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At least 91 records · Page 5

Triple oxygen and hydrogen stable isotope composition of hydroxyl water in Orgueil (CI-type) and Tagish Lake (C2-type) carbonaceous chondrites

The primitive carbonaceous chondrites are of interest to cosmochemical science because they contain relatively large amounts of ‘water’ (H 2 O and/or OH – ) within phyllosilicate minerals. This water is evidence for the accretion of ices by their parent planetesimals, and thus represents an archive of the isotopic compositions of H 2 O in the protoplanetary environments. Here, in this study, we used thermogravimetry-enabled laser spectroscopy (TGA-IRIS) analyses of the Orgueil and Tagish Lake meteorites to make δ 2 H, δ 18 O, and Δ′ 17 O measurements of the H 2 O and OH – contained in the different hydrous minerals that comprise each meteorite. In Orgueil, we measured mass-weighted averages of OH – in the saponite and serpentine phyllosilicate matrix to be δ 2 H = 192 ‰, δ 18 O = 1.5 ‰, which are unquestionably of extraterrestrial origin with Δ′ 17 O = 1.0 ‰. For Tagish Lake, analogous values of OH– in the saponite and serpentine phyllosilicate matrix are δ 2 H = 704 ‰, δ 18 O = 11.3 ‰, and are similarly unambiguously extraterrestrial with Δ′ 17 O = 0.82 ‰. We estimate that the parent H 2 O involved in aqueous alteration of Orgueil had δ 18 O value ≥ +23 ‰. In Orgueil, we interpret the phyllosilicate petrographic relationships, and the δ 18 O values of OH – in saponite and serpentine to indicate that saponite formed first, at a lower temperature by 35 to 53 °C than serpentine. This suggests that the Orgueil parent body experienced increasing temperature during the phase of active aqueous alteration (prograde) which set the δ 18 O OH values of the serpentine and saponite. In the case of Tagish Lake, serpentine formed at a lower temperature by 32 to 60 °C than saponite, for the simplest case with constant δ 18 O H2O values. If serpentine formed first, followed by saponite formation at 32 to 60 °C °C higher temperature, this suggests that Tagish Lake sample TL1 underwent prograde aqueous alteration as the parent body heated up. We find evidence that the parent H 2 O for Orgueil, Tagish Lake sample TL1, and Murchison (based on data from a previous study) may have had Δ′ 17 O values of >0.64 ‰.

Aqueous alteration↗

Mixing-Controlled CI Combustion and Fuel-Effects Research

This project is focused on developing advanced combustion strategies for mixing-controlled compressionignition (i.e., diesel-cycle) engines that are synergistic with renewable and/or unconventional fuels in a manner that enhances domestic energy security, economic competitiveness, and environmental quality. During this reporting period, the focus was on ducted fuel injection (DFI), a technology that differs from conventional diesel combustion (CDC) in that it involves injecting fuel along the axis of one or more small cylindrical ducts within the combustion chamber. Each duct performs a function similar to the tube on a Bunsen burner, helping to premix the fuel with the charge-gas before ignition, creating a stable flame that forms little to no soot. The purpose of the work conducted during Fiscal Year (FY) 2019 was to begin determining the extent to which the use of oxygenated fuels, when combined with DFI and charge-gas dilution, can simultaneously lower the soot and nitrogen-oxides (N0 x ) emissions from mixing-controlled compression-ignition engines, and what the corresponding impacts on other regulated emissions and efficiency are likely to be.

33 ADVANCED PROPULSION SYSTEMS↗

Irradiation of Mo-100 Targets and Testing Fe(ll)CI 2 Precipitation for Tc-99 Removal

The production of molybdenum-99 (Mo-99) is a critical step in the generation of technetium-99m (Tc-99m), a radioisotope widely used in medical imaging. NorthStar Medical Radioisotopes, LLC is planning to produce the important medical radioisotope Mo-99 through a photonuclear reaction on molybdenum-100 (Mo-100). Accelerator production of Mo-99 using enriched Mo-100 targets yields undesirable isotopes, such as niobium-95 (Nb-95) and zirconium-95 (Zr-95). Previous studies reported that Nb and Zr isotopes can be effectively removed from Mo-99 products through coprecipitation with Fe(III). To enable the potential utilization of the first milking of Tc-99m from a Mo-99/Tc-99m generator, it is desirable to remove long-lived Tc-99. This can be accomplished by substituting Fe(III) with Fe(II) during the precipitation step, without affecting the removal of Zr and Nb isotopes. Previous experiments demonstrated up to 99+% removal of Tc using this method. It was also observed that the presence of hydrogen peroxide significantly impacts Tc removal. This was evident in the processing of enriched Mo-100 targets, where only 25% of Tc was removed. To further investigate this, another irradiation of enriched Mo-100 disks was conducted, followed by Tc-99 removal using Fe(II). Prior to irradiation, experimental conditions for Tc removal were optimized through several test runs using Mo-100 disks spiked with Tc-99. The results of these tests are discussed in this report.

07 ISOTOPE AND RADIATION SOURCES↗

A nearly exact MCSCF+CI calculation of the dissociation energy of OH

The dissociation energy and dipole moment of the ground state of OH have been obtained with a newly developed multiconfiguration, self-consistent field plus configuration interaction CDC 7600 computer program. The computed value of the dissociation energy is 4.62 eV, which is within the uncertainty limits for the experimental value of 4.63 plus or minus 0.01 eV. The computed value of the dipole moment is 1.645 D, which is very close to the experimental result of 1.66 plus or minus 0.01 D. The present results are also compared to the data obtained from similar calculations with the BISON-MC computer program developed by Das and Wahl.

Arnold, J. O.↗

Cubanite - A new sulfide phase in CI meteorites

Cubanite (CuFe2S3) previously unobserved in meteorites, has been discovered in two carbonaceous chondrites, Orgueil and Alais. The association of this mineral with low-copper pyrrhotite suggests that it formed in a low-temperature environment on the meteorite parent body.

Macdougall, J. D.↗

SCF and CI calculations of the dipole moment function of ozone

The constant and linear terms in a Taylor series expansion of the dipole moment function of the ground state of ozone are calculated with Cartesian Gaussian basis sets ranging in quality from minimal to double zeta plus polarization. Results are presented at both the self-consistent field and configuration-interaction levels. Although the algebraic signs of the linear dipole moment derivatives are all established to be positive, the absolute magnitudes of these quantities, as well as the infrared intensities calculated from them, vary considerably with the level of theory.

Curtiss, L. A.↗

Integral dependent spin couplings in CI calculations

Although the number of ways to combine Slater determinants to form spin eigenfunctions increases rapidly with the number of open shells, most of these spin couplings will make only a small contribution to a given state, provided the spin coupling is chosen judiciously. The technique of limiting calculations to the interacting subspace pioneered by Bunge (1970) was employed by Munch and Davidson (1975) to the vanadium atom. The use of an interacting space looses its advantage in more complex cases. However, the problem can always be reduced to only one interacting spin coupling by making the coefficients integral dependent. The present investigation is concerned with the performance of integral dependent interacting couplings, taking into account the results of three test calculations.

Iberle, K.↗

Early solar system aqueous activity - Sr isotope evidence from the Orgueil CI meteorite

The Sr isotopic composition and Rb-87/Sr-86 ratio have been measured in carbonates and sulfate separated from the Orgueil meteorite in order to determine the time when liquid water may have acted on the parent body. Both of the studied phases probably precipitated from aqueous solution. The results show that carbonate deposition occurred contemporaneously with parent body formation or shortly after it, probably within 100 Myr. On the other hand, at least some of the calcium sulfate seems to have been formed recently.

Macdougall, J. D.↗

Matrix mineralogy of the Orgueil CI carbonaceous chondrite

This paper presents the results of petrographic, SEM, and TEM studies of the matrix minerals in Orgueil. It was found that the matrix consists mainly of Fe-bearing Mg-rich serpentine and saponite, and a poorly crystallized Fe-rich ferrihydrite containing small and varying amounts of S and Ni. The serpentine and saponite, which occur in roughly equal molar proportions, are coherently intergrown and occur mainly in fine phyllosilicates in intimate association with the ferrihydrite. Coarse phylosilicates occur in clusters relatively free of ferrihydrite. The matrix mineralogy of the Orgueil chondrite suggests that Orgueil experienced considerably different alteration conditions than did the CM chondrites.

Tomeoka, Kazushige↗

CI, CII, and CO as tracers of gas phase carbon

In the dense interstellar medium, we find that about 20 percent of the total carbon abundance is in the form of CO, about 3 percent in C(sub I), and 100 percent in C(sub II) with uncertainties of factors of order 2. The abundance of other forms of gaseous carbon is negligible. CO is widespread throughout molecular clouds as is C(sub I). C(sub II) has only been observed near bright star-formation regions so far because of its high excitation energy. Further from ultraviolet sources it may be less abundant. Altogether we have accounted for about 1/3 of the total carbon abundance associated with dense molecular clouds. Since the other gaseous forms are thought to have negligible abundances, the rest of the carbon is probably in solid form.

Keene, Jocelyn↗

The CI pressure shift and gravitational redshift of the cool DBQA5 white dwarf LDS678A

A high resolution ultraviolet spectrum of the helium rich degenerate LDS 678A, obtained with the International Ultraviolet Explorer (IUE) satellite is presented. LDS 678A is the coolest metallic line generate (DQ or DZ) yet observed with the IUE scale. These observations provide a detailed line profile of the strong C I 2479 absorption line with equivalent width (W sub 2479 = 2.35 plus or minus 0.06 angstroms) from which theoretical line profile fits yield a C abundance (log C/He = 6.4). The presence of carbon in a helium rich atmosphere lends credence to the notion that LDS 678A is a transitional case between the DB white dwarfs with nearly pure helium atmospheres and the helium rich DQ white dwarfs which exhibit carbon bands. Corrected for an inferred pressure shift for the C I line, a gravitational redshift is deduced from which a most probable mass of 0.55 solar mass is derived.

Sion, E. M.↗