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An all-digital associated particle imaging system for the 3D determination of isotopic distributions
Associated particle imaging (API) is a non-destructive nuclear technique for the 3D determination of isotopic distributions. By detecting the alpha particle associated with the emitted neutron in the deuterium–tritium fusion reaction with a position- and time-resolving detector, the direction of the 14.1 MeV neutron and its time of emission can be determined. Employing this method, isotope characteristic gamma rays emitted in inelastic neutron scattering events can be correlated with the neutron interaction location. Here, an API system consisting of a sealed-type neutron generator, gamma detectors, and a position-sensitive alpha detector was designed, constructed, and characterized. The system was tested with common soil elements and shown to be sensitive to 12 C, 16 O, 28 Si, 27 Al, and 56 Fe. New aspects of our approach are the use of a yttrium–aluminum–perovskite scintillator, using a sapphire window instead of a fiber-optic faceplate for light transport to the photomultiplier, and the all-digital data acquisition system. We present a description of the system with simulations and experimental results that show a position resolution on the alpha detector of 1 mm, a depth resolution using a LaBr 3 detector of 6.2 cm, and an angular resolution of 4.5°. Additionally, we present single-element gamma response measurements for the elements mentioned above together with a comparison to Monte Carlo simulations (MCNP6).
Format Proposal for Isotopic Distribution in TSL Files for ENDF/B-VIII.1 [Slides]
This presentation proposes a format of an ‘footer’ file for ENDF6-format TSL files. This would contain several pieces of pertinent information for the scattering atom. such as the Number of scattering atoms in molecule, Isotopic distribution within scattering atom, and free atom and atomic weight ratios for each isotope. This setup will not require significant changes to processing codes or to other sections of the MF7 file.
Computer programs for the interpretation of low resolution mass spectra: Program for calculation of molecular isotopic distribution and program for assignment of molecular formulas
Two FORTRAN computer programs for the interpretation of low resolution mass spectra were prepared and tested. One is for the calculation of the molecular isotopic distribution of any species from stored elemental distributions. The program requires only the input of the molecular formula and was designed for compatability with any computer system. The other program is for the determination of all possible combinations of atoms (and radicals) which may form an ion having a particular integer mass. It also uses a simplified input scheme and was designed for compatability with any system.
Inter- and intra-crystalline oxygen isotope distribution of fassaites in Allende CAI
Calcium, aluminum-rich inclusions (CAI's) from carbonaceous chondrite are believed to be among the first solids to have formed in the early solar system and thus to preserve a record of conditions and processes that prevailed early in the solar nebula. We have measured inter- and intra- crystalline oxygen isotope distribution of fassaite in Type B1 CAI of Allende meteorite. Secondary ion mass spectrometry (SIMS) using negative Au primary ion was applied to in situ oxygen isotope ratio analysis on a polished thin section of the CAI. Present data indicate that O isotope composition is homogeneous inside of fassaite grains as well as among grains in the HN3-1 CAI, and that the delta(exp 18) O value (-24.14 percent relative to SMOW) determined previously could be applied to most fassaite grains. The results suggest that most fassaite grains are preexisting solids like spinel grains.
Intramolecular 13 C isotope distributions of butane from natural gases
A single-step method allowing the measurement of 13 C intramolecular distribution of butane isomers (n- and i-butane) from natural gas samples was developed. The method builds up on the one that has been developed for propane, using on-line pyrolysis followed by isotope analysis of the pyrolytic fragments. The isotopic filiation between n-butane and its pyrolytic fragments was elucidated using samples spiked with 13 C on terminal positions. The isotopic filiation for i-butane could not be shown experimentally due to the lack of commercially available enriched i-butane. We thus used a recent model named Reaction Mechanism Generator (RMG) to assess the origin of the fragments arising from i-butane pyrolysis. Butanes from natural gas samples from the Carnarvon Basin (Australia) and the Arkoma Basin (USA) were analyzed. The results are consistent with a model for thermogenic natural gas generation and suggest that combined intramolecular isotope composition of propane and n-butane can be related to the gas maturity. In addition, the method allows the detection and shed light on the mechanism of n-butane and i-butane biodegradation in natural gas reservoirs.
Analysis of intramolecular carbon isotope distributions in alanine by electrospray ionization Orbitrap mass spectrometry
Not Available
Multimodal Imaging of Light Isotope Distributions in Irradiated Materials
This is the platform presentation proceeding paper.
Spatial distribution of pulmonary blood flow in dogs in increased force environments
Spatial distribution of pulmonary blood flow during 2- to 3-min exposures to 6-8 Gy acceleration was studied, using radioactive microspheres in dogs, and compared to previously reported 1 Gy control distributions. Isotope distributions were measured by scintiscanning individual 1-cm-thick cross sections of excised, fixed lungs. Results indicate: (1) the fraction of cardiac output traversing left and right lungs did not change systematically with the duration and magnitude of acceleration; but (2) the fraction is strongly affected by the occurrence or absence of fast deep breaths, which cause an increase or decrease, respectively, in blood flow through the dependent lung; and (3) Gy acceleration caused a significant increase in relative pulmonary vascular resistance (PVR) in nondependent and dependent regions of the lung concurrent with a decrease in PVR in the midsagittal region of the thorax.
Calculation of improved spallation cross sections
Several research groups have recently carried out highly precise measurements (to about 10 percent) of high-energy nuclear spallation cross sections. These measurements, above 5 GeV, cover a broad range of elements: V, Fe, Cu, Ag, Ta and Au. Even the small cross sections far off the peak of the isotopic distribution curves have been measured. The semiempirical calculations are compared with the measured values. Preliminary comparisons indicate that the parameters of our spallation relations (Silberberg and Tsao, 1973) for atomic numbers 20 to 83 need modifications, e.g. a reduced slope of the mass yield distribution, broader isotopic distributions, and a shift of the isotopic distribution toward the neutron-deficient side. The required modifications are negligible near Fe and Cu, but increase with increasing target mass.
The Stable Isotope Fractionation of Abiotic Reactions: A Benchmark in the Detection of Life
One very important tool in the analysis of biogenic, and potentially biogenic, samples is the study of their stable isotope distributions. The isotope distribution of a sample depends on the process(es) that created it. One important application of the analysis of C & N stable isotope ratios has been in the determination of whether organic matter in a sample is of biological origin or was produced abiotically. For example, the delta C-13 of organic material found embedded in phosphate grains was cited as a critical part of the evidence for life in 3.8 billion year old samples. The importance of such analysis in establishing biogenicity was highlighted again by the role this issue played in the recent debate over the validity of what had been accepted as the Earth s earliest microfossils. These kinds of analysis imply a comparison with the fractionation that one would have seen if the organic material had been produced by alternative, abiotic, pathways. Could abiotic reactions account for the same level of fractionation? Additionally, since the fractionation can vary between different abiotic reactions, understanding their fractionations can be important in distinguishing what reactions may have been significant in the formation of different abiological samples (such as extraterrestrial samples). There is however, a scarcity of data on the fractionation of carbon and nitrogen by abiotic reactions. In order to interpret properly what the stable isotope ratios of samples tell us about their biotic or abiotic nature, more needs to be known about how abiotic reactions fractionate C and N. Carbon isotope fractionations have been studied for a few abiotic processes. These studies presumed the presence of a reducing atmosphere, focusing on reactions involving spark discharge, W photolysis of reducing gas mixtures, and cyanide polymerization in the presence of ammonia. They did find that the initial products showed a depletion in I3C with values in the range of a few per mil to as low as -60 % (potentially comparable to that which accompanies the biosynthesis of organic matter). We need to understand what kind of fractionations are observed with reactions under the non-reducing or mildly reducing conditions now thought to be present on the early Earth. While nitrogen is receiving increased attention as a tool for these kinds of analyses, almost nothing is known about the isotope fractionation that one would expect for abiotic sources of fixed/reduced nitrogen. This project will measure the fixation from a series of abiotic reactions that may have been present on the early Earth (and other terrestrial planets) and produced organic material that could have ended up in the rock record. The work will look at a number of reactions, under a non- reducing, or mildly reducing, atmosphere, covering sources of prebiotic organic C & N from shock heating, to photochemistry, to hydrothermal reactions. Some reactions that we plan to study are; Shock heating of a non-reducing atmosphere to produce CO and NO (in collaboration with Chris McKay), formation of formaldehyde (and related compounds) from COY the formation of ammonia from nitrogen oxides (ultimately from NO) by ferrous iron reduction, and the hydrothermal synthesis of compounds including the hydrocarboxylation/hydrocarbonylation reaction (in collaboration with George Cody), reactions of oxalate to form hydrocarbons and other oxygenated compounds and the formation of lipids from oxalic/formic acid (in collaboration with Tom McCollom), and reactions of carbon monoxide & carbon dioxide with N2, ammonia or nitritehitrate to form hydrogen cyanide, nitriles, ammonia/amines and nitrous
Carbon, nitrogen and sulfur in lunar fines 15012 and 15013 - Abundances, distributions and isotopic compositions
Lunar fines 15012,16 and 15013,3 were analyzed by stepwise pyrolysis and acid hydrolysis as well as complete combustion in oxygen to determine carbon, nitrogen and sulfur. In addition, hydrogen was analysed during pyrolysis as well as during hydrolysis. By comparison of the distribution frequencies of C, N, S, H2 and Fe with He-4, considered to have arisen from solar wind contribution, it is concluded that nitrogen and hydrogen have largely a solar origin. Carbon has a significant solar contribution, and metallic iron may have resulted from solar wind interaction with ferrous minerals on the lunar surface. Sulfur probably has a predominantly lunar origin. There is no direct evidence for meteorotic contribution to these samples. Solar wind interaction also has a marked effect on the stable isotope distribution of C-13/C-12, N-15/N-14, and S-34/S-32. In all cases, the heavy isotope was most enriched in the smallest grain-size fraction.
Benchmark for Fuel Shuffling and Depletion for Pebble-Bed Reactors
Pebble bed reactors have specific operational characteristics when their fuel-cycle and fueling operations are considered. They are specifically distinguished by other type of nuclear reactor designs by their online fuel recycling scheme, where the fuel elements that have not yet reached discharge burnup can be reloaded and recycled continuously during normal operation. The fuel in a pebble bed reactor is not stationary and stochastically moves through the core once or several times during its lifetime, which allows them to operate without requiring a large excess reactivity hold for the burnup. However, this characteristic of pebble bed reactors introduces challenges in simulation, as each pebble can take many different trajectories through the core, its composition depends on the details of the irradiation history that is unique to its aggregated path through the core. For predicting the safety performance characteristics, such as source term, maximum fuel temperatures and fuel failure rates, etc., it is important to accurately incorporate the movement of pebbles through the core during their lifetime in a multi-physics simulation together with other phenomena. The equilibrium core analysis for pebble bed reactors are performed with multi-physics tools including fuel depletion in a multi pass reload coupled to the fuel movement. Currently, there are only a few legacy multi-physics simulation tools that can implement the pebble flow characteristics and perform equilibrium core analysis for pebble bed reactors. However, there are development efforts on-going under Department of Energy's Nuclear Energy Advanced Modelling and Simulation program and also in private industry for including these capabilities into their modelling and simulation tools. Any new development in the modelling and simulation tools needs to be validated by using tools such as experiments, analytical solutions or code-to-code benchmarks. In this work, a code-to-code benchmark for the equilibrium core analysis capability of pebble bed reactors was developed. Multiple cases were identified to capture different fuel cycle strategies that can be used in PBRs. The results of each case are presented in terms of overall equilibrium core characteristics: the discharge burnup; spatial burnup distribution; spatial isotopic distributions; axial and radial neutron flux distributions and power history of fuel elements per pass through the core for both a prototypical pebble bed High Temperature Gas-cooled Reactor and a prototypical pebble bed Fluoride-salt cooled High temperature Reactor.
Utilization of traceable standards to validate plutonium isotopic purification and separation of plutonium progeny using AG MP-1M resin for nuclear forensic investigations
Radio-chronometric studies on plutonium (Pu) materials require independent measurement of the Pu (parent) content and isotopic distribution as well as concentration and isotopic distribution of the plutonium isotopic decay products. We performed a series of experiments to demonstrate the consistency of separations using the Lewatit MP 800 macroporous anion exchange resin and the AG MP-1M resin with traceable Pu isotopic certified reference material (CRM) standards 136, 137, 138, and 126-A. Two different mesh-sizes of the AG MP-1M resin were tested and the 50–100 mesh size resin was found to work more efficiently for the separation task. Both Lewatit and AG MP-1M resins were found to perform satisfactorily for quantitatively extracting the americium (Am) and uranium (U) progeny as well as gallium (Ga) present as a tracer in the Pu material. Both resins were effective in removing isobaric interferences from the Pu fraction used in isotopic measurements by thermal ionization mass spectrometry (TIMS). To address the co-elution of uranium and gallium, Alizarin red S (ARS) was used as a colorimetric dye to determine the behavior of UO 2 2+ and Ga 3+ on AG MP-1M resin with various acidic solutions as eluents using UV–vis spectra. Poor resolution of these peaks complicated quantitative analysis by UV–vis spectroscopy, but these results were informative in planning automated separation experiments by HPLC. LA-UR-24-28919.
FRAM, Version 6.1 User Manual
This manual describes the use of version 6.1 of the FRAM gamma-ray isotopic analysis software developed in the Safeguards Science and Technology Group, NEN-1, Nuclear Engineering & Nonproliferation Division, Los Alamos National Laboratory. The software analyzes the gamma ray spectrum from plutonium-bearing items and determines the isotopic distribution of the plutonium, 241Am content, and concentration of other isotopes in the item. The software can also determine the isotopic distribution of uranium isotopes in items containing only uranium. The body of this manual describes the generic version of the code.
Momentum distributions of isotopes produced by fragmentation of relativistic C-12 and O-16 projectiles
The fragment momentum distributions in the projectile rest frame are, typically, Gaussian shaped, narrow, consistent with isotropy, depend on fragment and projectile, and have no significant correlation with target mass or beam energy. The nuclear temperature is inferred from the momentum distributions of the fragments and is approximately equal to the projectile nuclear binding energy, indicative of small energy transfer between target and fragment.
Distribution and origin of helium, neon, and argon isotopes in Apollo 12 samples measured by in situ analysis with a laser-probe mass spectrometer
He, Ne and Ar isotopic distribution and origin in Apollo 12 lunar samples, considering solar wind implantation