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NASA NTRS2011

The Atmospheres of Titan and Saturn in the Infrared from Cassini: The Interplay Between Observation and Laboratory Studies

The Composite Infrared Spectrometer (CIRS) aboard the Cassini spacecraft has been recording spectra of Saturn and Titan since its arrival in the Saturn system in 2004. CIRS, a Fourier transform spectrometer, observes the thermal infrared spectrum of both atmospheres from 10 to 1500/cm with resolutions up to 0.5/cm (Flasar et al. 2004). From these data CIRS provides global coverage of the molecular composition of the stratosphere and troposphere, as well as maps of temperature and winds. From such studies CIRS helps reveal the chemistry and evolutionary history of Saturn and Titan and their relationships to other Solar System bodies. The Cassini mission is continuing until 2017, permitting CIRS to search for atmospheric changes during more than a Saturnian season. By combining with results from Voyager (1980, 1981) the baseline becomes more than one Saturnian year (Coustenis et al. 2011). CIRS spectroscopy of the atmospheres of Saturn and Titan has raised a variety of questions that require new laboratory studies. A complete understanding of the CIRS high-resolution atmospheric spectra cannot be fully achieved without new or improved line positions and intensities for some trace molecules (e.g., Nixon et al. 2009). Isotopic variants of some of the more abundant species often need improved line parameters in order to derive isotopic ratios (e.g., Coustenis et al. 2008 and Fletcher et a!. 2009). Isotopic ratios contain information about the history of an atmosphere if experimental fractionation rates are available (Jennings et al. 2009). Some aerosol and haze features continue to defy identification and will not be explained without better knowledge of how these materials are formed and until we obtain their laboratory spectra. The interaction between CIRS investigations and laboratory research has been productive and has already led to new discoveries.

Jennings, D. E.↗

NASA NTRS2015

Nebular and Interstellar Materials in a Giant Cluster IDP of Probable Cometary Origin

Comets contain a complex mixture of materials with presolar and Solar System origins. Chondritic porous interplanetary dust particles (CP-IDPs) are associated with comets by their fragile nature, unequilibrated anhydrous mineralogy and high abundances of circumstellar grains and isotopically anomalous organic materials. Comet 81P/Wild 2 samples returned by the Stardust spacecraft contain presolar materials as well as refractory 16O-rich Ca-Al-rich inclusion- (CAI), chondrule-, and AOA-like materials. We are conducting coordinated chemical, mineralogical, and isotopic studies of a giant cluster CP-IDP (U2-20-GCA) to determine the proportions of inner Solar System and interstellar materials. We previously found that this IDP contains abundant presolar silicates (approx. 1,800 ppm) and 15N-rich hotspots [6].

Messenger, S.↗

NASA NTRS2006

Isotopic Analyses of Stardust Mission Samples

In January 2006 the NASA Stardust spacecraft successfully returned to Earth the first direct samples of cometary dust. Comets are considered to be the best preserved remnants of the original building blocks of the solar system, and should contain high abundances of interstellar dust. The isotopic analyses of the Stardust samples now underway will offer a sensitive measure of the relative proportions of solar system and preserved interstellar matter in comets. Though once considered to be unprocessed assemblages of interstellar materials, a minor population of crystalline silicates is apparent in some cometary spectra, suggesting that comets contain materials processed at high temperatures. Identifying and isotopically characterizing crystalline silicates among the collected Stardust materials is another high-priority goal of this mission. The results of these preliminary isotopic analyses of the Stardust mission samples will be presented.

Messenger, Scott↗

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 NTRS2017

Distinct Chlorine Isotopic Reservoirs on Mars: Implications for Character, Extent and Relative Timing of Crustal Interaction with Mantle-Derived Magmas, Evolution of the Martian Atmosphere, and the Building Blocks of an Early Mars

The style, magnitude, timing, and mixing components involved in the interaction between mantle derived Martian magmas and Martian crust have long been a point of debate. Understanding this process is fundamental to deciphering the composition of the Martian crust and its interaction with the atmosphere, the compositional diversity and oxygen fugacity variations in the Martian mantle, the bulk composition of Mars and the materials from which it accreted, and the noble gas composition of Mars and the Sun. Recent studies of the chlorine isotopic composition of Martian meteorites imply that although the variation in delta (sup 37) Cl is limited (total range of approximately14 per mille), there appears to be distinct signatures for the Martian crust and mantle. However, there are potential issues with this interpretation. New Cl isotope data from the SAM (Sample Analysis at Mars) instrument on the Mars Science Lab indicate a very wide range of Cl isotopic compositions on the Martian surface. Recent measurements by [10] duplicated the results of [7,8], but placed them within the context of SAM surface data. In addition, Martian meteorite Chassigny contains trapped noble gases with isotopic ratios similar to solar abundance, and has long been considered a pristine, mantle derived sample. However, previous studies of apatite in Chassigny indicate that crustal fluids have interacted with regions interstitial to the cumulus olivine. The initial Cl isotope measurements of apatite in Chassigny suggest an addition of crustal component to this lithology, apparently contradicting the rare gas data. Here, we examine the Cl isotopic composition of multiple generations and textures of apatite in Chassigny to extricate the crustal and mantle components in this meteorite and to reveal the style and timing of the addition of crustal components to mantle-derived magmas. These data reveal distinct Martian Cl sources whose signatures have their origins linked to both the early Solar System and the evolving Martian atmosphere.

Shearer, C. K.↗

NASA NTRS1978

Planetary-type rare gases in an upper mantle-derived amphibole

All 23 stable rare gas isotopes in a mantle-derived aluminous Ti-rich amphibole, kaersutite, were measured, and the abundance pattern indicated by the results is similar to the 'planetary' rare gas pattern of carbonaceous chondrites. The He-3/He-4 ratio of (4.9 + or - 0.6) times 10 to the -5th power is anomalously high. Ne-21 is enriched relative to the abundance of the other two neon isotopes in the atmosphere, while the heavy isotopes of Kr and the Xe isotopes are within error of the atmospheric values. The analytical procedure is described. It is concluded that part of the primordial rare gases of the earth are still present in some parts of the upper mantle and that these gases retain a faithful record of the 'planetary' primordial rare gas elemental signature.

Saito, K.↗

NASA NTRS1983

Rb-Sr, Sm-Nd, K-Ca, O, and H isotopic study of Cretaceous-Tertiary boundary sediments, Caravaca, Spain Evidence for an oceanic impact site

The results of isotopic and trace-element-abundance analyses of Ir-enriched Cretaceous-Tertiary-boundary clay sediments from Caravaca, Spain, and of adjacent carbonate and marl layers, are presented. Acetic-acid and HCl leachates and residues were analyzed by isotope dilution to determine K, Rb, Sr, Sm, and Nd concentrations and Sr-87/Sr-86 and Nd-143/Nd-144 ratios. The stable isotope ratios delta-D, delta-(C-13), and delta-(0-18) were also determined. The results are presented in tables and graphs and compared with published data on the Caravaca sediments and on samples from other locations. The boundary clay is found to be distinguished from the adjacent layers by its isotopic ratios and to be of mainly terrestrial, lithospheric (deeper than 3-km) origin. Although submarine-weathering effects are evident and difficult to quantify, the degree of variation in Ni, Ir, Sr, and REE concentrations is considered too large to be attributed to postdepositional processes alone. These findings are seen as evidence for the ocean impact of a large single asteroid producing a worldwide blanket of ejecta, a large injection of water vapor into the atmosphere, and perhaps a gigantic tsunami, at the end of the Cretaceous period.

Depaolo, D. J.↗

NASA NTRS2007

Sm-Nd and Rb-Sr Ages for MIL 05035: Implications for Surface and Mantle Sources

The Sm-Nd and Rb-Sr ages and also the initial Nd and Sr isotopic compositions of MIL 05035 are the same as those of A-881757. Comparing the radiometric ages of these meteorites to lunar surface ages as modeled from crater size-frequency distributions as well as the TiO2 abundances and initial Sr-isotopic compositions of other basalts places their likely place of origin as within the Australe or Humboldtianum basins. If so, a fundamental west-east lunar asymmetry in compositional and isotopic parameters that likely is due to the PKT is implied.

Nyquist, L. E.↗

NASA NTRS2004

The Nature and Origin of Interplanetary Dust: High Temperature Components

The specific parent bodies of individual interplanetary dust particles (IDPs) are un-known, but the anhydrous chondritic-porous (CP) sub-set has been linked directly to cometary sources [1]. The CP IDPs escaped the thermal processing and water-rock interactions that have severely modified or destroyed the original mineralogy of primitive meteorites. Their origin in the outer regions of the solar system suggests they should retain primitive chemical and physical characteristics from the earliest stages of solar system formation (including abundant presolar materials). Indeed, CP IDPs are the most primitive extraterrestrial materials available for laboratory studies based on their unequilibrated mineralogy [2], high concentrations of carbon, nitrogen and volatile trace elements relative to CI chondrites [3, 4, 5], presolar hydrogen and nitrogen isotopic signatures [6, 7] and abundant presolar silicates [8].

Keller, L. P.↗

NASA NTRS1982

The heavy element yields of neutron capture nucleosynthesis

Consideration of the contribution made to the abundances of the heavy element isotopes by the S- and R-processes of nucleosynthesis has led to the determination that the previous assumption concerning the exclusive alignment of isobars to one or the other of these processes is probably in error. If the relatively small odd and even mass number abundance fluctuations characterizing R-process abundances are always the case, as assumed by this study, S-process contributions to the abundances of R-process isobars are substantial, consistent with transient flashing episodes in the S-process neutron production processes. A smooth and monotonically-decreasing curve of the abundance of the S-process yields times the neutron capture cross-section versus mass number is therefore the primary tool for the separation of the abundances due to the two processes.

Cameron, A. G. W.↗

NASA NTRS1987

Al-26, Pu-244, Ti-50, REE, and trace element abundances in hibonite grains from CM and CV meteorites

Hibonites from the CM meteorites Murchison, Murray, and Cold Bokkeveld, and hibonites and Ti-rich pyroxene from the CV chondrite Allende are studied. Electron microprobe measurements of major element concentrations and track and ion probe measurements of Mg and Ti isotopic ratios, rare earth elements (REEs), and trace element abundances are analyzed. Correlations between isotopic anomalies in Ti, Al-26, Pu-244, and Mg-26(asterisk) are examined. Ti isotopic anomalies are compared with REE and trace element abundance patterns. Reasons for the lack of Al-26 in the hibonites are investigated and discussed. It is observed that there is no correlation between the Ti isotopic compositions, and the presence of Mg-26(asterisk), Pu-244, and REE and trace element patterns in individual hibonite samples. The data reveal that hibonites are not interstellar dust grains but formed on a short time scale and in localized regions of the early solar system.

Fahey, A. J.↗

NASA NTRS2024

Investigating Bennu’s Volatile Accretion History Through Step-Heating N-Ne-Ar Analyses of Single Aggregate Particles

NASA’s OSIRIS-REx spacecraft delivered a sample from the carbonaceous asteroid (101955) Bennu to Earth on September 24, 2023. Since Bennu presumably accreted in the outer protoplanetary disk, beyond Jupiter’s orbit, the collected material is expected to be rich in highly volatile elements such as H, C, N, and noble gases—similar to Ivuna-type (CI) carbonaceous chondrites and material from asteroid (162173) Ryugu returned by JAXA’s Hayabusa2 spacecraft. This type of material may have contributed to the volatile inventory of Earth and the other terrestrial planets. Bulk CI chondrites record a narrow range of δ 15 N values (i.e., the permil difference from the atmospheric 15 N/ 14 N ratio), averaging between +42 and 49‰. In contrast, recent analyses at CRPG’s noble gas facility revealed that two pelletized Ryugu samples have lower δ 15 N values of +18.1 ± 0.9‰ and +19.5 ± 0.9‰. Together with the low measured N abundances, this observation suggests that Ryugu has lost a 15 N-rich, labile organic phase due to pervasive aqueous alteration. Subsequent high-resolution step-heating analyses of an additional Ryugu particle demonstrated that the δ 15 N value varies significantly during successive extraction steps (between +1.0 ± 1.0‰ and 65.8 ± 1.1‰); the variable N isotopic composition points to the presence of several isotopically distinct N-carrier phases in CI-type material. Here, we report preliminary N-Ne-Ar results obtained for individual particles from an aggregate Bennu sample using the Noblesse-HR (Nu Instruments) noble gas mass spectrometer at CRPG’s noble gas facility. In a companion abstract, we will present the noble gas (He, Ne, Ar, Kr, Xe) characteristics of other aggregate particles determined with a HELIX MC Plus. Whereas the abundance and isotopic composition of noble gases permit detection of various presolar phases and the so-called phase Q, as well as quantification of solar wind–derived and cosmogenic components, the abundance and isotopic composition of N are expected to provide further insights into the origin and evolution of N-bearing phases in carbonaceous asteroids.

E Füri↗

NASA NTRS2023

Pervasive aqueous alteration in the early Solar System revealed by potassium isotopic variations in Ryugu samples and carbonaceous chondrites

C-type asteroids are the presumed home to carbonaceous chondrites, some of which contain abundant life-forming volatiles and organics. For the first time, samples from a C-type asteroid (162173 Ryugu) were successfully returned to Earth by JAXA’s Hayabusa2 mission. These pristine samples, uncontaminated by the terrestrial environment, allow a direct comparison with carbonaceous chondrites. This study reports the stable K isotopic compositions (expressed as δ 41 K) of Ryugu samples and seven carbonaceous chondrites to constrain the origin of K isotopic variations in the early Solar System. Three aliquots of Ryugu particles collected at two touchdown sites have identical δ 41 K values, averaged at -0.194 ± 0.038‰ (2SD). The K isotopic composition of Ryugu falls within the range of δ 41 K values measured on representative CI chondrites, and together, they define an average δ 41 K value of -0.185 ± 0.078‰ (2SE), which provides the current best estimate of the K isotopic composition of the bulk Solar System. Samples of CI chondrites with δ 41 K values that deviate from this range likely reflect terrestrial contaminations or compositional heterogeneities at sampled sizes. In addition to CI chondrites, substantial K isotopic variability is observed in other carbonaceous chondrites and within individual chondritic groups, with δ 41 K values inversely correlated with K abundances in many cases. These observations indicate widespread fluid activity occurred in chondrite parent bodies, which significantly altered the original K abundances and isotopic compositions of chondrules and matrices established at their accretion.

Asteroid Ryugu↗

NASA NTRS1977

The age of the galactic cosmic rays derived from the abundance of Be-10

Satellite measurements of the abundance of the Be-10 isotope in galactic cosmic rays are used to determine the cosmic-ray lifetime for escape. The data are analyzed by employing a technique based on an extensive calibration of a cosmic-ray telescope with the aid of high-energy Be beams accelerated in a bevatron. It is found that the Be-10/Be abundance ratio at 80 MeV/nucleon is 0.028 + or - 0.104. A comparison of this result with calculations based on a homogeneous steady-state model of galactic cosmic-ray confinement and propagation yields an average interstellar density of 0.18 (+0.18, -0.11) atom/cu cm and a corresponding cosmic-ray lifetime of 17 (+24, -8) million years after solar modulation is taken into account. The low average density traversed by the cosmic rays is shown to suggest that the particles may be spending the major part of their existence in regions of very low matter density. The consequences of these results are discussed for models of cosmic-ray propagation in the Galaxy, including such alternatives as propagation in a galactic halo or in regions of interstellar space where the interstellar gas density is very low.

Garcia-Munoz, M.↗

DOE OSTI2024

Chlorine Isotope Separations using Thermal Diffusion

As of the close of 2023 a thermal diffusion isotope separations (TDIS) apparatus was constructed, successful shakedown testing was achieved and enrichments of isotopic concentrations relative to natural abundance 35/37 Cl were collected. Further, the model for these enrichment experiments drove the timing for sampling and other critical, extrapolated functions that are discussed herein. Our decision to move forward in 2024 with the installation of a larger set of separation tubes and associated equipment was based on the successful development of the predictive model. The Chlorine Isotopes Project Team at PNNL is prepared to claim that the installation and hence its separative power is restricted only by the spatial limitations of the laboratory, and this at present appears to be the limiting feature to first pass high enriched 37 Cl.

07 ISOTOPE AND RADIATION SOURCES↗

NASA NTRS1994

Distribution of siderophile and other trace elements in melt rock at the Chicxulub impact structure

Recent isotopic and mineralogical studies have demonstrated a temporal and chemical link between the Chicxulub multiring impact basin and ejecta at the Cretaceous-Tertiary boundary. A fundamental problem yet to be resolved, however, is identification of the projectile responsible for this cataclysmic event. Drill core samples of impact melt rock from the Chichxulub structure contain Ir and Os abundances and Re-Os isotopic ratios indicating the presence of up to approx. 3 percent meteoritic material. We have used a technique involving microdrilling and high sensitivity instrumental neutron activation analysis (INAA) in conjunction with electron microprobe analysis to characterize further the distribution of siderophile and other trace elements among phases within the C1-N10 melt rock.

Schuraytz, B. C.↗

DOE OSTI2022

Modeling Isotope Separation in Electrochemical Lithium Deposition

Naturally occurring Li consists of two stable isotopes, 6 Li with an abundance of about 7.5%, and 7 Li making up the remainder with 92.5%. The development of a 6 Li enrichment technique, in terms of technical reliability and environmental safety to reach 6 Li future requirements, represents a key step in the roadmap for nuclear fusion energy supply worldwide. This paper uses finite element analysis-based models to simulate electrochemical Li isotope separation, which is an attractive method in terms of simplicity, safety, and scalability. In the model, we quantitatively analyze how different electrochemical factors including thermodynamics, charge-transfer kinetics, and diffusivities affect the separation process (separation factor), together with cell parameters, such as cell length and current density. The maximum separation factor of 1.128 could be obtained with the cell under the optimal thermodynamic, kinetic, and diffusive conditions, which is among the highest separation factors ever reported. Furthermore, these results will assist in designing the actual isotope separation setup with large separation factor and appropriate timing for sample collection.

07 ISOTOPE AND RADIATION SOURCES↗

NASA NTRS1986

Variations in the HCN/HNC abundance ratio in the Orion molecular cloud

Observations of the rare isotopes of HCN and HNC have been used to determine the relative abundance of these two chemical isomers along the central ridge of the Orion molecular cloud. The abundance ratio HCN/HNC decreases by more than an order of magnitude from the relatively warm plateau and hot core sources toward the KL nebula to the colder, more quiescent clouds to the north and south. Even in the cooler regions, however, the ratio is an order of magnitude larger than that found in previous investigations of cold dark clouds. The kinetic temperature in the regions studied is determined from new observations of methylacetylene (CH3CCH), together with other recent estimates of the gas temperature near KL. The results suggest that the warmer portions of the cloud are dominated by different chemical pathways that those in the general instellar cloud material.

Goldsmith, Paul F.↗