial Ba were found to be less than 0.1% for all isotopes.The per cent abundancesof Ba found in our work for Ba '•s, Ba•, Ba•% Ba '•, Ba TM,Ba •', and Ba'•ø are 71.699, 11.232, 7.853, 6.592, 2.417, 0.1012, and 0.1058, respectively. Because of the higher precision, these abundancesshould replace the currently accepted values. These results show the variations in the Ba isotopesreported by S. Umemoto (1962) to be unsubstantiated. INTRODUCTION Umemoto [1962] reported that the isotopic A comparison.of the isotopiccomposition of compositionof Ba in the Bruderheimchondrite and in the Pasamonte and Nuevo Laredo various elements in terrestrial samples,me- achondrites were distinct from terrestrial Ba teorites, and other materials of the solar system is of fundamental importance in determin- and showeda pattern of uniform fractionation relative to terrestrial Ba. The enrichments ob- ing the early history of the solar system and the mechanismsof nucleosynthesis.In ad- servedby him correspondto a 2% enrichment dition to effectsthat are a product of either in the ratio Ba•ø/Ba• compared with ter- long-lived natural activity or cosmic-rayinter- restrial materials. Previously, Krummenacher action with meteoritic material, isotopicabun- et al. [1962] found no anomaliesgreater than dancesmay be distinct from terrestrial material 3% for the isotopesBa •'-• in the Richardton chondrite. Since the established fractionation becauseof isotopicfractionation or incomplete isotopic homogenizationduring the formation patterns for Xe and the suggestedfractionation of the solar system. The only major variation of Ba reported by Umemoto were in the in isotopic abundancesobserved between ter- same direction, it was of great interest to con- restrial and meteoritic samples that is not firm or disprove the reality of this reported effect. The mechanisms for fractionation that causedby nuclear processesis found in the rare gasesneon [Pepin, 1967], krypton [Eugster et have been proposedfor Xe and Kr are far al., 1967], and xenon [Reynolds, 1960a]. The from satisfactory,and it was conceivablethat only apparent exceptionsto the constancyof someunknown mechanism might have also op- the isotopicabundances, with the exceptionof erated in fractionating the Ba isotopes.The the rare gases, are the elements lithium and magnitude of the fractionation proposedby barium. Investigationsof lithium by Gradsztajn Umemoto was significantly smaller than that et al. [1967] suggestthat there is a variation found for Xe, which is approximately4% per of the abundance of lithium in stone meteorites mass unit, whereasfor Ba Umemoto indicated of about 10%. These data have not yet been an effect of 0.25% per mass unit. It is well confirmedby work in other laboratories. known that isotopic fractionation may be in- duced during mass spectrometricanalysis, and great care must be taken to avoid the produc- x Contribution 1606 of the California Institute tion of this type of anomaly by laboratory of Technology. procedures.This is made quite evident by the work of Wetherill [1964] on molybdenum,who Copyright ¸ 1969 by the American GeophysicalUnion. demonstrated that the variations in molyb- 3897 3898 EUGSTER, TERA, AND WASSERBURG TABLE 1. Isotopic Composition of the Double Spike Atom per cent abundances. 1. Enriched Ba •37,measured 697 89.457 0.660 0.1290 0.0543 0.00119 0.00070 060 4-.070 4-.006 4-.0030 4-.0010 4-.00005 4-.00005 2. Enriched Ba TM,measured 867 1.646 1.789 4.080 84.572 0.0351 0.0115 150 4-.025 4-.018 4-.020 4-.200 4-.0004 4-.0003 3. Calculated compositionof 387 74.555 0.8515 0.7995 14.398 0.00695 0.00253 double spike based on com- 064 4-.058 4-.0059 4-.0040 4-.034 4-.00008 4-.00007 positionsof I and'2and on the amounts of Ba taken from the two salts *• 4. Measured compositionof 9.338 74.598 0.8500 0.7967 14.407 0.00690 0.00251 double spike, normalized to 4-. 004 4-. 0014 4-. 0014 4-. 00007 4-. 00006 Ba'37/Ba TM = 5.178 5. Typical compositionof a 39.403 44.020 4. 2322 3.5990 8.641 0.05260 0.05270 mixture of double spike plus 4-.010 4-.010 4-.0010 4-.0010 4-.010 4-. 00005 4-. 00005 sample, not corrected for fractionation (Nuevo Laredo) Notes. For I and 2 the total errors are based on the errors for the uncertainty of the fractionation and on the statistical errors. The total error equals [•i (ai)2]•t•..For 3 the errors are based on the errors of I and 2. For 4 and 5 statistical errors are shown. * For the double spike the ratio of the total number of Ba atoms contributed by the enriched Ba xs• salt to the total number of Ba atoms contributed by the enriched Ba TMsalt was 4.8929 as calculated from the gravimetric data and from the atomic weights of the enriched Ba which was based on I and 2, respectively. denumisotopic abundances reported by Murthy EXPERIMENTAL PROCEDURE [1962, 1963, 1964] were most likely due to in- Chemical treatment. A 0.2- to 5-gram sam- strumental fractionation. In this light, the iso- ple was mechanicallycleaned with a dental burr topic variations of Mo in terrestrial ore sam- to remove any surface contamination,washed ples reported by Crouch and Tuplin [1964] with acetone,dried in an oven, and, after grind- appear very doubtful. These authors seem to ing and splitting, weighedinto a 100-ml teflon be unaware of the other work in this field and beaker. The sample was dissolved in HC10, the instrumental problemsthat invariably exist. and HF, 5 ml of each acid per gram solid sam- Chakraburtty et al. [1964] reportedthat no en- ple, evaporated to dryness,and redissolvedin richment of Ag•ø• was found in seven iron me- 2.5 N HC1. An aliquot correspondingto about teorites, including Canyon Diablo for which an 0.2 gram of solid samplewas taken, evaporated anomalywas reportedby Murthy [1960], which to dryness, and then brought into solution in was most likely the effect of instrumental frac- 2 ml of 2 N HC1 which was loaded onto a cat- tionation. ion exchangecolumn (1 cm X 15 cm, packed It is known [Shields,1966] that isotopicfrac- with Dowex 50 X 8, 200-400 mesh). After most rionation effects can be minimized by very of the other elements were removed with 4 standard operational procedures during an- column volumes of 4 N HC1, the barium was alysis. It was deemed advisable, however, to collected in the following fraction of about 2 utilize a more reliable technique such as an in- column volumes of 4 N HC1. ternal isotopic standard of two isotopes.This Blank determinations showed that the barium technique,often called the double spiking tech- contamination introduced by the complete nique, was recently used by Wetherill [1964] chemical processingwas less than 5 X 10-g in his study on molybdenum.To distinguishbe- gram. This blank contribution to the sample tween laboratory effectscaused either by chem- was always less than 2%, which is negligible istry or massspectrometry, an isotopicinternal insofar as the isotopicratios are concerned.The standard or double spike was added to the sam- Ba concentrationswere, however,corrected for ples beforethe chemicalseparation. this small blank. ISOTOPIC ANALYSES OF BARIUM 3899 Mass spectrometry. The sampleof approxi- positionwas as shownin Table 1 for a typical mately 10-6 gram barium was depositedas the compositionof a mixture of doublespike plus chlorideand analyzedby meansof the single- sample.The Ba•/Ba •85ratios were always be.: filament (Ta) surface ionization technique.A tween 11 and 14. These ratios have been cor- single-focusing,30.48-cm radius, 60 ø sectortype, rected for the massspectrometer fractionation, programmablemagnetic field massspectrometer which was basedon the ratio Ba•/Ba •85.For all with digital output and with on-linedata proc- four samples this ratio was between 1.17 and essing[Wasserburg ei al., 1968,1969] wasused 1.18. Figure I showsthe variation of the ratio for most analyses.Some of the unspikedsam- Ba•37/Ba• as a function of the Ba•7 ion cur- ples were analyzedwith the same mass spec- rent normalized to the value of this ratio ob- trometer by usinga recorderfor analogoutput. tained at about 0.4 volt. Below 12 volts the The mass spectrometricdata were taken in input resistor can be consideredto be linear sets of ten completesweeps of the spectrum. within 0.1%. In a few casesin which data were Becauseof the programmablemagnetic field de- taken at intensities over 12 volts, corrections vice and the on-line data processing,one set of were applied for the nonlinearity. data for all isotopesincluding zeros on eachside Because of the wide range (up to 103) in of every peak couldbe taken within about 10 ion currents of the different isotopes,it was minutes. Systematicchanges in the isotopic necessaryto eliminate errors causedby the in- ratiosduring this time wereless than 2 parts in complete dischargeof the high input resistor 104 for all ratios. We therefore assume the frac- and the amplifier system. Time intervals be- tionation during each set to be constant.One tween data acquisition were established by analysisof a doublespiked sample consisted of making a time study of normal potassium,so six to ten sets taken at different intensities that any errors due to these sourceswere less rangingin most casesfrom about 0.5 to 12 than I part in 104 for all isotopes.This effect volts for Ba• with a 10•-ohm input res;stor.
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