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At least 613 records · Page 34

Measurements of Short-Lived Isomers from Photofission as a Method of Active Interrogation for Special Nuclear Materials

Isomeric fission products, such as 134m Te (T 1/2 = 164 ns) and 136m Xe (T 1/2 = 2.95 μs), are proposed as a signature of special nuclear materials in active interrogation applications. To test this conjecture, monoenergetic 9, 11, and 13 MeV photons from the HIγS facility are used to induce fission of 235 U, 238 U, and 239 Pu targets. The de-excitation γ rays of the isomers are measured using time-gated spectroscopy with high-purity germanium detectors. The 134m Te and 136m Xe isomers are detected and identified by the energy and decay half-life of their characteristic γ-ray transitions. The ratio of yields for these two signature γ rays, corresponding to 134m Te/( 136m Xe + 136 I), is found to be strongly correlated with the identity of the fissioning nuclei. These results show that fission-product isomers may be used in active interrogation to detect and identify special nuclear materials, even providing information on the isotopic enrichment. In conclusion, the feasibility of an active interrogation scenario using a bremsstrahlung beam is discussed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Investigating trends in actinide covalency and magnetism with 35/37 Cl SSNMR spectroscopy and first-principles calculations

Solid-state NMR (SSNMR) spectroscopy is a powerful technique for studying actinide chemistry but has been significantly limited due to the complex paramagnetism, and radiological hazards presented by these materials. Lanthanide and actinide salts often feature magnetic ordering and can be paramagnetic, ferromagnetic, or antiferromagnetic depending on temperature and electronic structure. Paramagnetic interactions can manifest in SSNMR both as secular spectral shifts and/or couplings as well as contributions from non-secular relaxation. Both effects can be directly measured with NMR and used to extrapolate rich chemical information such as coordination environments, bonding characteristics, local molecular dynamics, and correlation times. Typically, these studies are carried out on high-γ and highly abundant NMR-active isotopes (e.g., 1 H, 6/7 Li, 19 F, 23 Na, etc.) or on enriched rare isotopes (e.g., 2 H and 17 O), which can be expensive. Herein, we present a facile methodology to measure the 35/37 Cl electric-field gradient (EFG) and paramagnetic shift anisotropy (SA) tensor components using static wideline SSNMR measurements of LaCl 3 , NdCl 3 , UCl 3 , and UCl 4 . The static powder spectra were measured with both 35 Cl and 37 Cl SSNMR to increase the fidelity of the extracted tensor parameters. Variable temperature NMR of a select case confirms the Curie–Weiss paramagnetism. Relaxation measurements of both nuclei further corroborate observations owing to the paramagnetic relaxation enhancement and reveal simultaneous quadrupolar relaxation mechanisms. Density functional theory (DFT) calculations using Hubbard U corrections to the uranium valence orbitals show excellent agreement with experimental EFG tensor parameters and help describe the bonding characteristics in these lanthanide and actinide systems.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The fall, recovery, classification, and initial characterization of the Hamburg, Michigan H4 chondrite

Abstract The Hamburg meteorite fell on January 16, 2018, near Hamburg, Michigan, after a fireball event widely observed in the U.S. Midwest and in Ontario, Canada. Several fragments fell onto frozen surfaces of lakes and, thanks to weather radar data, were recovered days after the fall. The studied rock fragments show no or little signs of terrestrial weathering. Here, we present the initial results from an international consortium study to describe the fall, characterize the meteorite, and probe the collision history of Hamburg. About 1 kg of recovered meteorites was initially reported. Petrology, mineral chemistry, trace element and organic chemistry, and O and Cr isotopic compositions are characteristic of H4 chondrites. Cosmic ray exposure ages based on cosmogenic 3 He, 21 Ne, and 38 Ar are ~12 Ma, and roughly agree with each other. Noble gas data as well as the cosmogenic 10 Be concentration point to a small 40–60 cm diameter meteoroid. An 40 Ar‐ 39 Ar age of 4532 ± 24 Ma indicates no major impact event occurring later in its evolutionary history, consistent with data of other H4 chondrites. Microanalyses of phosphates with LA‐ICPMS give an average Pb‐Pb age of 4549 ± 36 Ma. This is in good agreement with the average SIMS Pb‐Pb phosphate age of 4535.3 ± 9.5 Ma and U‐Pb Concordia age of 4535 ± 10 Ma. The weighted average age of 4541.6 ± 9.5 Ma reflects the metamorphic phosphate crystallization age after parent body formation in the early solar system.

79 ASTRONOMY AND ASTROPHYSICS↗

Thermal Neutron Scattering Law Evaluation for Zirconium Carbide and Critical Mass Calculations

Zirconium carbide (ZrC) is a candidate material for use in advanced high temperature reactors, including space nuclear thermal propulsion applications. Thermal neutron scattering laws (TSLs) are generated for carbon bound in ZrC, C(ZrC), and zirconium bound in ZrC, Zr(ZrC), using ab initio lattice dynamics methods. These evaluations are to be submitted for inclusion in ENDF/B-VIII.1 and use the incoherent approximation for inelastic scattering as well as the new mixed elastic scattering treatment. The application of disordered alloy theory is introduced to appropriately capture the isotopic composition of Zr and C in the elastic scattering cross section. Localized higher energy vibrations in the C(ZrC) phonon density of states that are separated from lower energy modes result in quantized oscillations in the inelastic contributions to the TSL with a significant likelihood of large energy down-scattering and up-scattering interactions, where the latter increases in probability with temperature. The quanta of energy transfer during neutron thermalization is substantially greater than classically expected within the thermal neutron energy range. MC21 critical mass calculations of ZrC mixtures with high-enriched uranium demonstrate an impact of the TSLs when compared to free-gas treatment for 235 U concentrations less than 0.2 g/cm 3 . Additional MC21 critical mass calculations with homogenous mixtures of ZrC and reactor-grade graphite also demonstrate sensitivity to the ZrC TSL for thermal spectrum driven fission systems.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

On the distribution of noble gases in Allende - A differential oxidation study

The investigation makes use of an oxidizing technique which is based on methods widely employed in light stable isotope analysis. The utilization of closed-system differential combustion in molecular oxygen in an ultra-high vacuum system on-line with a spectrometer makes it possible to conduct precise abundance and isotopic measurements of all gases released in progressive oxidation and/or thermal outgassing of the host phases. Attention is given to the noble gases mobilized in progressive oxidation of a carbon-rich acid residue and a fine-grained matrix separate. The progressive oxidation of the Allende matrix is discussed. Release occurred over three distinct intervals, characterized by oxidation below 600 C, gas mobilization between 630 and 750 C, and high-temperature diffusive release.

Frick, U.↗

Colloidally separated samples from Allende residues - Noble gases, carbon and an ESCA-study

Results are presented which strengthen the hypothesis of heterogeneity among the carbon- and nitrogen-bearing phases of the Allende meteorite. These data also highlight the possibility of performing physical separations yielding samples in which some of the noble gas- and carbon-bearing phases are extraordinarily predominant over others. The conclusion, based on mass and isotope balance arguments, that a significant portion of the carbonaceous matter in Allende is likely to be gas-poor or gas-free need not weaken the case for carbonaceous carriers for the major noble gas components. The concept that acid-soluble carbonaceous phases contain a multiplicity of components, each of which may have formed under a multiplicity of different physical-chemical conditions, is reemphasized by the results of the present study.

Ott, U.↗

13CO2/12CO2 isotopic ratio measurements using a difference frequency-based sensor operating at 4.35 micrometers

A portable modular gas sensor for measuring the 13C/12C isotopic ratio in CO2 with a precision of 0.8%(+/-1 sigma) was developed for volcanic gas emission studies. This sensor employed a difference frequency generation (DFG)-based spectroscopic source operating at 4.35 micrometers (approximately 2300 cm-1) in combination with a dual-chamber gas absorption cell. Direct absorption spectroscopy using this specially designed cell permitted rapid comparisons of isotopic ratios of a gas sample and a reference standard for appropriately selected CO2 absorption lines. Special attention was given to minimizing undesirable precision degrading effects, in particular temperature and pressure fluctuations.

NASA Discipline Life Sciences Technologies↗

Nuclear Physics Made Very, Very Easy

The fundamental approach to nuclear physics was prepared to introduce basic reactor principles to various groups of non-nuclear technical personnel associated with NERVA Test Operations. NERVA Test Operations functions as the field test group for the Nuclear Rocket Engine Program. Nuclear Engine for Rocket Vehicle Application (NERVA) program is the combined efforts of Aerojet-General Corporation as prime contractor, and Westinghouse Astronuclear Laboratory as the major subcontractor, for the assembly and testing of nuclear rocket engines. Development of the NERVA Program is under the direction of the Space Nuclear Propulsion Office, a joint agency of the U. S. Atomic Energy Commission and the National Aeronautics and Space Administration. This report is being reprinted for use in the U. S. Atomic Energy Commission and National Aeronautics and Space Administration educational and technology utilization programs.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Element distribution and noble gas isotopic abundances in lunar meteorite Allan Hills A81005

Antarctic meteorite ALLAN HILLS A81005, an anorthositic breccia, is recognized to be of lunar origin. The noble gases in this meteorite were analyzed and found to be solar-wind implanted gases, whose absolute and relative concentrations are quite similar to those in lunar regolith samples. A sample of this meteorite was obtained for the analysis of the noble gas isotopes, including Kr(81), and for the determination of the elemental abundances. In order to better determine the volume derived from the surface correlated gases, grain size fractions were prepared. The results of the instrumental measurements of the gamma radiation are listed. From the amounts of cosmic ray produced noble gases and respective production rates, the lunar surface residence times were calculated. It was concluded that the lunar surface time is about half a billion years.

Kraehenbuehl, U.↗

Isotope analysis of crystalline impact melt rocks from Apollo 16 stations 11 and 13, North Ray Crater

The North Ray Crater Target Rock Consortium was formed to study a large number of rake samples collected at Apollo 16 stations 11 and 13 with comparative chemical, mineralogical, and chronological techniques in order to provide a larger data base for the discussion of lunar highland evolution in the vicinity of the Apollo 16 landing region. The present investigation is concerned with Rb-Sr and Sm-Nd isotopic analyses of a number of whole-rock samples of feldspathic microporhyritic (FM) impact melt, a sample type especially abundant among the North Ray crater (station 11) sample collection. Aspects of sample mineralogy and analytical procedures are discussed, taking into account FM impact melt rocks 6715 and 63538, intergranular impact melt rock 67775, subophitic impact melt rock 67747, subophitic impact melt rock 67559, and studies based on the utilization of electron microscopy and mass spectroscopy.

Reimold, W. U.↗

Proton emission in ultraperipheral Pb-Pb collisions at $\sqrt{𝑠_{𝑁⁢𝑁}}$ = 5.02 TeV

The first measurements of proton emission accompanied by neutron emission in the electromagnetic dissociation (EMD) of 208 Pb nuclei in the ALICE experiment at the Large Hadron Collider are presented. The EMD protons and neutrons emitted at very forward rapidities are detected by the proton and neutron zero degree calorimeters of the ALICE experiment. The emission cross sections of zero, one, two, and three protons accompanied by at least one neutron were measured in ultraperipheral 208 Pb − 208 Pb collisions at a center-of-mass energy per nucleon pair $\sqrt{𝑠_{𝑁⁢𝑁}}$ = 5.02TeV. The 0p and 3p cross sections are described by the RELDIS model within their measurement uncertainties, while the 1p and 2p cross sections are underestimated by the model by 17–25%. According to this model, these 0p, 1p, 2p, and 3p cross sections are associated, respectively, with the production of various isotopes of Pb, Tl, Hg, and Au in the EMD of 208 Pb . The cross sections of the emission of a single proton accompanied by the emission of one, two, or three neutrons in EMD were also measured. The data are significantly overestimated by the RELDIS model, which predicts that the (1p,1n), (1p,2n), and (1p,3n) cross sections are very similar to the cross sections for the production of the thallium isotopes 206,205,204 Tl.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Isotopic composition of Murchison organic compounds: Intramolecular carbon isotope fractionation of acetic acid. Simulation studies of cosmochemical organic syntheses

Recently, in our laboratories, samples of Murchison acetic acid were decarboxylated successfully and the carbon isotopic composition was measured for the methane released by this procedure. These analyses showed significant differences in C-13/C-12 ratios for the methyl and carboxyl carbons of the acetic acid molecule, strongly suggesting that more than one carbon source may be involved in the synthesis of the Murchison organic compounds. On the basis of this finding, laboratory model systems simulating cosmochemical synthesis are being studied, especially those processes capable of involving two or more starting carbon sources.

Yuen, G. U.↗

Gamma Rays as a Signature of r -process Producing Supernovae: Remnants and Future Galactic Explosions

We consider the question of whether core-collapse supernovae (CCSNe) can produce rapid neutron capture process (r-process) elements and how future MeV gamma-ray observations could address this. Rare types of CCSNe characterized by substantial magnetic fields and rotation, known as magnetorotational supernovae (MR-SNe), are theoretically predicted to produce these elements, although direct observational evidence is lacking. We suggest that this critical question be addressed through the study of some of the 11 CCSN remnants located within 10 kpc, as well as through the detection of gamma-ray emission from a future Galactic supernova. We use a two-dimensional MR-SN model to estimate the expected gamma flux stemming from nuclear decays in the range of a few tens of keV to a few MeV. Our results indicate that an observation of 126 Sn ( 126 Sb) in a remnant stands out as a signature of an r-process-producing supernova. Since the neutron-rich conditions that lead to the production of the r-process could also enhance the production of 60 Fe, the detection of substantial 60 Fe ( 60 Co) would be indicative of favorable conditions for the r-process. In the case of a future supernova explosion, when the evolution of the spectrum is studied over 10 days to a few years, a rich picture emerges. At various epochs, the second peak r-process isotopes such as 125 Sn, 131 I, 132 Te, 132 I, and 140 La produce signals that are not obscured by the gamma emission from explosive burning products and electron–positron annihilation. The weak r-process isotopes 95 Nb, 103 Ru, and 106 Rh also have periods of prominence.

Gamma-rays↗

Fuel cycle depletion validation and code-to-code verification studies for High Flux Isotope Reactor highly and low-enriched uranium fuel designs

Here, this paper documents fuel cycle depletion validation and code-to-code verification studies for the High Flux Isotope Reactor (HFIR) highly enriched uranium (HEU) and proposed low-enriched uranium (LEU) fuel designs. In support of HFIR’s world-leading performance, transport and depletion simulations are performed to ensure safe operations, design and qualify irradiation experiments, enhance core components and irradiation facilities, and design and characterize LEU fuel designs. Identifying well-validated, computationally efficient codes is required for the success of these efforts. The HFIR Controller, Shift, and VESTA codes were deployed to simulate HEU uranium–oxide dispersion fuel cycles at 85, 95, and 100 MW operations, as well as LEU fuel cycles operating at 95 MW with uranium–silicide dispersion and uranium–molybdenum monolithic alloy fuel forms. Excellent agreement between the codes and with experimentally obtained 235 U enrichment distributions provides increased confidence in the ability of these codes to model and simulate HFIR’s unique core design.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A genomic timescale of prokaryote evolution: insights into the origin of methanogenesis, phototrophy, and the colonization of land

BACKGROUND: The timescale of prokaryote evolution has been difficult to reconstruct because of a limited fossil record and complexities associated with molecular clocks and deep divergences. However, the relatively large number of genome sequences currently available has provided a better opportunity to control for potential biases such as horizontal gene transfer and rate differences among lineages. We assembled a data set of sequences from 32 proteins (approximately 7600 amino acids) common to 72 species and estimated phylogenetic relationships and divergence times with a local clock method. RESULTS: Our phylogenetic results support most of the currently recognized higher-level groupings of prokaryotes. Of particular interest is a well-supported group of three major lineages of eubacteria (Actinobacteria, Deinococcus, and Cyanobacteria) that we call Terrabacteria and associate with an early colonization of land. Divergence time estimates for the major groups of eubacteria are between 2.5-3.2 billion years ago (Ga) while those for archaebacteria are mostly between 3.1-4.1 Ga. The time estimates suggest a Hadean origin of life (prior to 4.1 Ga), an early origin of methanogenesis (3.8-4.1 Ga), an origin of anaerobic methanotrophy after 3.1 Ga, an origin of phototrophy prior to 3.2 Ga, an early colonization of land 2.8-3.1 Ga, and an origin of aerobic methanotrophy 2.5-2.8 Ga. CONCLUSIONS: Our early time estimates for methanogenesis support the consideration of methane, in addition to carbon dioxide, as a greenhouse gas responsible for the early warming of the Earths' surface. Our divergence times for the origin of anaerobic methanotrophy are compatible with highly depleted carbon isotopic values found in rocks dated 2.8-2.6 Ga. An early origin of phototrophy is consistent with the earliest bacterial mats and structures identified as stromatolites, but a 2.6 Ga origin of cyanobacteria suggests that those Archean structures, if biologically produced, were made by anoxygenic photosynthesizers. The resistance to desiccation of Terrabacteria and their elaboration of photoprotective compounds suggests that the common ancestor of this group inhabited land. If true, then oxygenic photosynthesis may owe its origin to terrestrial adaptations.

Methane/metabolism↗

The internal structure and geodynamics of Mars inferred from a 4.2-Gyr zircon record

Combining U–Pb ages with Lu–Hf data in zircon provides insights into the magmatic history of rocky planets. The Northwest Africa (NWA) 7034/7533 meteorites are samples of the southern highlands of Mars containing zircon with ages as old as 4476.3 ± 0.9 Ma, interpreted to reflect reworking of the primordial Martian crust by impacts. We extracted a statistically significant zircon population (n= 57) from NWA 7533 that defines a temporal record spanning 4.2 Gyr. Ancient zircons record ages from 4485.5 ± 2.2 Ma to 4331.0 ± 1.4 Ma, defining a bimodal distribution with groupings at 4474 ± 10 Ma and 4442 ± 17 Ma. We interpret these to represent intense bombardment episodes at the planet’s surface, possibly triggered by the early migration of gas giant planets. The unradiogenic initial Hf-isotope composition of these zircons establishes that Mars’s igneous activity prior to ~4.3 Ga was limited to impact-related reworking of a chemically enriched, primordial crust. A group of younger detrital zircons record ages from 1548.0 ± 8.8 Ma to 299.5 ± 0.6 Ma. The only plausible sources for these grains are the temporally associated Elysium and Tharsis volcanic provinces that are the expressions of deep-seated mantle plumes. The chondritic-like Hf-isotope compositions of these zircons require the existence of a primitive and convecting mantle reservoir, indicating that Mars has been in a stagnant-lid tectonic regime for most of its history. Our results imply that zircon is ubiquitous on the Martian surface, providing a faithful record of the planet’s magmatic history.

58 GEOSCIENCES↗

Abrasion-fission reactions at intermediate energies

The availability of high-intensity, heavy-ion beams coupled to sensitive, large solid-angle acceptance spectrometers has enabled a detailed examination of the fission fragments produced in induced-fission reactions. The abrasion fission process involves the formation of projectile-like prefragments in violent nuclear collisions at relative energies in excess of 100 MeV/u. At intermediate energies below this threshold, experiments suggest a change in the prefragment kinematic qualities. Information regarding the influence of this transitional phase upon the evolution of nuclei approaching the point of scission is scarce. In this article, data are presented for over 200 nuclei from nickel to palladium produced in abrasion-fission reactions of a 80 MeV/u 238 U beam. Cross sections were obtained following yield measurements performed for the principal charge states of the identified fission fragments and a detailed analysis of the ion transmission. A full kinematic analysis of the fission fragments has been performed using the LISE ++ software package, where the trajectory of an ion passing through a spectrometer can be reconstructed based upon measurements at the focal plane. Furthermore, the results obtained at the S800 spectrograph are compared with predictions obtained with a three-fission progenitor (3EER) model. Systematic studies of fission-fragment properties continue to provide a valuable experimental benchmark for theoretical efforts directed toward describing this complex decay channel, that is important in the context of planning experiments to explore the neutron-rich region of the nuclear chart at rare-isotope beam facilities.

59 ≤ A ≤ 8990 ≤ A ≤ 149↗

Development of Analytical Method for Measuring U and Pu Particles by Laser Ablation MC-ICP-MS for the NWAL

This project will develop methodology to identify and analyze U and Pu containing particles using laser ablation MC-ICP-MS. The proposed work will involve: i) setup and optimization of the LA-MC-ICP-MS system, ii) testing and validation by analysis of QC standards, iii) designing analytical protocols for single particles, and iv) developing a data processing system. Ultimately, this project will output a detailed operating procedure documenting the experimental techniques and data processing routines required to perform particle identification and analysis by laser ablation MC-ICP-MS.

07 ISOTOPE AND RADIATION SOURCES↗