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• Thermal ionization mass spectrometry (TIMS) is a “gold standard’ technique for actinide isotope amount ratio and assay measurements. • Ubiquitously used in: • Nuclear Nonproliferation • Nuclear Safeguards • Nuclear Forensics • Basic Science • Savannah River National Laboratory (SRNL) installed a new Thermo Scientific TRITON Plus TIMS in early 2024.
Core-collapse supernovae are intense sources of tens-of-MeV neutrinos. Each explosion releases about 1058 neutrinos in a burst lasting tens of seconds. As neutrinos are weakly interacting, they escape more easily compared to photons, allowing them to be observed before the light signal. Understanding low-energy neutrino interactions with argon will be critical for future supernova measurements with the Deep Underground Neutrino Experiment (DUNE). Interpreting future DUNE supernova neutrino data will require a high-quality model of O(10 MeV) neutrino interactions, but the dominant charged-current cross section has never been measured at these low energies for an argon target. We exploit the theoretical similarities between muon capture, which has been measured, and antineutrino scattering to test MARLEY (Model of Argon Reaction Low Energy Yields), the simulation code used by DUNE to model supernova neutrino reactions. I implemented C++ code to add a muon capture mode to MARLEY and compared the predictions of the new simulation to measured isotope branching ratios of the residual nuclei. The preliminary branching ratios predicted by MARLEY running in muon capture mode demonstrate promising baseline performance when compared to experimental data and are expected to improve with further model adjustments.
Thermal ionization mass spectrometry (TIMS) is a “gold standard’ technique for actinide isotope amount ratio and assay measurements. • Ubiquitously used in: • Nuclear Nonproliferation • Nuclear Safeguards • Nuclear Forensics • Basic Science • Savannah River National Laboratory (SRNL) installed a new Thermo Scientific TRITON Plus TIMS in early 2024.
At the extremes, all analytical spectrometric measurements are limited by the resolution of the spectrometer system. Spectral overlaps, isobars in the case of mass spectrometry, can lead to the implementation of complex and time-consuming chemical separations to alleviate those interferences. In the area of elemental/isotopic mass spectrometry, use of sector-field instruments can provide a mass resolution of ~10,000, but still necessitate chemical separations. Described here is the coupling of the liquid sampling-atmospheric pressure glow discharge (LS-APGD) microplasma to ultra-high resolution Orbitrap mass analyzer systems to yield mass resolution values ranging from 70k to 1M. Resolution of this order, with commensurate improvements in precision and accuracy, holds the promise to affect elemental/isotopic determinations without the need for chemical separations.
An ongoing experimental campaign at the National Ignition Facility (NIF) aims to measure neutron induced nuclear reaction cross–sections using radiochemically doped target capsules. Critical to this campaign is the ability to collect a representative sample of the reaction products using Solid Radiochemical Collectors (SRCs) fielded around the NIF chamber. The shot presented in this paper used a doped target capsule with a neopentane gas fill was to investigate the ratio of isotopes collected at three chamber angles. It was found that SRC samples of rare earth elements collected from NIF are representative of the ingoing dopant mix, thereby concluding that fractionation does not occur during a NIF implosion. This validates the doped capsule method for use in measuring neutron induced reaction cross-sections.
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The infrared and Raman spectra of azomethane and azomethane-d(6) were examined in detail. Vibrational data provided definitive verification of a trans-structure with C(2h) symmetry. A vibrational assignment is proposed for the 24 fundamental modes based upon the observed contours, isotopic shift ratios, and group frequency correlations. Spectra of the polycrystalline samples indicate that there are at least four molecules per unit cell, since a number of the bands were observed to be split into doublets. The crystal also appeared to have a center of symmetry, since mutual exclusion was clearly operative.
Laboratory spectra of the 3nu(sub 3) band of (C-13)H4 at 1.1 micron were analyzed along with high-resolution image-tube spectra of Jupiter in the appropriate spectral region. Comparison of several J-multiplets in these spectra resulted in the identification of (C-13)H4 in the atmosphere of Jupiter. A Jovian C-12/C-13 isotopic abundance ratio of 110 (plus or minus 35) has been derived from the equivalent width of the R(2) multiplet measured on the two best spectrograms.
The IR-emitting core and shell of IRC +10216 are investigated using a high-resolution spectrum covering the wavelength interval between 3 and 5 microns. Line identifications made or confirmed include those due to (C-12)(O-16), (C-13)(O-16), (C-12)(O-17), and (C-12)(O-18). A mean heliocentric velocity of about -32 km/s is obtained from the 42 least blended (C-12)O and (C-13)O lines, and the following isotopic abundance ratios are derived by comparing equivalent widths of the observed lines: C-12/C-13, C-12/C-14, O-16/O-17, and O-17/O-18. The structure of the expanding gas shell is examined, an explanation is offered for the lack of P Cygni profiles in the spectrum, and an unsuccessful search for other molecules is briefly discussed. It is concluded that a low C-12/C-13 ratio is not necessarily a signature of a carbon star.
The relative charge abundance of galactic cosmic-ray nuclei is measured between 600 and 1000 MeV per nucleon over a range of Z from 2 to 28. The abundances observed at earth are extrapolated to the cosmic-ray source, yielding accurate source abundances for 15 elements. These abundances, together with recently measured isotopic abundance ratios, are compared with the average abundances observed in another sample of accelerated material - solar cosmic rays. Appreciable differences are found in the composition for the elements He, C, N, and Ne. The galactic and solar cosmic-ray abundances are also compared with a variety of compilations of unaccelerated matter.
High resolution 1.6, 3.3 and 4.6 micron spectra were obtained on the F8 supergiant star IRC + 10420 on June 9-11, 1984, using the 4 m Mayall telescope and Fourier Transform Spectrometer at Kitt Peak. IRC + 10420 is distinguished by its hydrogen maser, unusual for stars of this type. The measured column densities of CO led to an estimated isotopic carbon ratio of 7-11, supporting a model of the object as a highly evolved star. The redshift is interpreted as due to scattering by outward-moving circumstellar dust grains. The IR spectrum of IRC + 10420 suggests that the object is a post-asymptotic branch star still surrounded by the thick dust shell it produced while it was much cooler.
The progress is reported of high resolution spectra of selected bright comets with the aim of determining the carbon isotope abundance ratio, C-12/C-13. The ratio was determined for various Solar System objects (in the atmospheres of the giant planets, meteorites, the Earth, and the solar photosphere), where the C-12/C-13 = 89/1. In the interstellar medium, optical and radio observations give a range of C-12/C-13 = 43-67/1 depending on the observing techniques used and the specific interstellar cloud observed. The echelle spectra is presented of the CN(0,0) violet system in three comets: P/Brorsen-Metcalf, C/Okazaki-Levy-Rudenko, and C/Austin. P/Brorsen-Metcalf has a period of 70 y (prograde) compared with P/Halley which is 76 y (retrograde). The similar periods made P/Brorsen-Metcalf of special interest for comparison with P/Halley.
Being icy, cometary nuclei are the most easily modified bodies in the solar system - even modest heating is sufficient to induce significant weight loss. This sublimative loss and longterm storage far from the sun protect the nucleus against internal warming and ensure that cometary nuclei today contain the least processed material remaining from the early nebula - or perhaps from the natal cloud. The chemical compositions of ices, low temperature-refractory organics, and refractory minerals (and their physical states) provide sensitive probes of the origin and history of this material. The fortunate appearance of Hyakutake and Hale-Bopp has provided a wealth of information on these Oort cloud comets, obtained with a wide range of astronomical approaches. I will review certain key results for these comets, such as chemical abundances, isotopic abundance ratios, nuclear spin statistics, and nuclear vs extended production of "parent volatiles", and will illustrate how these test the origins of cometary material. A comparison with 1P/Halley--a third comet from the giant planet nebular region--will be discussed in the context of heterogeneity among these bodies.
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Recent studies have shown that Martian magmas had wide range of oxygen fugacities (fO2) and that this variation is correlated with the variation of La/Yb ratio and isotopic characteristics of the Martian basalts, shergottite meteorites. The origin of this correlation must have important information about mantle sources and Martian evolution. In order to understand this correlation, it is necessary to know accurate value of oxidation state of other Martian meteorite groups. Nakhlites, cumulate clinopyroxenites, are another major group of Martian meteorites and have distinctly different trace element and isotopic characteristics from shergottites. Thus, estimates of oxidation state of nakhlites will give us important insight into the mantle source in general. Several workers have estimated oxidation state of nakhlites by using Fe-Ti oxide equilibrium. However, Fe-Ti oxides may not record the oxidation state of the parent melt of the nakhlite because it is a late-stage mineral. Furthermore, there is no comprehensive study which analyzed all nakhlite samples at the same time. Therefore, in this study (1) we reduced the uncertainty of the estimate using the same electron microprobe and the same standards under the same condition for Fe-Ti oxide in 6 nakhlites and (2) we also performed crystallization experiments to measure partition coefficients of Eu into pyroxene in the nakhlite system in order to estimate fO2 when the pyroxene core formed (i.e. Eu oxybarometer [e.g. 2,6]).
Submillimeter spectroscopic observations of comets provide an important tool for understanding their chemical composition and enable a taxonomic classification. Aims. We aim to determine the production rates of several parent- and product volatiles and the C-12/C-13 isotopic carbon ratio in the long-period comet C/2004 Q2 (Machholz), which is likely to originate from the Oort Cloud. Methods. The line emission from several molecules in the coma was measured with high signal-to-noise ratio in January 2005 at heliocentric distance of 1.2 AU by means of high-resolution spectroscopic observations using the Submillimeter Telescope (SMT) at the Arizona Radio Observatory (ARO). Results. We have obtained production rates of several volatiles (CH3OH, HCN, H(sup 13)CN, HNC, H2CO, CO, and CS) by comparing the observed and simulated line-integrated intensities. We calculated the synthetic profiles using a radiative transfer code that includes collisions between neutrals and electrons, and the effects of radiative pumping of the fundamental vibrational levels by solar infrared radiation. Furthermore, multiline observations of the CH3OH J = 7-6 series allow us to estimate the rotational temperature using the rotation diagram technique. We find that the CH3OH population distribution of the levels sampled by these lines can be described by a rotational temperature of 40 +/- 3 K. Derived mixing ratios relative to hydrogen cyanide are CO/CH3OH/H2CO/CS/HNC/HC-13N/HCN= 30.9/24.6/4.8/0.57/0.031/0.013/1 assuming a pointing offset of 8" due to the uncertain ephemeris at the time of the observations and the telescope pointing error. Conclusions. The measured relative molecular abundances in C/2004 Q2 (Machholz) are between low- to typical values of those obtained in Oort Cloud comets, suggesting that it has visited the inner solar system previously and undergone thermal processing. The HNC/HCN abundance ratio of approx 3.1% is comparable to that found in other comets, accounting for the dependence on the heliocentric distance, and could possibly be explained by ion-molecule chemical processes in the low-temperature atmosphere. From a tentative HC-13N detection, the measured value of 97 +/- 30 for the HC-12N/HC-13N isotopologue pair is consistent with a telluric value. The outgassing variability observed in the HCN production rates over a period of two hours is consistent with the rotation of the nucleus derived using different observational techniques.
Comets provide important clues to the physical and chemical processes that occurred during the formation and early evolution of the Solar System, and could also have been important for initiating prebiotic chemistry on the early Earth. Comets are comprised of molecular ices, that may be pristine inter-stellar remnants of Solar System formation, along with high-temperature crystalline silicate dust that is indicative of a more thermally varied history in the protosolar nebula. Comparing abundances of cometary parent volatiles, and isotopic fractionation ratios, to those found in the interstellar medium, in disks around young stars, and between cometary families, is vital to understanding planetary system formation and the processing history experienced by organic matter in the so-called interstellar-comet connection. We will present a comparison of molecular abundances in these comets to those observed in others, supporting a long-term effort of building a comet taxonomy based on composition.
Nitrogen-bearing molecules in cold molecular clouds exhibit a range of isotopic fractionation ratios and these molecules may be the precursors of 15N enrichments found in comets and meteorites. Chemical model calculations indicate that atom-molecular ion and ion-molecule reactions could account for most of the fractionation patterns observed. However, recent quantum-chemical computations demonstrate that several of the key processes are unlikely to occur in dense clouds. Related model calculations of dense cloud chemistry show that the revised 15N enrichments fail to match observed values. We have investigated the effects of these reaction rate modifications on the chemical model of Wirstrom et al. (2012) for which there are significant physical and chemical differences with respect to other models. We have included 15N fractionation of CN in neutral-neutral reactions and also updated rate coefficients for key reactions in the nitrogen chemistry. We find that the revised fractionation rates have the effect of suppressing 15N enrichment in ammonia at all times, while the depletion is even more pronounced, reaching 14N/15N ratios of >2000. Taking the updated nitrogen chemistry into account, no significant enrichment occurs in HCN or HNC, contrary to observational evidence in dark clouds and comets, although the 14N/15N ratio can still be below 100 in CN itself. However, such low CN abundances are predicted that the updated model falls short of explaining the bulk 15N enhancements observed in primitive materials. It is clear that alternative fractionating reactions are necessary to reproduce observations, so further laboratory and theoretical studies are urgently needed.