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A Chlorine Isotope Transect Across the Sudbury Impact Deposits Reveals Enigmatic Isotopic Fractionation

Volatile elements play an important role in a variety of cosmochemical and geochemical processes. As such, there has been significant interest in their abundance and isotopic composition. Chlorine is an important element for tracing these processes because it is incompatible in nearly all minerals, extremely volatile, and strongly hydrophilic [1]. The Cl isotope composition ( 37 Cl/ 35 Cl) of meteoritic components, therefore, can provide useful information regarding the isotopic reservoirs that were present in the early Solar System and any secondary processes that may have occurred on different parent bodies (e.g., [2-4]). There is a relatively narrow range in the Cl isotope compositions of terrestrial, Martian, and chondritic meteorites (δ 37 Cl ~ −6 to +4‰) (e.g., [2,3,5,6]), with exceptions to this being the Moon and Vesta (up to ~ +81‰ and ~ +40‰, respectively) [4, 5, 7-10]. One hypothesis for the extreme Cl isotope fractionation observed on the Moon is degassing following large-scale (possibly even crust-breaching) impact events [7-9]. The role of hypervelocity impacts and impact-generated magmatism in the isotopic evolution of planetary materials, however, has been until recently an area of limited published research with the majority of works focusing on the effects of impact shock (e.g., [10-13]). The ~ 1.85 Ga Sudbury impact crater [14] located in Ontario, Canada, is one of the three largest impact craters on Earth with good exposures of its impact melt sheet and overlying breccias [15,16]. The impact melt sheet, called the Sudbury Igneous Complex (SIC), is up to 5 km thick [17], with an estimated original volume of >10 4 km 3 [18], and differentiated. Recent work demonstrated evaporative loss and isotope fractionation of the moderately volatile element zinc and suggest melt sheets produced by impacts could have a significant effect on the Earth’s volatile inventory [19]. In this study we investigate the abundance and isotopic composition of Cl as well the water abundance of apatite from the SIC and the overlying crater-fill to test the hypothesis that large-scale impacts may have generated the extensive Cl isotopic fractionation observed on the Moon.

Sudbury↗
DOE OSTI2021

Global Microscopic Description of Nucleon-Nucleus Scattering with Quantified Uncertainties

We develop for the first time a microscopic global nucleon-nucleus optical potential with quantified uncertainties suitable for analyzing nuclear reaction experiments at next-generation rare-isotope beam facilities. Within the improved local density approximation and without any adjustable parameters, we begin by computing proton-nucleus and neutron-nucleus optical potentials from a set of five nuclear forces from chiral effective field theory for 1800 target nuclei in the mass range 12 ≤ A ≤ 242 for energies between 0 MeV < E ≲ 150 MeV. We then parameterize a global optical potential for each chiral force that depends smoothly on the projectile energy as well as the target nucleus mass number and isospin asymmetry. Uncertainty bands for elastic scattering observables are generated from a full covariance analysis of the parameters entering in the description of our global optical potential and benchmarked against existing experimental data for stable target nuclei. Since our approach is purely microscopic, we anticipate a similar quality of the model for nucleon scattering on unstable isotopes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Accelerating the development of a sustainable bioenergy portfolio through stable isotopes

Bioenergy could help limit global warming to 2°C above pre-industrial levels while supplying almost a fourth of the world's renewable energy needs by 2050. However, the deployment of bioenergy raises concerns that adoption at meaningful scales may lead to unintended negative environmental consequences. Meanwhile, the full consolidation of a bioenergy industry is currently challenged by a sufficient, resilient, and resource-efficient biomass supply and an effective conversion process. Here, we provide a comprehensive analysis of how stable isotope approaches have accelerated the development of a robust bioeconomy by advancing knowledge about environmental sustainability, feedstock development, and biological conversion. We show that advances in stable isotope research have generated crucial information to (1) gain mechanistic insight into the potential of bioenergy crops to mitigate climate change as well as their impact on water and nutrient cycling; (2) develop high-yielding, resilient feedstocks that produce high-value bioproducts in planta; and (3) engineer microbes to enhance feedstock conversion to bioenergy products. Further, we highlight knowledge gaps that could benefit from future research facilitated by stable isotope approaches. We conclude that advances in mechanistic knowledge and innovations within the field of stable isotopes in cross-disciplinary research actions will greatly contribute to breaking down the barriers to establishing a robust bioeconomy.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

Status Update on the High Precision Isotopic Measurements on High Burnup LWR Fuel in 2020

The US Department of Energy (DOE) Office of Nuclear Energy (NE) is currently investigating the feasibility of directly disposing dual-purpose (storage and transportation) canisters (DPCs) in a spent nuclear fuel (SNF) repository. Criticality during the repository performance period (10,000 years or more) is one of the major concerns related to direct disposal of DPCs, specifically as the system undergoes degradation in the repository environment and timeframe. Oak Ridge National Laboratory (ORNL) is developing an as-loaded criticality analysis methodology using full (actinides + fission products) burnup credit that exploits the inherent criticality margin associated with actual canister-specific loading configuration. Burnup credit criticality analysis requires validation of the depletion/decay codes used to generate the burned isotopic inventory of an assembly by comparing the code-predicted inventory with experimentally determined isotopic data. Currently, isotopic measurement data for boiling water reactors (BWR) SNF are limited, and additional measurements will be highly beneficial for BWR burnup credit analysis, which is essential to demonstrate disposability of BWR DPCs. Moreover, new pressurized water reactor (PWR) samples of isotopic measurements will expand the PWR sample population and consequently will greatly improve sample statistics. In turn, this will reduce uncertainty in the computational determination of the isotopic composition of commercial SNF and eliminate additional penalties currently used for lack of data. As part of the isotopic analysis task, eight diverse, high burnup (HBU) samples from several PWR rods are being dissolved and isotopically analyzed to provide high-quality measurement data for PWR SNF to reducing the uncertainties associated with PWR isotopic depletion validation. The isotopics of interest focus on nuclides important to burnup credit, shielding, and decay heat in PWR SNF. Additionally, eight high burnup BWR fuel samples from the Limerick nuclear power plant have been identified for measurement to support reducing uncertainties associated with BWR isotopic depletion validation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS1972

Manned space flight nuclear system safety. Volume 5: Nuclear System safety guidelines. Part 1: Space base nuclear safety

The design and operations guidelines and requirements developed in the study of space base nuclear system safety are presented. Guidelines and requirements are presented for the space base subsystems, nuclear hardware (reactor, isotope sources, dynamic generator equipment), experiments, interfacing vehicles, ground support systems, range safety and facilities. Cross indices and references are provided which relate guidelines to each other, and to substantiating data in other volumes. The guidelines are intended for the implementation of nuclear safety related design and operational considerations in future space programs.

Source record↗
NASA NTRS1992

Cosmic ray composition investigations using ICE/ISEE-3

The analysis of data from the high energy cosmic experiment on ISEE-3 and associated modeling and interpretation activities are discussed. The ISEE-3 payload included two instruments capable of measuring the composition of heavy cosmic rays. The designs of these two instruments incorporated innovations which made it possible, for the first time, to measure isotopic as well as the chemical composition for a wide range of elements. As the result of the demonstrations by these two instruments of the capability to resolve individual cosmic ray isotopes, a new generation of detectors was developed using very similar designs, but having improved reliability and increased sensitive area. The composition measurements which were obtained from the ISEE-3 experiment are summarized.

Wiedenbeck, Mark E.↗
NASA NTRS2018

Low Power Radioisotope Conversion Technology and Performance Summary

This work presents a summary of low-power radioisotope-based power sources. This includes systems that use direct energy conversion from radioactive decay such as betavoltaics and systems that convert heat generated by the isotope decay. These types of power systems have terrestrial and space-based applications. Their main application is to provide low levels of power in remote environments where long life and reliability are the main objectives. This work looked at the potential performance of these types of systems and the range of output power they can achieve. Also considered was the amount of power that could be achieved from these different conversion technologies, while remaining under the critical limit acceptable for space flight without the need for special handling and controls. This is of interest for space missions where low power levels can be used for operating sensors or other devices, but the expense associated with the incorporation of radioactive material above this critical level would be cost prohibitive.

Colozza, Anthony J.↗
DOE OSTI2020

Process for the separation and purification of medical isotopes

The invention provides a method for isolating medical isotopes, the method having the steps of dissolving titanium nuclear targets to create a solution; contacting the solution with a resin so as to retain the isotopes on the resin and generate an eluent containing titanium; contacting the isotope-containing resin with acid of a first concentration to remove impurities from the resin; and contacting the isotope-containing resin with an acid of a second concentration to remove isotope from the resin.

07 ISOTOPE AND RADIATION SOURCES↗
NASA NTRS1983

Sulphur isotopic compositions of deep-sea hydrothermal vent animals

The S-34/S-32 ratios of tissues from vestimentiferan worms, brachyuran crabs, and giant clams living around deep hydrothermal vents are reported. Clean tissues were dried, ground, suspended in 0.1 M LiCl, shaken twice at 37 C to remove seawater sulfates, dried at 60 C, combusted in O2 in a Parr bomb. Sulfur was recovered as BaSO4, and the isotopic abundances in SO2 generated by thermal decomposition of 5-30-mg samples were determined using an isotope-ratio mass spectrometer. The results are expressed as delta S-34 and compared with values measured in seawater sulfates and in normal marine fauna. The values ranged from -4.7 to 4.7 per thousand, comparable to vent sulfide minerals (1.3-4.1 per thousand) and distinct from seawater sulfates (20.1 per thousand) and normal marine fauna (about 13-20 per thousand). These results indicate that vent sulfur rather than seawater sulfur is utilized by these animals, a process probably mediated by chemoautotrophic bacteria which can use inorganic sulfur compounds as energy sources.

Fry, B.↗
NASA NTRS2001

The Origin of Noble Gas Isotopic Heterogeneity in Icelandic Basalts

Two models for generation of heterogeneous He, Ne and Ar isotopic ratios in Icelandic basalts are evaluated using a mixing model and the observed noble gas elemental ratios in Icelandic basalts,Ocean island Basalt (OIBs) and Mid-Ocean Ridge Basalt (MORBs). Additional information is contained in the original extended abstract.

Dixon, E. T.↗
DOE OSTI2023

LISE$^{++}_{cute}$, the latest generation of the LISE ++ package, to simulate rare isotope production with fragment-separators

The LISE ++ software for fragment separator simulations has undergone a major update. The package, widely used at rare isotope beam facilities, can be used to predict intensities and purities of rare isotope beams and for planning and running of experiments using in-flight separators. It is especially useful for radioactive beam production as its results can be quickly compared to on-line data. The LISE ++ package has been ported to the Qt-framework in order to support modern compilers and computing methods. The benefits include 64-bit operation and LISE ++ availability on three different platforms: Windows, MacOS and Linux. In addition, the porting provides the ability to take advantage of future computational improvements. The updated package is named LISE$^{++}_{cute}$ to indicate a major step forward from the previous Borland-based versions. In addition to porting to the new platform, new main features and modifications have been added, mostly devoted to improving models and implementing other codes involved in rare isotope production at FRIB. Finally, a summary of modifications completed to improve the functionality of the code are discussed in this work, as well as future plans.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

R -Matrix Analysis and Statistical Properties of Dysprosium Isotopes in the Neutron Energy Ranges Up To A Few Kev

In support of the Nuclear Criticality Safety Program, a set of evaluated resonance parameters was generated for seven dysprosium isotopes in the neutron energy range from thermal up to a few keV. The evaluation methodology used the Reich-Moore approximation to fit, with the R-matrix code SAMMY, the high-resolution capture and transmission measurements on natural and enriched samples recently performed at the Rensselaer Polytechnic Institute Gaerttner LINear ACcelerator facility. Additional transmission data measured on enriched samples by Liou at the Columbia University Nevis synchrocyclotron in the mid-seventies were used to gauge the neutron widths above 15 eV. Thermal constants such as absorption and (in)coherent scattering cross sections and corresponding scattering lengths were calibrated to the National Institute of Standards and Technology’s compilation except for 161,164 Dy isotopes.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2020

Epithermal Neutron Resonance Analysis Using a Compact D-T Generator

Nuclear material identification and isotopic composition analysis are important capabilities for safeguards and the verification of nuclear arms control and nonproliferation treaties. Epithermal neutron resonance imaging has been proposed for spent fuel assay measurements, and the development of a mobile neutron imaging system could provide such a tool for on-site applications. This technique is highly sensitive to isotopes of interest for safeguards applications (e.g. 235,238 U, 238,239,240 Pu) and yields unique transmission spectra for a target containing actinides and some mid- and high-Z elements. Paired with a position-sensitive neutron detector, such a system could provide spatial information of the target isotopic composition. Recent progress in the development of high intensity neutron sources could make mobile epithermal neutron imaging designs increasingly feasible to serve as a tool for nuclear inspectors. In this work, Monte Carlo (MC) simulations were performed to further optimize a previous design for an epithermal neutron resonance-based analysis apparatus using a D-T portable neutron generator. Additionally, experimental work is being performed to test the feasibility of this method. The MC simulations of moderation time distributions for different moderator compositions and thicknesses were measured to provide a multi-group correction for neutron time-of-flight energy reconstruction.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
NASA NTRS2010

Trace Gas Measurements on Mars and Earth Using Optical Parametric Generation

Trace gases and their isotopic ratios in planetary atmospheres offer important but subtle clues as to the origins of a planet's atmosphere, hydrology, geology, and potential for biology. An orbiting laser remote sensing instrument is capable of measuring trace gases on a global scale with unprecedented accuracy, and higher spatial resolution that can be obtained by passive instruments. We have developed an active sensing instrument for the remote measurement of trace gases in planetary atmospheres (including Earth). The technique uses widely tunable, seeded optical parametric generation (OPG) to measure methane, CO2, water vapor, and other trace gases in the near and mid-infrared spectral regions. Methane is a strong greenhouse gas on Earth and it is also a potential biogenic marker on Mars and other planets. Methane in the Earth's atmosphere survives for a shorter time than CO2 but its impact on climate change can be larger than CO2. Methane levels have remained relatively constant over the last decade around 1.78 parts per million (ppm) but recent observations indicate that methane levels may be on the rise. Increasing methane concentrations may trigger a positive feedback loop and a subsequent runaway greenhouse effect, where increasing temperatures result in increasing methane levels. The NRC Decadal Survey recognized the importance of global observations of greenhouse gases and called for simultaneous CH4, CO, and CO2 measurements but also underlined the technological limitations for these observations. For Mars, methane measurements are of great interest because of its potential as a strong biogenic marker. A remote sensing instrument that can measure day and night over all seasons and latitudes can identify and localize sources of biogenic gas plumes produced by subsurface chemistry or biology, and aid in the search for extra-terrestrial life. It can identify the dynamics of methane generation over time and latitude and identify future lander mission sites for more detailed in-situ analysis. In this paper we report on remote sensing measurements of methane using a high peak power, widely tunable optical parametric generator (OPG) operating at 3.3 micron and 1.65 micron. The OPG is pumped by a passively q-switched single frequency laser (3ns, 5KHz, 50uJ) and seeded by a diode laser. The spectral width of both signal and idler of seeded OPG is nearly Fourier transform limited. The output of seeded OPG is single frequency with high spectral purity and is widely tunable. Both 1650 nm and 3300 nm can be generated with a conversion efficiency of more than 30%. We have demonstrated detection of methane at 3274 nm and 1650 nm in a cell and also performed open path atmospheric measurements of methane at the same wavelengths. Finally, we were able to demonstrate simultaneous detection of methane at 3270.4 nm and CO2 at 1578.2 nm. In this paper we will discuss the OPG performance and atmospheric open path measurement results.

Numata, Kenji↗
DOE OSTI2020

HFIRCON Version 1.0.5 User Guide

The High Flux Isotope Reactor (HFIR) Controller (HFIRCON) code is a collection of python routines and C plugins that automate the workflow for fuel and single- or multicycle target depletion analyses for HFIR at Oak Ridge National Laboratory (ORNL). This code calls the LAVAMINT (LAVA Model Interrogator) parallel (MCNP) Monte Carlo N-Particle model interrogator to stochastically calculate cell volumes and bounding boxes, the ADVANTG (Automatic Variance Reduction Generation) code package for all variance reduction and source biasing calculations, the ORNL-Transformative Neutronics/MCNP5 transport solver for all transport solutions, and the MSX_DEPLETE module to perform all depletion calculations via the ORIGEN (Oak Ridge Isotope Generation) application programming interface. It also performs a robust set of postprocessing functions to automatically provide summaries of several key metrics that are common to a wide variety of typical HFIR design and safety-basis analyses.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Advancements in Multiphysics Microdepletion Analysis of an eVinci TM -like Microreactor Leveraging OpenMC-CRAB Workflow

Nuclear microreactors (MRs) are a class of nuclear reactor technology, characterized by reduced dimensions, modular design, and reduced power output in contrast to conventional Light Water Reactors (LWRs). MRs are proposed for supplying electricity and eventual process heat to remote locations, such as military installations and disaster-affected areas. Current research work sponsored by the US Department of Energy Microreactor Program (MRP) is devoted to the development of novel modeling and simulation tools to better support MR vendors and regulatory bodies. Notably, the NRC is projected to utilize the CRAB multiphysics software driver for executing both design and beyond-design-basis accident analyses. Furthermore, the NRC has been utilizing the MELCOR code to calculate mechanistic source terms during accidents. Since MELCOR relies on isotopic inventory and reactor temperature/power profiles under accident conditions, which theoretically can be derived from CRAB, the goal is to establish a comprehensive CRAB-MELCOR computational framework. Past work was focused on testing and demonstrating CRAB's capability to generate results that can be used to inform mechanistic source term calculations in MELCOR. In particular, a computational workflow leveraging OpenMC-generated microscopic cross sections and CRAB was first applied to perform multiphysics microscopic depletion calculation followed by an accident scenario for a stylized microreactor problem. In fiscal year 2024, the research work has been focused on applying the OpenMC-CRAB workflow, which was first tested in fiscal year 2023, to a realistic 3D heat-pipe cooled MR problem representative of the eVinci TM design. The latter computational problem was developed with inputs from WEC to conserve selected neutronic and thermal characteristics of the eVinci TM design without releasing proprietary data. The results of this simulation, encompassing isotopic inventory, power density distribution, and kinetic parameters, will inform both MELCOR and the WEC-developed FATE code for mechanistic source terms calculations. The results from the two codes will then be compared for code verification purposes. This report contains the design characteristics of the realist heat pipe cooled microreactor developed as a use-case for the verification exercise, and the current results for the multiphysics microscopic depletion performed with the OpenMC-CRAB workflow. The results include eigenvalue as a function of time, power distribution at EOL, in addition to nuclides inventory's time evolution and spatial distribution. Finally, we report improvements to the workflow efficiency achieved through a collaboration with the NEAMS programs. Through this collaborative effort, we were able to strongly decrease the computational time for the multiphysics microdepletion calculation (i.e., from 17.4 hours to 5.7 hours on 280 processors) in addition to simplifying the interface to generate isotopics spatial distribution utilizable by FATE and MELCOR. Future work, including the improvement of the current microscopic cross-sections' library and the simulation of an accident scenario at EOL, is also discussed.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2023

Engineering a modular 44 Ti/ 44 Sc generator: eluate evaluation in preclinical models and estimation of human radiation dosimetry

Background: 44 Sc/ 47 Sc is an attractive theranostic pair for targeted in vivo positron emission tomographic (PET) imaging and beta-particle treatment of cancer. The 44 Ti/ 44 Sc generator allows daily onsite production of this diagnostic isotope, which may provide an attractive alternative for PET facilities that lack in-house irradiation capabilities. Early animal and patient studies have demonstrated the utility of 44 Sc. In our current study, we built and evaluated a novel clinical-scale 44 Ti/ 44 Sc generator, explored the pharmacokinetic profiles of 44 ScCl 3 , [ 44 Sc]-citrate and [ 44 Sc]-NODAGA (1,4,7-triazacyclononane,1-glutaric acid-4,7-acetic acid) in naïve mice, and estimated the radiation burden of 44 ScCl 3 in humans. Methods: 44 Ti/ 44 Sc (101.2 MBq) in 6 M HCl solution was utilized to assemble a modular ZR resin containing generator. After assembly, 44 Sc was eluted with 0.05 M HCl for further PET imaging and biodistribution studies in female Swiss Webster mice. Based on the biodistribution data, absorbed doses of 44 / 47 ScCl 3 in human adults were calculated for 18 organs and tissues using the IDAC-Dose software. Results: 44 Ti in 6 M HCl was loaded onto the organic resin generator with a yield of 99.97%. After loading and initial stabilization, 44 ScCl 3 was eluted with 0.05 M HCl in typical yields of 82.9 ± 5.3% (N = 16), which was normalized to the estimated generator capacity. Estimated generator capacity was computed based on elution time interval and the total amount of 44 Ti loaded on the generator. Run in forward and reverse directions, the 44 Sc/ 44 Ti ratio from a primary column was significantly improved from 1038 ± 440 to 3557 ± 680 (Bq/Bq) when a secondary, replaceable, ZR resin cartridge was employed at the flow outlet. In vivo imaging and ex vivo distribution studies of the reversible modular generator for 44 ScCl 3 , [ 44 Sc]-citrate and [ 44 Sc]-NODAGA show that free 44 Sc remained in the circulation significantly longer than the chelated 44 Sc. The dose estimation of 44 ScCl 3 reveals that the radiation burden is 0.146 mSv/MBq for a 70 kg adult male and 0.179 mSv/MBq for a 57 kg adult female. Liver, spleen and heart wall will receive the highest absorbed dose: 0.524, 0.502, and 0.303 mGy/MBq, respectively, for the adult male. Conclusions: A clinical-scale 44 Ti/ 44 Sc generator system with a modular design was developed to supply 44 ScCl 3 in 0.05 M HCl, which is suitable for further radiolabeling and in vivo use. Our data demonstrated that free 44 ScCl 3 remained in the circulation for extended periods, which resulted in approximately 10 times greater radiation burden than stably chelated 44 Sc. Stable 44 Sc/ 47 Sc-complexation will be more favorable for in vivo use and for clinical utility.

62 RADIOLOGY AND NUCLEAR MEDICINE↗