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At least 163 records · Page 9

Refining Methods to Determine the Isotopic Composition of Uranium Particles by Laser Ablation MC-ICP-MS

We report on efforts to mitigate the generation of isotopic anomalies during the ablation of micrometer-sized uranium oxide particles and analysis by MC-ICP-MS. The results of testing on particles of U200 indicate that laser fluence and frequency can affect isotopic data produced by laser ablation, but no settings were tested that could eradicate the signal spiking effect and generation of anomalous isotopic data for 234U/238U and 236U/238U. These anomalies are more frequent in samples with higher 235U enrichments, which is expected given their higher abundances of 234U and 236U. Of the standards tested here, only U005-A was anomaly-free. Efforts to compare the laser traces for particles with normal and anomalous isotopic compositions showed subtle differences in the behavior of the 234U/238U and 236U/238U ratios. However, it would be challenging to identify anomalous data points from a population of unknowns using this distinction, i.e., this is unlikely to be diagnostic. Thus, using current analytical hardware, we cannot eradicate the signal spiking phenomenon and cannot unambiguously identify isotopic anomalies from laser ablation traces. Ultimately, laser ablation ICP-MS would either require dramatic improvement to the ablation process and generation of more homogenous aerosols and/or improvements to detector electronics to identify and correct for the spiking phenomenon. Even if the reliability of the technique could be improved, a broader question to address is whether current data quality is of a high enough standard for laser ablation MC-ICP-MS to be used as a complementary technique to LG-SIMS for Safeguards.

organic↗

Distribution, abundance and carbon isotopic composition of gaseous hydrocarbons in Big Soda Lake, Nevada - An alkaline, meromictic lake

The study of the distribution and isotopic composition of low molecular weight hydrocarbon gases at the Big Soda Lake, Nevada, has shown that while neither ethylene nor propylene were found in the lake, ethane, propane, isobutane and n-butane concentrations all increased with water column depth. It is concluded that methane has a biogenic origin in both the sediments and the anoxic water column, and that C2-C4 alkanes have biogenic origins in the monimolimnion water and shallow sediments. The changes observed in delta C-13/CH4/ and CH4/(C2H6 + C3H8) with depth in the water column and sedimeents are probably due to bacterial processes, which may include anaerobic methane oxidation and different rates of methanogenesis, and C2-to-C4 alkane production by microorganisms.

Oremland, R. S.↗

Stable Isotope Composition of Carbonates Formed in Low-Temperature Terrestrial Environments as Martian Analogs

We examine the carbon and oxygen isotope composition of carbonate minerals that formed in two low-temperature terrestrial environments. Field locations were chosen to represent environments where microcrystalline carbonates (caliches) form. Samples include caliche crusts collected from the tsekel zone of N. Yucatan, Mexico, as well as carbonate mud from the edge of a near-by salt pan, representing both ancient and modern-precipitated carbonates. Additional field samples of surface-coating caliche were collected from two volcanic fields in Arizona. Preliminary results indicate that there is an overall depletion of 18O and 13C as a function of the extent of meteoric diagenesis. These data are used as terrestrial analogs to gauge whether carbonates that have been found within Martian meteorites could possibly have formed under these or similar conditions on Mars.

Socki, Richard A.↗

Isotopic Composition of Silicon Carbide in the CO3 Chondrite Colony

Presolar grains have been identified in primitive members of all chondrite classes. The isotopic compositions of presolar grains provide probes of galactic evolution and nucleosynthesis in stars, while the abundances and characteristics of presolar grains contain a record of thermal processing in the solar system. Most of the detailed isotopic work has been done on SiC from Murchison and Orgueil, supplemented by a few studies of ordinary and enstatite chondrites. This work investigates SiC in the Colony CO3.O meteorite. SiC is present in Colony at a matrix-normalized abundance of approximately 3.7 ppm, much less than in CI chondrites and the matrixes of CM and primitive ordinary and enstatite chondrites. The abundances of SiC and other presolar grains in Colony seem to correlate with the chemical processing that produced CO3 chondrites. This implies that the known presolar grains experienced the same processing as the bulk CO3 material and assumes that the parent material was the same as that for other chondrites, including CI. That parent material is most plausibly the average material in the sun s parent molecular cloud. One test of this idea is to look for primary differences between SiC in Colony (and other meteorites) and that in CI and CM chondrites. True differences not related to thermal processing would falsify the assumption that all chondrite classes originated from the same reservoir of presolar dust.

Smith, J. B.↗

The isotopic composition of Fe and fragmentation nuclei with Z equals 17-25

Using the combined data from 1976 and 1977 balloon flights the isotopic composition of cosmic ray Fe and fragmentation nuclei with Z equals 17-25 have been determined. The telescope used in these studies contains two Cerenkov counters and four total energy counters with an overall mass resolution sigma equals 0.35-0.40 amu. For Fe, approximately 320 nuclei with C/C(max) less than 0.5 are mass analyzed with the result extrapolated to the cosmic ray source, Fe-56 equals 0.952, Fe-54 equals 0.048 plus or minus 0.030 and Fe-58 less than 0.030 of all Fe. Two other isotopes are found to have a significant source abundance, A-36 with an abundance of 0.048 plus or minus 0.013 x Fe and Ca-40 equals 0.088 plus or minus 0.016 x Fe at the source. The source abundance of all other isotopes is less than 0.015 x Fe at the 1 sigma level. Of these fragmentation isotopes there is evidence that most of the Cl-36 has decayed as well as possibly some Mn-54.

Webber, W. R.↗

Nucleosynthesis and the Isotopic Composition of Stardust

Various components have been isolated from carbonaceous meteorites with an isotopically anomalous elemental composition. Several of these are generally thought to represent stardust containing a nucleosynthetic record of their birthsites. This paper discusses the expected isotopic composition of stardust based upon astronomical observations and theoretical studies of their birthsites: red giants and supergiants, planetary nebulae, C-rich Wolf-Rayet stars, novae and supernovae. Analyzing the stardust budget, it is concluded that about 15% of the elements will be locked up in stardust components in the interstellar medium. This stardust will be isotopically heterogenous on an individual grain basis by factors ranging from 2 to several orders of magnitude. Since comets may have preserved a relatively unprocessed record of the stardust entering the solar nebula, isotopic studies of returned comet samples may provide valuable information on the nucleosynthetic processes taking place in the interiors of stars and the elemental evolution of the Milky Way.

Tielens, Alexander G. M.↗

The effects of terrestrial weathering on samarium-neodymium isotopic composition of ordinary chondrites

Following their fall to Earth, meteorites experience weathering. In this systematic study, we evaluate the trace element composition of ordinary chondrites from the Antarctic cold desert, and Atacama (Chile) and Lut (Iran) hot deserts, with an emphasis on rare earth elements (REE). Our data confirms that terrestrial weathering of meteorites in hot deserts changes their trace element (Sr, Ba, REE, Hf, Th, and U) concentrations. However, weathering effects in majority of Antarctic samples are limited to slight Ba, REE, Hf, and Th depletions and in some case to U enrichment. In comparison to the Antarctic meteorites, hot desert samples show greater disturbances and REE fractionation relative to the average fall values. We measured the Sm-Nd isotopic composition of the hot desert meteorites that have heavily affected REE compositions. Our Sm-Nd isotopic data show a significant effect of terrestrial weathering evidenced by non-CHUR (147)Sm/(144)Nd and (143)Nd/(144)Nd ratios. Measurements show a higher variation and lower values of (147)Sm/(144)Nd for the Atacama samples than those from the Lut Desert. Deviations from CHUR (147)Sm/(144)Nd value are in positive accordance with the degree of La/Lu fractionation caused by weathering. The ɛNd values of Atacama and Lut deserts meteorites range from −2.20 to +1.61, which is wider than the −1.07 to +0.64 range for falls. We suggest that disturbance of primary Sm/Nd ratios resulting from mixing with terrestrial components originating from soil during weathering is responsible for lower (147)Sm/(144)Nd ratio in these meteorites. The majority of the Atacama meteorites regardless of their weathering degrees have their REE compositions and ɛNd affected by terrestrial contamination. Both (147)Sm/(144)Nd ratio and ɛNd values show no straightforward relationship with weathering degree. However, in both cases the samples with the highest negative isotopic disturbances are H chondrites from the Atacama and Lut deserts. In addition, Ba concentration shows a negative correlation with (147)Sm/(144)Nd ratio. Care must be taken into account while dealing with samples collected from hot deserts, even fresh-looking ones.

Isotope geochemistry↗

Water Vapor and its Isotopic Composition in the Upper Troposphere and Stratosphere

Any theory of water vapor in the tropical tropopause layer (TTL) must explain both the abundance and isotopic composition of water there. We have previously presented a model of the TTL that simulated the abundance of water vapor as well as the details of the vertical profile. That model included the effects of 'overshooting convection', which injects dry air directly into the TTL. Here, we present results for the model after modifying it to include water's stable isotope HDO. The model is capable of accurately simulating the recently observed, nearly uniform HDO depletion (delta D) in the TTL. We find that lofted ice is necessary to accurately simulate the profile of delta D in the TTL, as has been suggested previously. We also find that vertical mixing due to overshooting convection plays an important role in maintaining the observed profile. Finally, any theory of lofted ice requires a complementary source of dry air in the TTL; without that, the TTL will rapidly saturate and the lofted ice will not evaporate.

Dessler, A. E.↗

The isotopic composition of cosmic-ray beryllium and its implication for the cosmic ray's age

We report a new measurement of the cosmic-ray isotopic composition of beryllium in the low-energy range from 35 to 113 MeV per nucleon. This measurement was made using the High Energy Telescope of the CRS experiment on the Voyager 1 and 2 spacecraft during the time period from 1977 to 1991. In this overall time period of 14 years the average solar modulation level was about 500 MV. The cosmic-ray beryllium isotopes were completely separated with an average mass resolution sigma of 0.185 amu. The isotope fractions of Be-7, Be-9, and Be-10 obtained are 52.4 +/- 2.9%, 43.3 +/- 3.7%, and 4.3 +/- 1.5%, respectively. The measured cosmic-ray abundances of Be-7 and Be-9 are found to be in agreement with calculations based on standard Leaky-Box model for the interstellar propagation of cosmic-ray nuclei using the recent cross sections of the New Mexico-Saclay collaboration. From our observed ratio Be-10/Be = 4.3 +/- 1.5% we deduce an average interstellar density of about 0.28 (+0.14, -0.11) atoms/cu cm, and acosmic-ray lifetime for escape of 27 (+19, -9) x 10(exp 6) years. The surviving fraction of Be-10 is found to be 0.19 +/- 0.07. Modifications to the conclusions of the Leaky-Box model when a diffusion + convection halo model for propagation is used are also considered.

Lukasiak, A.↗

The charge and isotopic composition of Z equals 7-16 cosmic ray nuclei at their source

Using the combined data from our 1976 and 1977 balloon flights, the charge and isotopic composition of Z equals 7-16 cosmic ray nuclei have been determined. A low abundance of both N and Ne in the cosmic ray source relative to solar cosmic rays is observed. However, the cosmic ray source ratio, Ne-22/Ne is 2.75 plus or minus 0.42 times the solar ratio. A possible enhancement of the Mg-26/Mg ratio, which is 1.29 plus or minus 0.14 times the solar ratio is also observed.

Webber, W. R.↗

Silicon isotopic composition in large meteoritic SiC particles and Na-22 origin of Ne-22

Large SiC particles extracted from acid-insoluble residues of carbonaceous chondrites are isotopically anomalous in both silicon and carbon and contain isotopically extreme noble gases. These particles are thought to have originated in mass outflows from red giant stars and to have existed in the interstellar medium at the time the solar system formed from an interstellar cloud. Calculations show that the silicon isotope correlations in those large SiC particles can be generated only in the most massive carbon stars. Consequently, the almost pure Ne-22 in those particles must be interpreted as the condensation of radioactive Na-22 in the particles as they flowed away from the stars. The Na-22 is produced through proton capture by Ne-21 at the base of the surface convection zone. Ne-22 does not exist abundantly in helium shells hot enough to burn magnesium, which is necessary to establish the measured silicon isotopic composition.

Brown, Lawrence E.↗

The carbon-isotopic composition of Proterozoic carbonates: Riphean successions from northwestern Siberia (Anabar Massif, Turukhansk Uplift)

Thick carbonate-dominated successions in northwestern Siberia document secular variations in the C-isotopic composition of seawater through Mesoproterozoic and early Neoproterozoic (Early to early Late Riphean) time. Mesoproterozoic dolomites of the Billyakh Group, Anabar Massif, have delta 13C values that fall between 0 and -1.9 permil versus PDB, with values in the upper part of the succession (Yusmastakh Formation) consistently higher than those of the lower (Ust'-Il'ya and Kotuikan formations). Consistent with available biostratigraphic and radiometric data, delta 13C values for Billyakh carbonates compare closely with those characterizing early Mesoproterozoic carbonates (about 1600-1200 Ma) worldwide. In contrast, late Mesoproterozoic to early Neoproterozoic limestones and dolomites in the Turukhansk Uplift exhibit moderate levels of secular variation. Only the lowermost carbonates in the Turukhansk succession (Linok Formation) have delta 13C values that approximate Billyakh values. Higher in the Turukhansk succession, delta 13C values vary from -2.7 to +4.6 permil (with outliers as low as -5.0 permil interpreted as diagentically altered). Again, consistent with paleontological and radiometric data, these values compare well with isotopic values from 1200 to 850 Ma successions elsewhere. Five sections measured in different parts of the Turukhansk basin show nearly identical patterns of variation, confirming that carbonate delta 13C correlates primarily with time and not facies. The Siberian sections illustrate the potential of integrated biostratigraphic and chemostratigraphic data in the intra- and interbasinal correlation of Mesoproterozoic and early Neoproterozoic rocks.

NASA Discipline Exobiology↗

Cosmic-ray isotopic composition of C, N, O, Ne, Mg, Si nuclei in the energy range 50-200 MeV per nucleon measured by the Voyager spacecraft during the solar minimum period

The isotopic composition of C, N, O, Ne, Mg, Si cosmic ray nuclei has been measured in the energy range 50-200 MeV per nucleon using data collected by the High-Energy Telescope of the cosmic-ray subsystem experiment on the Voyager 1 and 2 spacecraft. These data were collected during the period of minimum solar activity in 1986-1988 at an average distance of 27 AU with an effective solar modulation that was much less than at the Earth. The isotope analysis, based on the energy loss - total energy method, has a mass resolution of 0.2 amu for carbon and 0.4 amu at silicon. We find a (C-13)/(C-12) ratio slightly lower and a (O-18)/(O-16) ratio slightly enhanced over their solar system value. We also observe the previously reported enhancement of the (Ne-22)/(Ne-20) ratio relative to solar at the cosmic-ray source but only a weak, if any, enhancement of the (Mg-25)/(Mg-24), (Mg-26)/(Mg 24), and (Si-30)/(Si-28) ratios.

Lukasiak, A.↗

Grains of anomalous isotopic composition from novae

The effects of grain formation in nova ejecta are studied in order to model the optical and infrared luminosities schematically and to identify the anomalies of isotopic composition that should be present in large abundance in these grains. The large carbon concentration makes rapid and efficient grain formation possible and accounts for the peculiar luminosities observed in Nova Serpentis 1970. In the anticipated range of nova conditions, rapid addition of hot protons during the outburst produces large overabundances of C-13, O-18, Na-22, Al-26, Si-30, and perhaps others. Anomalous C-14 is expected subsequent to the C-13(alpha, n)O-16 reaction, and will be trapped in grains formed by subsequent atmospheric loss. Each of these anomalies may have been detected on the moon (due to accretion of interstellar dust) or in carbonaceous chondrites. Perhaps nova grains are responsible.

Clayton, D. D.↗

The isotopic composition of cosmic ray calcium

Data from the high energy cosmic ray experiment on the international sun earth explorer 3 (ISEE-3) spacecraft have been used to study the isotopic composition of cosmic ray calcium at an energy of approx. 260 MeV/amu. The arriving calcium is found to consist of (32 + or - 6)%. A propagation model consistent with both the light and the subiron secondary element abundances was used for the interpretation of the observed calcium composition. The measured 42Ca+43Ca+44Ca abundance is consistent with the calculated secondary production, while the 40Ca abundance implies a source ratio of 40Ca/Fe = (7.0 + or - 1.7)%.

Krombel, K. E.↗