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NASA NTRS2012

Isotopic Anomalies in Primitive Solar System Matter: Spin-State Dependent Fractionation of Nitrogen and Deuterium in Interstellar Clouds

Organic material found in meteorites and interplanetary dust particles is enriched in D and N-15, This is consistent with the idea that the functional groups carrying these isotopic anomalies, nitriles and amines, were formed by ion-molecule chemistry in the protosolar core. Theoretical models of interstellar fractionation at low temperatures predict large enrichments in both D and N-15 and can account for the largest isotop c enrichments measured in carbonaceous meteorites, However, more recent measurements have shown that, in some primitive samples, a large N-15 enrichment does not correlate with one in D, and that some D-enriched primitive material displays little, if any, N-15 enrichment. By considering the spin-state dependence in ion-molecule reactions involving the ortho and para forms of H2, we show that ammonia and related molecules can exhibit such a wide range of fractionation for both N-15 and D in dense cloud cores, We also show that while the nitriles, HCN and HNC, contain the greatest N-15 enrichment, this is not expected to correlate with extreme D emichment. These calculations therefore support the view that Solar System N-15 and D isotopic anomalies have an interstellar heritage, We also compare our results to existing astronomical observations and briefly discuss future tests of this model.

Wirstrom, Eva S.↗

NASA NTRS1994

Search for isotopic anomalies in oldhamite (CaS) from unequilibrated (E3) enstatite chondrites

The Ca isotopic compositions of 32 oldhamite (CaS) grains from the Qingzhen (EH3), MAC88136 (EL3), and Indarch (EH4) enstatite chondrites were determined by ion microprobe mass spectrometry. Also measured were the S isotopic compositions of eight oldhamite, two niningerite (MgS), and seven troilite (FeS) grains. The S isotopic compositions of all minerals are normal, but oldhamite grains of the first two meteorites exhibit apparent small Ca-48 excesses and deficits that are correlated with isotopic mass fractionation as determined from the Ca-40-Ca-44 pair. The interpretation of these results is complicated by the fact that none of the established mass fractionation laws can account for the data in the Norton County oldhamite standard. The method of analysis is carefully scrutinized for experimental artifacts. Neither interferences nor any known mass frationation effect can satisfactorily explain the observed small deviations from normal isotopic composition. If these are truly isotopic anomalies, they are much smaller than those observed in hibonite. The nucleosynthetic origin of Ca isotopes is discussed.

Lundberg, Laura L.↗

NASA NTRS1988

Isotopic anomalies - Chemical memory of Galactic evolution

New mechanisms for the chemical memory of isotopic anomalies are proposed which are based on the temporal change during the chemical evolution of the Galaxy of the isotopic composition of the mean ejecta from stars. Because of the differing temporal evolution of primary and secondary products of nucleosynthesis, the isotopic composition of the bulk interstellar medium changes approximately linearly with time, and thus any dust component having an age different from that of average dust will be isotopically anomalous. Special attention is given to C, O, Mg, Si, and isotopically heavy average-stellar condensates of SiC.

Clayton, Donald D.↗

NASA NTRS1994

Isotopically distinct reservoirs in the solar nebula: Isotope anomalies in Vigarano meteorite inclusions

The isotopic compositions of Mg, Ca, Ti, Cr, Zn, Sr, Ba, Nd, and Sm were measured in four relatively unaltered refractory inclusions from the Vigarano carbonaceous chondrite meteorite. Three of the inclusions (USNM 1623-2, 1623-3, and 1623-8) show similar Mg, Ca, Ti, and Cr isotopic compositions to those found in most inclusions in the Allende carbonaceous chondrite. This indicates that these Vigarano inclusions sampled the same isotopic reservoirs as the majority of the Allende inclusions that isotope signatures in the latter were not significantly modified by the secondary alteration that permeates most Allende inclusions. In contrast, inclusion 1623-5 has large deficits in Mg-26, Ca-48, and Ti-50 and small but distinct Cr-54, Zn-66, Sr-84, Ba-135, Ba-137, and Sm-144 anomalies. The magnitudes of these unusual anomalies in the refractory elements are within analytical uncertainty of those found in the Allende 'FUN" inclusion C1, yet 1623-5 has a very different bulk chemical composition from C1. The fact that 1623-5 and C1 have identical isotopic anomalies yet have significantly distinct major and trace element contents provide convincing evidence for the presence of isotopically distinct reservoirs in the early solar system.

Loss, R. 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 NTRS1981

Ubiquitous isotopic anomalies in Ti from normal Allende inclusions

A novel technique for the high-precision isotopic analysis of titanium was applied to three terrestrial rocks and coarse- and fine-grained Allende inclusions. Repeated analyses of the three terrestrial rocks gave excellent agreement with a Ti metal standard. All seven Allende inclusions were previously determined to contain isotopically normal Nd and/or Sm, indicating that none belongs to a small group of peculiar intrusions. The discovery of widespread Ti isotopic anomalies in normal Allende inclusions establishes Ti as the first non-noble gas element studied since oxygen to show such isotopic heterogeneity. A survey of nucleosynthetic origins of Ti isotopes suggests that the dominant Ti-50 excesses in these inclusions are due to the relative enrichment of isotopes synthesized during hydrostatic burning in, or near, the core of a massive star.

Niemeyer, S.↗

NASA NTRS1978

Isotopic anomalies from neutron reactions during explosive carbon burning

The possibility that the newly discovered correlated isotopic anomalies for heavy elements in the Allende meteorite were synthesized in the secondary neutron capture episode during the explosive carbon burning, the possible source of the O-16 and Al-26 anomalies, is examined. Explosive carbon burning calculations under typical conditions were first performed to generate time profiles of temperature, density, and free particle concentrations. These quantities were inputted into a general neutron capture code which calculates the resulting isotopic pattern from exposing the preexisting heavy seed nuclei to these free particles during the explosive carbon burning conditions. The interpretation avoids the problem of the Sr isotopic data and may resolve the conflict between the time scales inferred from 1-129, Pu-244, and Al-26.

Lee, T.↗

NASA NTRS1979

Grain carriers of isotopic anomalies

The dynamics of grain motion through gas are examined in terms of the injection of isotopically anomalous (compared to solar abundances) material into the early solar nebula. Calculations indicate that the injected grains cannot penetrate to the center of any of a range of reasonable configurations, suggesting the formation of an edge region enriched in injected material. Furthermore, the dynamical behavior of grains in turbulent flows indicates that pockets of grains can have some resistance to turbulent diffusion. The constraints developed here are used to delineate a set of consistent, injected-grain models for the origin of the isotopic anomalies in meteorite inclusions.

Margolis, S. H.↗

NASA NTRS1978

An interpretation of special and general isotopic anomalies in r-process nuclei

My analysis of new discoveries by McCulloch and Wasserburg of Ba and Nd isotopic anomalies in inclusions of the Allende meteorite argues that (1) these anomalies contain special extinct radioactivities resulting from radioactive decay within grains formed in and ejected from the supernova interior, (2) the inclusions studied are fused assemblies of interstellar grains that were never totally vaporized, and (3) theoretical separation into r and s abundances suggests that fluctuations between r and s components has occurred during the accumulation processes. These points lend support to a new chemical picture of the early solar system that I have developed, although many interpretations remain possible. Measurements of the neutron-capture cross sections of Nd isotopes are urgently needed to experimentally validate these conclusions.

Clayton, D. D.↗

NASA NTRS1991

Hibonite-bearing microspherules - A new type of refractory inclusions with large isotopic anomalies

This paper presents petrographic description as well as results on the major- and trace-element chemistry and on Mg, Ca, and Ti isotopic compositions of three refractory inclusions, including 3413-1/31 inclusion from Lance and Murchison 7-228 and 7-753, the mineralogy of which is dominated by the oxide minerals spinel, hibonite, and perovskite. The microspherules examined seem to constitute a separate class of refractory inclusions, characterized by a distinct morphology and mineralogy; large excesses of Ca-48 and Ti-50, and Mg-26 depletions. It is suggested that this type of inclusions must have formed early, prior to the dilution of isotopic anomalies by mixing processes, and in an area characterized by excesses of Ca-48 and Ti-50, depletions of Mg-26, and a lack of Al-26.

Ireland, T. R.↗

NASA NTRS1979

On isotopic anomalies in samarium

The solar isotopic composition of Sm is decomposed into s, r, and p components. The anomaly pattern discovered by Lugmair et al. (1978) in EK1-04 Allende inclusion can be presented as a fractionation of the average s-pattern from the average r-pattern. This representation requires a fractionation of 0.029%/(amu) and either (1) a 0.42% deficiency of s relative to r and a 0.15% deficiency of p relative to r, or (2) a 0.42% excess of r relative to s and a 0.27% excess of p relative to s. The nature of this anomaly suggest a systematic physical fractionation of r, s, and p nuclei from each other in the initial condition leading to EK1-04. A neighboring supernova injection would not be expected to produce this anomaly.

Clayton, D. D.↗

NASA NTRS2015

Strong Water Isotopic Anomalies in the Martian Atmosphere: Probing Current and Ancient Reservoirs

We measured maps of atmospheric water (H2O) and its deuterated form (HDO) across the martian globe, showing strong isotopic anomalies and a significant high deuterium/hydrogen (D/H) enrichment indicative of great water loss. The maps sample the evolution of sublimation from the north polar cap, revealing that the released water has a representative D/H value enriched by a factor of about 7 relative to Earth's ocean [Vienna standard mean ocean water (VSMOW)]. Certain basins and orographic depressions show even higher enrichment, whereas high-altitude regions show much lower values (1 to 3 VSMOW). Our atmospheric maps indicate that water ice in the polar reservoirs is enriched in deuterium to at least 8 VSMOW, which would mean that early Mars (4.5 billion years ago) had a global equivalent water layer at least 137 meters deep.

Research Support, U.S. Gov't, Non-P.H.S.↗

NASA NTRS1978

A local proton irradiation model for isotopic anomalies in the solar system

An attempt is made to explain the O-16 and Al-26 anomalies observed in solar-system bodies in the framework of a local irradiation model wherein a small amount of solar system matter of normal isotopic composition was irradiated by energetic protons from the primeval sun. Several isotopic constraints are summarized with which the model should be consistent, and a proton energy distribution and fluence and a target elemental composition are chosen such that the extraordinary component produced by irradiation satisfies the constraints. Detailed attention is given to the relevant oxygen reactions, Al-26 production, and effects of proton irradiation on isotopes of Mg, Ca, and Ba. A scenario is outlined which satisfies all the constraints. Consequences of the model are discussed with respect to the isotopic anomalies observed in Allende inclusions.

Lee, T.↗

NASA NTRS1985

A spectacular nitrogen isotope anomaly in Bencubbin

Results of isotopic measurements on an unusual stony-iron meteorite named Bencubbin, which was found in Western Australia in 1930, are reported. Nitrogen from both the metallic and stony parts of the Bencubbin meteorite was analyzed, and in both materials large excesses of (15)N were found, resulting in values of the (14)N/(15)N abundance ratios as low as 137. That is, (15)N is enriched in Bencubbin by about a factor of two relative to terrestrial nitrogen. This is the largest (15)N enrichment of any known natural material. The effect is so large that chemical processes are probably inadequate to account for it. Nuclear processes which may be responsible for the anomalous isotope abundance are discussed.

Prombo, C. A.↗

NASA NTRS1984

Titanium isotopic anomalies in meteorites

Studies of Ti isotopic compositions have shown that virtually every Ca-Al-rich Allende inclusion contains anomalous Ti. The present investigation is concerned with the results of a study of Ti isotopic compositions in meteorites. One objective of the study is to evaluate the possibility of a relation between oxygen and Ti anomalies, while another objective is to explore questions regarding the origin of the Ti anomalies. A summary of the major experimental findings of the study of Ti isotopic compositions is also presented. It is noted that an assessment of the implications of the Ti results favors a chemical memory type of model in which products from various nucleosynthetic sources survive in mineral grains. Isotopic heterogeneities are then preserved due to incomplete mixing and/or equilibriation with the bulk of solar system matter. Strong arguments are found to exist against a pure late supernova injection model.

Niemeyer, S.↗

NASA NTRS1985

Self-shielding in O2 - A possible explanation for oxygen isotopic anomalies in meteorites?

The production of isotopic effects in oxygen due to self-shielding of photolysing radiation by the Schumann-Runge bands of (O-16)2 is investigated. The model studied is the simple case of incoming radiation falling on a gaseous medium of uniform composition. The enhancement of O-17 and O-18 production upon photodissociation of O2 is calculated for various column densities, and its dependence on temperature and the presence of other molecules is examined. The issue of whether the products of photolysis can be trapped and thus preserve a peculiar isotopic composition is discussed.

Navon, O.↗

NASA NTRS1989

Iron isotope anomalies

Precise determinations of the Fe isotope abundances yield identical results for a terrestrial standard and for samples of carbonaceous meteorites. Fe-54/Fe-56 = 0.062669; Fe-57/Fe-56 = 0.023261 + or - 0.000002; and Fe-58/Fe-56 = 0.0031132 + or - 0.0000011 are found. Refractory element-rich inclusions from the Allende carbonaceous meteorite yield hints of deficits in Fe-57/Fe-56 of up to -3.9 + or - 2.6 parts in 10,000 and a hint of excess in Fe-58/Fe-56 of up to 27 + or - 11 parts in 10,000. One special (FUN) inclusion shows a large excess of 2.9 percent, uniquely attributable to Fe-58. This excess correlates with large excesses in the same inclusion in the neutron-rich isotopes Ca-48, Ti-50 and Cr-54. These results strengthen the evidence for an exotic nucleosynthetic component produced by neutron-rich, statistical equilibrium burning, and injected into the interstellar medium.

Voelkening, J.↗

NASA NTRS1990

Zinc isotope anomalies in Allende meteorite inclusions

The isotopic compositions of Zn, Cr, Ti, and Ca have been measured in a number of CAIs from the Allende meteorite. The aim was to test astrophysical models which predict large excesses of Zn-66 to accompany excesses in the neutron-rich isotopes of Ca, Ti, Cr, and Ni. Some of the CAIs show clearly resolved but small excesses for Zn-66 which are at least an order of magnitude smaller than predicted. This result may simply reflect the volatility and chemical behavior of Zn as compared to the other (more refractory) anomalous elements found in these samples. Alternatively, revision of parameters and assumptions used for the model calculations may be required.

Loss, R. D.↗