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NASA NTRS1973

Ultrafiltration by a compacted clay membrane. I - Oxygen and hydrogen isotopic fractionation. II - Sodium ion exclusion at various ionic strengths.

Laboratory experiments were carried out to determine the magnitude of the isotopic fractionation of distilled water and of 0.01N NaCl forced to flow at ambient temperature under a hydraulic pressure drop of 100 bars across a montmorillonite disk compacted to a porosity of 35% by a pressure of 330 bars. The ultrafiltrates in both experiments were depleted in D by 2.5% and in O-18 by 0.8% relative to the residual solution. No additional isotopic fractionation due to a salt-filtering mechanism was observed at NaCl concentrations up to 0.01N. Adsorption is most likely the principal mechanism which produces isotopic fractionation, but molecular diffusion may play a minor role. The results suggest that oxygen and hydrogen isotopic fractionation of ground water during passage through compacted clayey sediments should be a common occurrence, in accord with published interpretations of isotopic data from the Illinois and Alberta basins. It is shown how it is possible to proceed from the ion exchange capacity of clay minerals and, by means of the Donnan membrane equilibrium concept and the Teorell-Meyer-Siever theory, develop a theory to explain why and to what extent ultrafiltration occurs when solutions of known concentration are forced to flow through a clay membrane.

Coplen, T. B.↗

NASA NTRS1974

Isotopic composition of lithium, potassium, rubidium, and strontium in lunar surface material

The isotopic composition of alkali and alkaline earth elements in the Luna 16 regolith was investigated by the method of thermionic emission, without chemical separation. The isotopic composition of the lithium in two regolith samples did not differ (within the limits 0.5 percent) from the mean of the terrestrial reference standard. At the same time, the observed difference (1 percent) in the isotopic composition of lithium between the samples requires further investigation and confirmation. The isotopic compositions of K and Rb did not differ within the limits of experimental error from the isotopic composition of the reference standard.

Zaslavskiy, V. G.↗

NASA NTRS1978

On the origin and evolution of isotopes of carbon, nitrogen, and oxygen

Calculations of CNO processing in stellar envelopes, based on theoretical nucleosynthesis rather than empirical abundances in evolving stars, are presented and used in two models for the chemical evolution of the solar neighborhood. Seven stable isotopes are considered: C-12, C-13, N-14, N-15, O-16, O-17, and O-18. The two models ('infall' and 'initial-burst') represent extremes of types consistent with general constraints and include theoretical estimates of other nucleosynthesis sites and yields for CNO isotopes. The results obtained are found to predict that all CNO isotopes are produced mainly by stars with lifetimes much less than the age of the Galaxy (even at the present time when low-mass stars have the greatest death rate), so that isotopic ratios evolve very slowly after the first few billion years. Consequences of these slow changes are that the isotopic ratios cannot be employed to test between alternative hypotheses and that galactic evolution does not seem to be able to account for the apparent difference between the C-13/C-12 ratio in the solar system and in molecular clouds. The predicted envelope processing is shown to lead to approximately the solar-system values for the C-13/C-12 and O-17/O-16 abundance ratios but to a N-14/C-12 ratio that is too small by at least a factor of 2.

Dearborn, D.↗

NASA NTRS1978

On strontium isotopic anomalies and odd-A p-process abundances

Several aspects of the nucleosynthesis of Sr isotopes are considered in an attempt to shed light on the problem of the Sr isotopic anomalies discovered in an inclusion of the Allende meteorite. Decomposition of the Sr isotopes into average r-, s-, and p-process nucleosynthetic classes is performed. It is suggested that the Allende inclusion most likely has an excess of s-process Sr and that the initial Sr-87/Sr-86 isotopic ratio is probably slightly more primitive than basaltic achondrites. The results also show that Sn-115 is mostly due to the r-process and that odd-A yields are very small. It is concluded that if the Sr anomaly in the inclusion is an average s enhancement, it argues somewhat in favor of a model of gas/dust fractionation of s and r isotopes during accumulation of the inclusion parent in the protosolar cloud.

Clayton, D. D.↗

NASA NTRS1979

The isotopic composition of Nd in different ocean masses

The paper examines the isotopic composition of Nd in marine environments. The Sm-Nd data for authigenic ferromanganese sediments indicate that the Atlantic, Pacific, and Indian Oceans have a distinct range in Nd isotopic composition characteristics of each ocean basin and reflect the dissolved load of Nd in the water mass. Measurements of the Nd isotopic seawater composition of seawater indicate that the rare earth elements (REE) in ferromanganese sediments are derived by direct precipitation of these elements out of seawater. It is believed that the Nd isotopic variations in these sediments represent true variations in the dissolved Nd isotopic composition which reflect the age and (Sm-147)/(Nd-144) ratios of the continental masses sampled believed to be the major source of REE in seawater.

Piepgras, D. J.↗

NASA NTRS1981

The isotopic composition of uranium and lead in Allende inclusions and meteoritic phosphates

The isotopic compositions of uranium and lead in Ca-Al-rich inclusions from the Allende chondrite and in whitlockite from the St. Severin chondrite and the Angra dos Reis achondrite are reported. Isoptopic analysis of acid soluble fractions of the Allende inclusions and the meteoritic whitlockite, which show isotopic anomalies in other elements, reveals U-235/U-238 ratios from 1/137.6 to 1/138.3, within 20 per mil of normal terrestrial U abundances. The Pb isotopic compositions of five coarse-grained Allende inclusions give a mean Pb-207/Pb-206 model age of 4.559 + or - 0.015 AE, in agreement with the U results. Pb isotope ratios of two fine-grained inclusions and a coarse-grained inclusion with strong mass fractionation and some nonlinear isotopic anomalies indicate that the U-Pb systems of these inclusions have evolved differently from the rest of Allende. Th/U abundance ratios in the Allende inclusions and meteoritic phosphate are found to range from 3.8 to 96, presumably indicating an optimal case for Cm/U fractionation, although the normal U concentrations do not support claims of abundant live Cm-247 or Cm-247/U-238 fractionation at the time of meteorite formation, in contrast to previous results. A limiting Cm-247/U-235 ratio of 0.004 at the time of meteorite formation is calculated which implies that the last major r process contribution at the protosolar nebula was approximately 100 million years prior to Al-26 formation and injection.

Chen, J. H.↗

NASA NTRS1982

A reexamination of the RB-SR isotopic systematics of lunar breccia 12013

Lunar breccia 12013 is one of the few rocks for which isotopic evidence has been interpreted as indicating a 4.5-AE age, and it is the only lunar rock which contains abundant granitic material that may date back to the initial lunar differentiation. An investigation of 12013 conducted by Quick et al. (1981) has led to the conclusion that 12013 is an extremely complex mixture of impact-generated melt and clastic components of uncertain affinities. It was found that the granitic component in 12013 need not be any older than 4.16-4.17 AE. In the present study a model is presented for the Rb-Sr evolution of 12013 which explains the isotopic data without resorting to a 4.5-AE age for any component. Attention is given to petrographic constraints, isotopic investigations, and an evaluation of the Rb-Sr isotopic data. It is concluded that lunar rock 12013 is an extremely complex polymict breccia in which the Rb-Sr isotopic systematics have been greatly influenced by mixing during breccia formation and by subsequent reequilibration.

Quick, J. E.↗

NASA NTRS1983

Importance of the Lu-Hf isotopic system in studies of planetary chronology and chemical evolution

The Lu-176-Hf-176 isotope method and its applications in earth sciences are discussed with regard to planetary-evolution studies. From new data on basalts from oceanic islands, Hf-176/Hf-177 and Nd-143/Nd-144 are found to display a single linear isotopic variation in the suboceanic mantle, whereas considerable divergences occur in Hf-176/Hf-177-Sr-87/Sr-86 and Nd-143/Nd-144-Sr87/Sr-86 diagrams. With the acquisition of further Hf-Sr-Nd isotopic data, these discordant Sr-87/Sr-86 relationships may allow a distinction between processes such as mantle metasomatism, influence of sea-water altered material in the magma source, or recycling of sediments into the mantle. The best quality Hf isotope data are obtained from granitoid or zircons, and are most suitable for studying ancient terrestrial Hf isotopic variations. Lu-Hf is shown to be a viable method for dating ancient terrestrial and extraterrestrial samples, but is unlikely to find wide application in pure chronological studies because it offers little advantage over existing methods.

Patchett, P. J.↗

NASA NTRS1983

Further isotopic studies of heavy nuclei in the 9/23/78 solar flare

The isotopes considered range from He to Mg (Z from 2 to 12). A more accurate value of the Ne-22/Ne-20 ratio is obtained by extending the energy interval for isotope analysis. A significant difference persists between the Ne-22/Ne-20 ratio in this flare and that for the solar wind. How the sun can apparently emit two distinct isotopic components remains a question. Although relatively little is known about the solar wind isotopic composition, it does not appear that the solar wind isotopes have been altered by a simple mass-dependent fractionation process. Reference is made to models that have been proposed which might produce selective enhancements.

Mewaldt, R. A.↗

NASA NTRS1984

A high-resolution study of the isotopes of solar flare nuclei

Individual isotopes of the elements He, C, N, O, Ne, and Mg with energies from 5 to 50 MeV per nucleon have been resolved in energetic flare particles during the September 23, 1978 solar flare event. In addition, an earlier determination of Ne-22/Ne-20 in this flare was improved on by extending the energy interval for isotope analysis. A significant difference between the isotopic composition of solar flare and solar wind neon is found, which is compared to similar evidence from studies of solar energetic particles implanted in lunar and meteoritic samples. Although limited by statistics, the measurements of He, C, N, O, and Mg isotopes are consistent with typical isotopic abundances found in other samples of solar system material. The ensemble of these results is used to test for the possibility of mass-dependent fractionation during solar flare acceleration and propagation.

Mewaldt, R. A.↗

NASA NTRS1984

Ca isotopes in refractory inclusions

The present absolute isotope abundance measurements of Ca in Ca-Al-rich inclusions from the Allende and Leoville meteorites show the extreme rarity of nonlinear isotope effects in Ca, in sharp contrast to the endemic effects in Ti. The Ca in the Ca-Al-rich inclusions shows mass-dependent isotope fractionation effects whose range is a factor of 20 wider than the range previously established for bulk meteorites and for terrestrial and lunar samples. A correlation is found between Ca and Mg isotope fractionation effects and inclusion type, and a possible correlation between isotope fractionation and rare earth element abundance patterns is discussed.

Niederer, F. R.↗

NASA NTRS1984

Oxygen isotopes in deep sea spherules

The determination of the genetic relationships between the dust and small particles in the solar system, and the meteorites and larger bodies are examined. Oxygen isotopes proved useful in the identification of such relationships between one meteorite group and another. Of the various samples of submillimeter extraterrestrial particles available for laboratory study, only the deep sea spherules are abundant enough for precise oxygen isotope analysis using existing techniques. Complications arise in interpretation of the isotopic data, since these particles were melted during passage through the Earth's atmosphere, and have been in contact with seawater for prolonged periods. Spherules that were originally silicates are considered with the originally metallic ones to deduce their preterrestrial isotopic compositions. The type 1 spherules which enter the atmosphere as metallic particles, contain only atmospheric oxygen. The type S spherules contain a mixture of atmospheric oxygen and their original extraterrestrial oxygen. It is suggested that the Earth's mesosphere is strongly enriched in heavy isotopes of oxygen at altitudes near 90 km at which the iron particles are oxidized. Fractionation due to the combined diffusion of O atoms and O2 molecules may be responsible.

Mayeda, T. K.↗

NASA NTRS1984

Ca isotope variations in Allende

Ca-isotope measurements of Allende Ca-Al-rich inclusions (CAIs), together with those on an apatite-enriched fraction from Orgueil, indicate the existence of widespread excesses on the neutron-rich isotope Ca-48. Isotopic anomalies are noted in 7 out of 11 CAIs analyzed. This abundance of isotopic excesses places Ca alongside Ti and O, although no clear correlation has yet been found between Ca-48 and Ti-50, which are thought to be coproduced by neutron-rich nucleosynthetic processes within stars. It is suggested that the higher volatility of Ca, by comparison with Ti compounds, led to a variable dilution with isotopically normal Ca in vaporization and recondensation processes in stellar envelopes, the interstellar medium, and/or the solar nebula.

Jungck, M. H. A.↗

NASA NTRS1983

Oxygen isotopic compositions of chondrules in Allende and ordinary chondrites

The ferromagnesian chondrules in Allende follow a trend in the oxygen three-isotope plot that diverges significantly from the 16-O mixing line defined by light and dark inclusions and the matrix of the meteorite. The trend probably results from isotopic exchange with an external gaseous reservoir during the process of chondrule formation sometime after the establishment of the isotopic compositions of the inclusions and matrix. The Allende chondrules approach, but do not reach, the isotopic compositions of chondrules in unequilibrated ordinary chondrites, implying exchange with a similar ambient gas, but isotopically different solid precursors for the two types of meteorite.

Clayton, R. N.↗

NASA NTRS1985

Constraints on chondrule origin from petrology of isotopically characterized chondrules in the Allende meteorite

The petrologic and chemical properties of the ferromagnesian chondrules in the Allende carbonaceous chondrite were examined in terms of the isotopic composition and the correlations between isotopic patterns. Areas of thin sections were studied with a SEM and bulk chemical fractions of 12 constituents were quantified to calculate correlations with petrologic features. A possible correlation between (CaO + Al2O2)/MgO and oxygen isotopes imply the formation of oxygen isotopic compositions in the chondrules by exchanges between isotopically heavy nebular gases and O-16 enriched solids. Different rates of gaseous exchange occurred with the various types of chondrules. Factors which may have controlled the exchanges are discussed.

Mcsween, H. Y., Jr.↗

NASA NTRS1987

Rare earth element transport in the western North Atlantic inferred from Nd isotopic observations

The relationship between the Nd isotopic composition in the Atlantic waters and the origin and circulation of the water masses was investigated. Samples were collected in the western North Atlantic between 7 and 54 deg N. The isotopic composition (Nd-143/Nd-144 ratios) showed extensive vertical structure at all locations. In regions where a thermocline was well-developed, large isotopic shifts were observed across the base of the thermocline, while regions without a thermocline were characterized by much more gradual shifts in isotopic composition with depth. The data reveal an excellent correlation between the Nd isotopic distribution in the western North Atlantic water column and the distribution of water masses identified from temperature and salinity measurements.

Piepgras, D. J.↗

NASA NTRS1987

The effect of pressure and excitation energy on the isotopic fractionation in the formation of ozone by discharge of O2

Isotopic fractionation processes in the formation of O3 by discharge (at 20 kV and 3 MHz) of O2 in a fused silica container at 77 K are investigated experimentally, with a focus on the effects of changes in the isotopic abundances in the predischarge O2, the O2 pressure, and the excitation energy on the isotope abundances in the postdischarge O2 and O3. The results are presented in extensive tables and graphs and characterized in detail, and good general agreement is found with data obtained using 60-kHz excitation (Yang and Epstein, 1987). It is shown that O-17 and O-18 enrichment of the residual O2 (when the predischarge gas is enriched) or of the O3 (when atmospheric isotope abundances are used) can occur independently of one another. It is inferred that the rate of anharmonic predissociation of vibrationally hot O3 depends on the symmetry and mass of the O3 molecules. The significance of the present findings for studies of anomalous oxygen isotope abundances in meteorites is indicated.

Yang, Jongmann↗

NASA NTRS1987

O-16 excesses in Murchison and Murray hibonites - A case against a late supernova injection origin of isotopic anomalies in O, Mg, Ca, and Ti

Ion probe measurements of the oxygen isotopic composition of seven hibonite samples from the CM chondrites Murchison and Murray are reported. All samples show large O-16 excesses relative to terrestrial oxygen. The data for all samples plot along the carbonaceous chondrite O-16-rich mixing line and show no evidence for isotopic mass fractionation effects characteristic of FUN inclusions. These hibonites have the largest Ca-48 and Ti-50 isotopic anomalies found to date; thus there is no intrinsic relationship between anomalies of a nucleosynthetic origin and isotopic mass fractionation effects. The large O-16 excess seen in the sample with the largest measured Ca-48 and Ti-50 depletions argues against a late injection of exotic material from a nearby supernova as a source for the isotopic anomalies.

Fahey, A. J.↗