Accurate Decay Measurements of Nuclear Isotopes Embedded in Cryogenic Detectors
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A one-and-half-day meeting on the Accelerator Science & Engineering (AS&E) Workforce Roundtable and a one-day meeting of Traineeship Principal Investigators took place at Facility for Rare Isotope Beams at Michigan State University on January 21-23, 2025. The meeting identified critical issues in the AS&E workforce and potential solutions, with a focus on DOE’s major accelerator facilities. The Traineeship PIs meeting focused on sharing experience, efficiency, and improvements of the Traineeship Programs conducted in six US universities. Several managers from the DOE High Energy Physics Office participated in the meetings. The discussions resulted in a decision to conduct similar meetings every year.
Significant improvements in engine readiness with reductions in maintenance costs and turn-around times can be achieved with an engine condition monitoring systems (CMS). The CMS provides health status of critical engine components, without disassembly, through monitoring with advanced sensors. Engine failure reports over 35 years were categorized into 20 different modes of failure. Rotor bearings and turbine blades were determined to be the most critical in limiting turbopump life. Measurement technologies were matched to each of the failure modes identified. Three were selected to monitor the rotor bearings and turbine blades: the isotope wear detector and fiberoptic deflectometer (bearings), and the fiberoptic pyrometer (blades). Signal processing algorithms were evaluated for their ability to provide useful health data to maintenance personnel. Design modifications to the Space Shuttle Main Engine (SSME) high pressure turbopumps were developed to incorporate the sensors. Laboratory test fixtures have been designed for monitoring the rotor bearings and turbine blades in simulated turbopump operating conditions.
Porous electrodes that conduct electrons, protons, and oxygen ions with dramatically expanded catalytic active sites can replace conventional electrodes with sluggish kinetics in protonic ceramic electrochemical cells. In this work, a strategy is utilized to promote triple conduction by facilitating proton conduction in praseodymium cobaltite perovskite through engineering non-equivalent B-site Ni/Co occupancy. Surface infrared spectroscopy is used to study the dehydration behavior, which proves the existence of protons in the perovskite lattice. The proton mobility and proton stability are investigated by hydrogen/deuterium (H/D) isotope exchange and temperature-programmed desorption. It is observed that the increased nickel replacement on the B-site has a positive impact on proton defect stability, catalytic activity, and electrochemical performance. This doping strategy is demonstrated to be a promising pathway to increase catalytic activity toward the oxygen reduction and water splitting reactions. The chosen PrNi 0.7 Co 0.3 O 3–δ oxygen electrode demonstrates excellent full-cell performance with high electrolysis current density of –1.48 A cm –2 at 1.3 V and a peak fuel-cell power density of 0.95 W cm –2 at 600 °C and also enables lower-temperature operations down to 350 °C, and superior long-term durability.
The High Flux Isotope Reactor (HFIR) is a versatile research reactor that provides one of the highest steady-state neutron fluxes of any reactor in the world. The HFIR reactor physics team investigated the conversion of the current 93 wt% highly enriched uranium U 3 O 8 -Al dispersion fuel to a 19.75% low-enriched uranium (LEU) U 3 Si 2 -Al dispersion fuel. The team continuously develops a Python module to streamline the analysis steps required for an LEU core design to ensure reproducible and agile design iteration. The Python module automates the data processing between analysis steps and automates the input perturbation for branch calculations and design changes. The automated framework has proven to significantly increase the efficiency and reproducibility of the reactor physics team to design High Flux Isotope Reactor (HFIR) LEU cores and thoroughly analyze performance metrics, safety metrics, and thermal safety margins. Consequently, the team can now respond rapidly to fuel fabrication engineer and thermal-hydraulic-structural analyst requests. Numerous combinations of LEU fuel designs are explored, of which two LEU fuel designs are presented here in this paper: a low density silicide design, and a high-density silicide design. Results show that both designs meet or exceed safety and performance metrics with exception for minor differences caused by the hardened spectrum from LEU.
Design of a multihundred-watt Dynamic Isotope Power System (DIPS) based on the U.S. Department of Energy (DOE) General Purpose Heat Source (GPHS) and small (multihundred-watt) free-piston Stirling engine (FPSE) technology is being pursued as a potential lower cost alternative to radioisotope thermoelectric generators (RTG's). The design is targeted at the power needs of future unmanned deep space and planetary surface exploration missions ranging from scientific probes to Space Exploration Initiative precursor missions. Power level for these missions is less than a kilowatt. Unlike previous DIPS designs which were based on turbomachinery conversion (e.g. Brayton), this small Stirling DIPS can be advantageously scaled down to multihundred-watt unit size while preserving size and mass competitiveness with RTG's. Preliminary characterization of units in the output power ranges 200-600 We indicate that on an electrical watt basis the GPHS/small Stirling DIPS will be roughly equivalent to an advanced RTG in size and mass but require less than a third of the isotope inventory.
A review and interlaboratory comparison of secondary ion mass spectrometry (SIMS) data obtained by laboratories participating in the International Technical Nuclear Forensics Working Group (ITWG) 7th Collaborative Material Exercise (CMX-7) has been conducted. The analyzed materials were two uranium compounds in powder form and two pieces of uranium metal. The instruments used in this comparison were a small-geometry (SG) SIMS, CAMECA IMS 7f from the Research Centre Rez, and a large-geometry (LG) SIMS, CAMECA IMS 1280 from Los Alamos National Laboratory. Despite the differences in instruments and analytical procedures, e.g., sample preparation, SIMS setups, and data post-processing, there was good agreement for the 234 U/ 238 U, 235 U/ 238 U, and 236 U/ 238 U ratios in the analyzed materials. The main difference was in the precision, which was, as expected, higher for the LG-SIMS. In addition, a comparison between the laboratories was also made for the image processing algorithms applied to raw data acquired in automated particle measurement (APM) mode. In conclusion, the result of this comparison has led to identification of best practices for setting up parameters of the APM software.
Determining the origin and history of interdicted nuclear materials is a central challenge in nuclear forensics. The oxygen stable isotope composition of uranium oxide compounds has emerged as a promising forensic signature, attracting increasing attention since the early 2000s. This review examines analytical techniques for measuring oxygen isotope compositions in uranium oxides and evaluates how the nuclear fuel production cycle introduces or modifies these isotopic signatures. The potential for forensic geolocation is explored through workflows that calibrate the relationship between environmental water oxygen isotopes and those found in uranium oxides. Key strengths and limitations of this approach are assessed, including gaps in knowledge related to isotope fractionation during specific stages of the fuel cycle, and processing facility water inputs. The importance of proper sample handling and storage under inert atmospheres, as well as a deeper understanding of both intra-sample oxygen isotope heterogeneity, and hydrous uranium oxide phase formation, is highlighted for improving the reliability of forensic interpretations. In conclusion, the development of uranium oxide standards with well-characterized δ 18 O values and international collaboration toward consensus on their use are identified as essential steps for advancing the field.
Neutron scattering and neutron imaging have emerged as powerful methods for experimentally investigating material deformation and fluid flow in the interior of otherwise inaccessible or opaque structures. This paper describes the design and provides example uses of a pressure cell developed for investigating such behaviors within geological materials. The cell can accommodate cylindrical samples with diameters up to 38.1 mm and lengths up to 154 mm. Additionally, ports in the cell and a pressure isolating sleeve around the sample allow the independent application of confining pressure up to 69 MPa and axial pressure up to 34.5 MPa. Furthermore, two material versions of the cell have been manufactured and used to date. An aluminum version is typically used for temperatures below 40 °C, because of its relative transparency to neutrons, while a titanium version, which is comparatively more neutron attenuating, is used for experiments requiring triaxial pressurization under conditions up to 350 °C. The pressure cells were commissioned at the VULCAN engineering diffractometer at the Oak Ridge National Laboratory (ORNL), Spallation Neutron Source, and have since been used at the ORNL high flux isotope reactor CG1-D imaging beamline, National Institute of Standard and Technology (NIST) BT-2, and NIST NG6 imaging beamlines.
Annual report of the Johnson Space Center Director's Discretionary Fund documenting effective use of resources. The $1,694,000 funding for FY92 was distributed among 27 projects. The projects are an overall aid to the NASA mission, as well as providing development opportunities for the science and engineering staff with eventual spinoff to commercial uses. Projects described include space-based medical research such as the use of stable isotopes of deuterium and oxygen to measure crew energy use and techniques for noninvasive motion sickness medication. Recycling essentials for space crew support is conducted in the Regenerative Life Support and the Hybrid Regenerative Water Recovery test beds. Two-phase fluid flow simulated under low-gravity conditions, hypervelocity particle impact on open mesh bumpers, and microcalorimetry to measure the long-term hydrazine/material compatibility were investigated. A patent application was made on a shape-memory-alloy release nut. Computer estimate of crew accommodations for advanced concepts was demonstrated. Training techniques were evaluated using multimedia and virtual environment. Upgrades of an electronic still camera provide high resolution images from orbit are presented.
Semiconductors are the backbone of modern technology, garnering decades of investment in high-quality materials and devices. Electron spin systems in semiconductors, including atomic defects and quantum dots, have been demonstrated in the last two decades to host quantum coherent spin qubits, often with coherent spin–photon interfaces and proximal nuclear spins. These systems are at the center of developing quantum technology. However, new material challenges arise when considering the isotopic composition of host and qubit systems. The isotopic composition governs the nature and concentration of nuclear spins, which naturally occur in leading host materials. These spins generate magnetic noise—detrimental to qubit coherence—but also show promise as local quantum memories and processors, necessitating careful engineering dependent on the targeted application. Reviewing recent experimental and theoretical progress toward understanding local nuclear spin environments in semiconductors, we show this aspect of material engineering as critical to quantum information technology.
The design of a multihundred-watt Dynamic Isotope Power System (DIPS), based on the U.S. Department of Energy (DOE) General Purpose Heat Source (GPHS) and small (multihundred-watt) free-piston Stirling engine (FPSE), is being pursued as a potential lower cost alternative to radioisotope thermoelectric generators (RTG's). The design is targeted at the power needs of future unmanned deep space and planetary surface exploration missions ranging from scientific probes to Space Exploration Initiative precursor missions. Power level for these missions is less than a kilowatt. The incentive for any dynamic system is that it can save fuel and reduce costs and radiological hazard. Unlike DIPS based on turbomachinery conversion (e.g. Brayton), this small Stirling DIPS can be advantageously scaled to multihundred-watt unit size while preserving size and mass competitiveness with RTG's. Stirling conversion extends the competitive range for dynamic systems down to a few hundred watts--a power level not previously considered for dynamic systems. The challenge for Stirling conversion will be to demonstrate reliability and life similar to RTG experience. Since the competitive potential of FPSE as an isotope converter was first identified, work has focused on feasibility of directly integrating GPHS with the Stirling heater head. Thermal modeling of various radiatively coupled heat source/heater head geometries has been performed using data furnished by the developers of FPSE and GPHS. The analysis indicates that, for the 1050 K heater head configurations considered, GPHS fuel clad temperatures remain within acceptable operating limits. Based on these results, preliminary characterizations of multihundred-watt units have been established.
R&D efforts in support of the Oak Ridge National Laboratory (ORNL) Isotope Program Radioisotope Portfolio are led by the Radioisotope Science and Technology Division (RSTD). In addition to supporting the ORNL Isotope Program Radioisotope Portfolio, RSTD supports a portfolio of research related to fundamental properties of radioisotopes and radioisotope applications, including diagnostic and therapeutic uses of medical radioisotopes, radioisotopes for national security, and the production of 238 Pu for the National Aeronautics and Space Administration (NASA) and US Department of Energy (DOE) Office of Nuclear Energy. RSTD is organized into functional science and engineering groups, with most staff members supporting multiple programs. The goal of this organization is to enable synergy between programs such that R&D advances coming from other programs may provide benefit to the ORNL Isotope Program. R&D within RSTD is focused around addressing five grand challenges, as documented in the strategic plan for the DOE Office of Isotope R&D and Production, or DOE Isotope Program (IP), Radioisotope Production R&D activities at ORNL: 1. Maximizing the scientific output of radioisotope transmutation resources, 2. Maximizing the scientific output of radioisotope processing resources, 3. Minimizing waste and having optimal waste disposition, 4. Focusing on product quality and reliability, and 5. Expanding the use of beneficial isotopes. The ORNL Core R&D program, one of the primary R&D components within the ORNL Isotope Program Radioisotope Portfolio, ranges from benchtop to demonstration activities, with a focus on researching enhanced production techniques, developing emerging isotopes, and developing the talent pipeline for radioisotope science and technology. Projects within the Core R&D Program are led primarily by RSTD staff members. In supporting enhanced production techniques, the Core R&D program presents an opportunity to fund novel R&D that might not be tied to a specific radioisotope product but still presents a high potential for broad applicability in the longer term. In supporting the development of emerging isotopes, the Core R&D program develops high-priority isotopes that are not able to be fully supported through production funds.
Human activities have the potential to redistribute radium (Ra) in the marine environment in a manner that may necessitate monitoring or management of subsequent human or environmental exposures. There is therefore a need to identify accurate and accessible techniques for Ra measurement in high salinity samples and to describe the distribution of Ra in estuarine and marine environments, but most efforts in these areas have focused on low salinity matrices. In addition, rapid and reliable measurements are crucial for time-sensitive samples such as short-lived isotopes or emergency situations. The objective of this study is to describe the limits of detection, cost, and relative ease for measurement of Ra in both low and high salinity aqueous samples via three analytical methods: liquid scintillation counting (LSC), high purity germanium (HPGe) gamma spectrometry, and inductively coupled plasma mass spectrometry (ICP-MS). To contextualize these measurements for real-world scenarios, the partitioning of 226 Ra to substrates relevant to the marine environment was also characterized. Although HPGe detection with solid phase extraction had the lowest limit of detection for low salinity samples (0.27 Bq L −1 ), poor 226 Ra recovery for high salinity samples and high materials costs make this method prohibitive for many users. Limits of detection for high salinity samples were lower for LSC (1.28 Bq L −1 ) than for ICP-MS without dilution (11.4 Bq L −1 ), but significant and unexpected degradation of the high salinity LSC standards was observed after six months. Furthermore, our preferred measurement method for high salinity Ra samples is ICP-MS with sample dilution as necessary to reduce matrix effects.
Mathematical relations prescribing unidirectional forward and reverse rates originally derived based on single-path reaction sequences do not apply to interconnected reaction networks. The presence of branches in reaction networks, leading to alternative stable products, decreases unidirectional rates in reference to those calculated by single-path functional forms, as shown by simulated isotopic exchange rates, but impacts the unidirectional forward and reverse rates equally such that the functional form of effective reversibility remains unchanged. Regardless of stoichiometric numbers and network connectivity, the application of the pseudo-steady-state hypothesis on reactive intermediates in conjunction with consideration of unidirectional rates toward the product of interest and all alternative stable products results in mathematical expressions that accurately reflect simulated isotopic exchange rates. Further analyses based on kinetic resistance, a property akin to electrical resistance, illustrate the manifestation of nodal resistances in addition to the single-path kinetic resistance for interconnected reaction networks. The generalized formalism for assessing rates and reversibilities in interconnected networks derived herein enables us to demonstrate that unidirectional rates cannot be assessed solely from effective reversibilities and net rates of generation of stable species in such networks. Furthermore, isotopic exchange rates, under the condition that each elementary step in the overall reaction sequence forms a unique reactive intermediate that is consumed solely by the subsequent step, can be utilized to determine unidirectional rates and can serve to validate postulated reaction pathways in highly interconnected reaction networks (e.g., CO x hydrogenation).
Eighteen cobalt targets (C003, C001, C005, C022, C021, C020, C032, C033, C038, C035, C036, C039, C053, C054, C055, C065, C066, & C067) were assayed on July 28-29, 2020, following irradiation in ATR cycle 168A. The average specific activity of each target was determined by using the cobalt assay system located in the ATR canal following procedure ACMM-3610.
The H-Canyon facility is currently dissolving spent nuclear fuel, including Material Test Reactor (MTR) and High Flux Isotope Reactor (HFIR) fuel. Dissolution of aluminum spent nuclear fuel produces hydrogen and other NOx gases. A theory long held by H-Canyon Engineering and Facility Technical Advisors that the silver nitrate-coated berl saddles, present in the iodine reactor, used for off-gas treatment were acting as a catalytic hydrogen recombiner was captured during an external review of the Accelerated Basin Deinventory program. Results from a separate SRNL project using a Raman Spectrometer to monitor the offgas from the dissolution process indicated a lack of the expected hydrogen in the off-gas stream. To test this hypothesis, a laboratory scale iodine reactor was assembled and filled with silver nitrate-coated berl saddles. Testing with this laboratory scale reactor confirmed the recombination of hydrogen when a simulated dissolver off-gas was passed through the reactor containing silver nitrate-coated berl saddles at 173-188 °C. Control experiments performed with uncoated berl saddles resulted in no change to the hydrogen concentration after passing through the reactor. The residence time of the gas in the reactor was varied to determine if residence time had an impact on the amount of hydrogen recombination occurring. Results from these experiments indicated that at the shortest residence times tested (~5 seconds) recombination of the hydrogen still exceeded 90%; however, the percent recombination did increase at longer residence times, reaching 97.9% or greater for residence times over 10 seconds. Finally, testing performed with a simplified off-gas composition containing only hydrogen and air gave similar results, indicating that the presence of NO and N 2 O gases in the stream do not play a role in the recombination reaction.
Cyanobacteria are emerging as hosts for photoautotrophic production of chemicals. Recent studies have attempted to stretch the limits of photosynthetic production, typically focusing on one product at a time, possibly to minimise the additional burden of product separation. Here, we explore the simultaneous production of two products that can be easily separated: ethylene, a gaseous product, and succinate, an organic acid that accumulates in the culture medium. This was achieved by expressing a single copy of the ethylene forming enzyme (efe) under the control of P cpcB , the inducer-free super-strong promoter of phycocyanin β subunit. We chose the recently reported, fast-growing and robust cyanobacterium, Synechococcus elongatus PCC 11801, as the host strain. A stable recombinant strain was constructed using CRISPR-Cpf1 in a first report of markerless genome editing of this cyanobacterium. Under photoautotrophic conditions, the recombinant strain shows specific productivities of 338.26 and 1044.18 μmole/g dry cell weight/h for ethylene and succinate, respectively. These results compare favourably with the reported productivities for individual products in cyanobacteria that are highly engineered. Metabolome profiling and 13 C labelling studies indicate carbon flux redistribution and suggest avenues for further improvement. Our results show that S. elongatus PCC 11801 is a promising candidate for metabolic engineering.