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At least 487 records · Page 27

An improved method for uranium separation from urine for rapid bioassay by inductively coupled plasma mass spectrometry

Bioassay monitoring is an important capability for any facility that works with significant amounts of radioactive material. The speed at which these analyses can be made is critical in the event of a potential exposure. Here, we present a new method that facilitates the rapid separation of uranium from a urine matrix for assay and isotopic determination by inductively coupled plasma mass spectrometry. This method is validated with archived urine samples that were previously analyzed using established, more time consuming methods. The sources of uncertainty for uranium assay and isotopic measurements are modelled using the Monte Carlo method to better understand the precision and accuracy of this method at the limit of quantification.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Isotope-selective radiography and material assay using high-brilliance, quasi-monochromatic, high-energy photons

We demonstrate the possibility to directly detect microgram amounts of the isotope 7 Li using a quasi-monochromatic high-energy photon beam. The isotope selective detection is based on a witness scatterer absorbing and re-emitting photons via nuclear resonance fluorescence. This enables the detection of isotopes with microgram accuracy at long distances from the actual sample. Further, we demonstrate that the technique can deliver quantitative information without specific knowledge of the photon flux and no spectral capabilities or knowledge of the resonance fluorescence cross section. Detection of low-atomic-weight isotopes screened by heavy shielding is also shown. The techniques described are applicable to all next-generation, ultrahigh brilliance, laser-Compton light sources currently under construction.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Optimization of ray-tracing simulations to confirm performance of the GP-SANS instrument at the High-Flux Isotope Reactor

The CG-2 beamline at the High Flux Isotope Reactor (HFIR) exhibits a notable discrepancy between observed count rates and the count rates we would expect based on a Monte-Carlo neutron ray-trace simulation. These simulations consistently predict count rates approximately five times greater than those observed in four separate experimental runs involving different instrument configurations. This discrepancy suggests that certain factors are causing losses in measurements that are not adequately accounted for in the simulation, in particular guide reflectivity or misalignment. To investigate these discrepancies, a high-dimensional simulation parameter approach is applied in order to understand the losses. Region of Interest (ROI) groups along the instrument are assigned to different surfaces of the guide components within the simulation. This allows the parameters of those guide components to be varied as a group to minimize the complexity of the search space. The result is an optimization of simulation parameters using an iterative scheme that aims to minimize the difference between experimentally measured count rates and simulated count rates across all tested collimator combinations. This proposed methodology holds the potential to reveal previously unrecognized sources of intensity loss in the CG-2 beamline at HFIR and improve the accuracy of simulations, leading to enhanced understanding and performance of the beamline for various scientific applications.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Modeling of fission and activation products in molten salt reactors and their potential impact on the radionuclide monitoring stations of the International Monitoring System

Molten Salt Reactors (MSRs) are one of six Generation IV reactor designs currently under development around the world. Because of the unique operating conditions of MSRs, which include molten fuel and the continuous removal of gaseous fission products during operation, work was performed to analyze the potential impact of emissions on the International Monitoring System (IMS) of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). Simulations were performed to predict the production of IMS-relevant radionuclides in four MSR designs operating under two scenarios – (1) a sealed reactor with releases only during operational shutdown and (2) continuous reprocessing or sparging of the fuel salt. From these production estimates the radioxenon and radioiodine signatures were extracted and compared to three current reactor designs (PWR, BWR, RBMK). In the cases where continuous reprocessing of the fuel salt occurred both the radioxenon and radioiodine signatures are nearly indistinguishable from a nuclear explosion. Estimates were also made of the potential emission rate of radioxenon for three reactor designs and it was found that MSRs have the potential to emit radioxenon isotopes at a rate of 1015 – 8×1016 Bq/d for 133Xe if no abatement is used. An assessment was also made of activation products using a candidate fuel salt (FLiBe) mixed with corrosion products for the Thorium Molten Salt Reactor (TMSR-LF1)

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Trace Actinide Signatures of a Bulk Neptunium Sample

In nuclear forensic analyses, measurements of actinide elements in a sample can assist with identifying interdicted or unknown materials. While these radiochemical signatures have been extensively investigated in uranium materials, less is known about bulk neptunium samples. This paper describes the measurement of trace actinide concentrations and isotopic profiles in a 237 Np oxide sample. Uranium, plutonium, americium, and curium concentrations and isotopic profiles in the sample were determined and deemed potentially useful for distinguishing different sources of 237 Np. Furthermore, several different potential radiochronometry systems were also investigated; discordant results indicate that the Np sample was never completely purified of other actinide elements, or that subsequent contamination of the sample occurred. Few prior studies of neptunium materials have been reported, and these data suggest that trace actinide constituents could provide unique signatures to identify material out of regulatory control.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Laboratory for Laser Energetics Targets Inertial Confinement Fusion

The University of Rochester’s Laboratory for Laser Energetics is targeting laser-driven inertial confinement fusion, as part of National Nuclear Security Administration’s Stockpile Stewardship Program and in the quest for clean sources of energy. The Laboratory for Laser Energetics (LLE) is home to two extremely powerful lasers—OMEGA and OMEGA EP—and researchers are using them to explore laser-driven inertial confinement fusion (ICF). ICF involves compressing a small amount of fuel consisting of hydrogen isotopes, deuterium (D), and tritium (T), and heating it to temperatures greater than the center of stars. “When these conditions are reached, the fuel undergoes fusion—releasing enormous energy that can be used for research relevant to the National Nuclear Security Administration’s (NNSA) Stockpile Stewardship Program (SSP) and to drive carbon-free power plants,” explains Valeri Goncharov, distinguished scientist and director of the Theory Division at LLE. LLE was established at the University of Rochester in 1970 and is the largest U.S. Department of Energy university-based research program in the nation, supported by the National Nuclear Security Administration as part of its Stockpile Stewardship Program (SSP). “As a center for exploring the interaction of intense radiation with matter, LLE is a unique national resource for research and education in science and technology,” says Goncharov. “Our current research includes exploring fusion for the SSP program and as a future source of energy, developing new laser and materials technologies, and pursuing a better understanding of high-energy-density phenomena.”

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

GADRAS-DRF Validation for Safeguards and Custom Peak Fit Enhancements

In previous years, SGTech funded enhancements to the isotopics routine in the software called Gamma Detector Response and Analysis Software-Detector Response Function (GADRAS-DRF), including the addition of peak fit customization capabilities. A project was also funded that focused on implementing a peak-based model fitting routine, allowing model fitting to be performed without dependence on export-controlled cross-sections. In FY25 significant improvements were made to the custom peak fitting interface, accompanied by several validation studies within GADRAS-DRF. These studies encompassed IsotopeID performance, distributed source analysis, isotopics validation, and activity estimation. Additionally, the peak-only model fitting option was validated using an HPGe measurement of a rotating drum with line sources.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Constraining Inputs to Realistic Kilonova Simulations through Comparison to Observed r -process Abundances

Kilonovae, one source of electromagnetic emission associated with neutron star mergers, are powered by the decay of radioactive isotopes in the neutron-rich merger ejecta. Models for kilonova emission consistent with the electromagnetic counterpart to GW170817 predict characteristic abundance patterns, determined by the relative balance of different types of material in the outflow. Assuming that the observed source is prototypical, this inferred abundance pattern in turn must match r -process abundances deduced by other means, such as what is observed in the solar system. We report on analysis comparing the input mass-weighted elemental compositions adopted in our radiative transfer simulations to the mass fractions of elements in the Sun, as a practical prototype for the potentially universal abundance signature from neutron star mergers. We characterize the extent to which our parameter inference results depend on our assumed composition for the dynamical and wind ejecta and examine how the new results compare to previous work. We find that a dynamical ejecta composition calculated using the FRDM2012 nuclear mass and FRLDM fission models with extremely neutron-rich ejecta ($Y_e$ = 0.035) along with moderately neutron-rich ($Y_e$ = 0.27) wind ejecta composition yields a wind-to-dynamical mass ratio of $M_w$/$M_d$ = 0.47, which best matches the observed AT2017gfo kilonova light curves while also producing the bestmatching abundance of neutron capture elements in the solar system, though, allowing for systematics, the ratio may be as high as of order unity.

79 ASTRONOMY AND ASTROPHYSICS↗

A Tool Kit for Generating Simulated Radiation Measurements for Advanced Reactor Safeguards and Security

A tool kit was developed to simulate and analyze passive radiation measurements of molten salt reactor (MSR) operations to support development of nuclear safeguards approaches for this emerging reactor technology. A Transient Simulation Framework of Reconfigurable Modules (TRANSFORM) multiphysics simulation of an MSR produces time-dependent isotopic inventories at user-selected locations within the model. The tool kit implements the Gamma Detector Response and Analysis Software (GADRAS) application programming interface to inject the TRANSFORM isotopic inventories extracted/processed by a Python pipeline into GADRAS models of user-defined geometries. The TRANSFORM inventories are the source terms used to obtain synthetic measurements from GADRAS-defined detectors. The speed of TRANSFORM and GADRAS simulations enables surveying the large design space of MSRs (e.g., fuel type, fuel salt composition, number of loops) and the plethora of measurements (e.g., location, detector type, and collimation) within the reactor. This has enabled timely assessment of the various measurement locations and detectors to identify the most effective and efficient safeguards approach for a specific MSR design. Lastly, the tool kit also simulates extracted samples that can be aged to a desired dose, enabling stakeholders to optimize a measurement plan to use sample analysis as an element within a broader material accountancy plan.

Westphal, Greg↗

LLNL International Working Group on Gamma Spectrometry - Preparation of IDB Dataset

The spectral information and associated metadata, including source information, detector setup, and shielding configuration is described in human readable, comma-separated text files (csv). Five csv files are associated with each material type and include the following information (where [Isotope] is U, Pu, and MOX): [Isotope]_measurement_metadata - Metadata of the measurement configuration, including material composition at time of acquisition (decay corrected from certificate date). Data that is unique to a measurement configuration e.g. detector geometry, source-detector distance, analyzer and other electronics used, attenuating materials are provided in this file. [Isotope]_spectrum_metadata - The information that is unique to the spectrum. This includes detector specifications (e.g. date of acquisition, number of channels, gain (keV/channel), energy range, real and live time, full width half-maximum (FWHM) of the 186 or 208 peak for uranium or plutonium measurements, respectively. [Isotope]_source_metadata - The source material used for the measurement, this includes the ratio and uncertainties of isotopes present and processing information of the material. In addition, the certificate information for the source material is listed. [Isotope]_spectrum_counts_metadata - The counts per channel for each spectrum. This data is linked via the UID.spectrum index to the measurement_metadata file. [Isotope]_spectrum_checksum_metadata The MD5 checksum for the original spectrum file. This data is linked via the UID.spectrum index to the measurement_metadata file. This information is provided to prevent duplication of entries in the database.

42 ENGINEERING↗

SAIL-Isotopologue (SAIL-iso) Field Campaign Report

The SAIL-iso project took place from November 19, 2022 to June 3, 2023 as part of the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s Surface Atmosphere Integrated Field Laboratory (SAIL) project at the main project site in Gothic, Colorado. The project sought to use measurements of the stable isotopic composition of water vapor to better understand cloud-aerosol interactions in a remote mountainous watershed. Water vapor isotopologue and humidity measurements were determined using a Los Gatos Research Triple Water Vapor Isotope Analyzer (TWVIA). The instrument was deployed in the guest van and consists of three main components: a water vapor isotope analyzer, a Los Gatos Research Water Vapor Isotope Standard Source (WVISS), and a Los Gatos Research Dry Air Source. Ambient air samples were collected through an inlet located about one meter above roof of the shipping container. Samples were then delivered to the analyzer through Teflon tubing by use of an external pump to minimize the transport time between the inlet and analyzer. The inlet tubing was surrounded by a Briskheat heat trace and insulating material to ensure ambient air samples did not fall below the dew point and result in condensation. The analyzer uses cavity ringdown spectroscopy to report isotopic ratios of ambient air samples at a frequency of 1 Hz. The calibration unit of the instrument was used in conjunction with the dry air source to periodically measure the δ values of standard waters. It uses a nebulizer to push small water droplets into a hot chamber that vaporizes the water without fractionation. This vapor was then transported to the analyzer using a built-in compressor and the dry air source, which allows each standard with known δ values to be measured at a wide range of humidity values for post-measurement calibration of ambient air samples. Multiple sources of uncertainty are introduced at different stages during the data collection and processing. These include (1) instrument precision, (2) uncertainty in the secondary standards, (3) humidity-correction uncertainty, and (4) Vienna Standard Mean Ocean Water – Standard Light Antarctic Precipitation (VSMOW-SLAP) calibration uncertainty. Uncertainty from each step is propagated in quadrature to calculate a total uncertainty of each isotopologue. Uncertainty was determined to be 2.3‰ for δD and 0.4‰ for δ 18 O.

54 ENVIRONMENTAL SCIENCES↗

Chemical separation of 146 Sm for half-life determination

Here, although methods for the chemical separation of samarium from a rock matrix are well established, chemical separation of samarium from non-natural isotopic impurities for the purpose of 146 Sm half-life measurement requires modifications to these procedures, as well as additional checks for effective separation. This work describes the chemical purification procedures associated with the 146 Sm source and the results from gamma spectroscopy. The purification procedure allowed for the quantitative determination of the number of 146Sm atoms using a modified isotope dilution technique. Alpha-decay counting of the sample will be applied in the future to determine the half-life of 146 Sm.

146Sm↗

MCNP Intrinsic Source Constructor (MISC): A User’s Guide

The MCNP Intrinsic Source Constructor (MISC) facilitates the construction of MCNP source definition cards for radioactive materials. Given a material nuclide specification, either weight or atom fractions of those nuclides, and either a weight or atom density of the material, MISC will construct the source spectrum distribution of a specified particle type. MISC also calculates the absolute number of particles emitted per second per unit mass or volume. Furthermore, if decay chain information is available in the data sets selected by the user, the initial isotopes specified by the user can be approximately decayed to the resulting isotopes after a specified amount of time.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Photonuclear cross sections for the 197 Au ⁢(𝛾, 𝑝⁢𝑛)⁢ 195⁢𝑚 Pt reaction near threshold

Platinum radioisotopes are of growing interest for targeted cancer therapy and diagnostic imaging because their decay delivers highly localized radiation doses in tissue, herewith enabling precise DNA damage through Auger-electron emission. Developing production technologies that provide platinum isotopes with high specific activity is essential in radioisotope therapy. Photonuclear reactions on stable nuclei offer a viable accelerator-based route for isotope production when supported by reliable cross-section data. We report photonuclear cross-section measurements for the 197 Au(γ, pn) 195m Pt reaction at incident γ-ray energies of 27, 29, and 31 MeV using the activation method. The measurements were performed by irradiating a stack of concentric-ring gold targets with a quasi-monoenergetic γ-ray beam provided by the High Intensity Gamma-ray Source (HI γS). The induced 195m Pt activity was quantified using off-line γ-ray spectroscopy. These data provide the first experimental constraints on the 197 Au(γ, pn) 195m Pt cross section in the near-threshold region. Furthermore, the comparison of the measured excitation function to PHITS and TALYS calculations indicates that the reaction becomes measurable only near 30 MeV and that substantially higher bremsstrahlung end-point energies are required for practically meaningful production.

190 ≤ A ≤ 219↗

Simulating Alpha Particles Incident on MKID Chips for Quantum Sensitivity Analysis

Superconducting quantum devices, such as microwave kinetic inductance detectors (MKIDs), are highly sensitive instruments used in quantum computing and advanced sensing technologies. However, their extreme sensitivity also makes them vulnerable to background noise from natural sources like radiation. One significant contributor to this noise is alpha particles emitted by 210Po, a radon decay daughter that accumulates on surfaces near the detector. This project investigates how alpha particles emitted from 210Po interact with MKID chips. These particles can deposit energy on the detector surface, disrupting its operation and generating false signals. Understanding the energy and behavior of these particles is crucial for improving the design and reliability of quantum devices. To explore this, we first modeled the decay chain starting from 210Pb to 210Po using differential equations. This allowed us to predict how the activity of alpha-emitting isotopes changes over time, reaching a steady state after about two years. Next, we simulated alpha particle interactions with the MKID chip using the Geant4 software toolkit. We built a detailed computer model of the detector housing, including the copper lid where alpha particles originate, the silicon chip, and a thin aluminum sensor layer. Alpha particles were emitted isotropically from just beneath the copper lid’s surface, mimicking natural decay conditions. The simulation tracked how these particles deposit energy on the chip, generating electron-hole pairs and phonons. The results provide insight into the behavior of the resultant electron-hole pairs and phonons, giving us a clear understanding of the energy deposition distribution on the chip. This work supports efforts to mitigate background noise in superconducting sensors, advancing their use in quantum computing and sensitive physics experiments.

Hall, Matthew [Fermilab; UCLA]↗

Environmental evaluation of radioactivity levels and associated radiation hazards in groundwater around the WIPP site

Groundwater may contain radioactive substances which can be dangerous to human health. Concentrations of natural radionuclides polonium (Po), thorium (Th), uranium (U), and radium (Ra) isotopes were measured in groundwater samples collected from different locations in the vicinity of the Waste Isolation Pilot Plant (WIPP) site in Carlsbad, New Mexico. The average values of gross activity concentrations of 210 Po, 228 Th, 238 U, 234 U, 226 Ra and 228 Ra isotopes were determined to be 1.62 Bq L -1 in shallow groundwater and 5.88 Bq L -1 in deep groundwater, respectively. The total radioactivity in deep groundwater was higher than that in shallow groundwater, and most of the radioactivity in the water is from 226 Ra. Furthermore, the effective doses for ingestion of natural radionuclides were about 0.333 mSv y–1 for shallow groundwater and about 1.338 mSv y –1 for deep groundwater samples, which are higher than the World Health Organization (WHO, 2017) guideline level (0.1 mSv y –1 ) for drinking water. Ra dominated the total ingestion dose, contributing 93.06 % and 75.40 % of the total effective doses to the deep and shallow groundwater, respectively. The ingrowth and decay of natural radionuclides suggested that 228 Ra/ 226 Ra ratio can be a useful indicator of the source of radioactive contamination. The radioactivity data obtained from the investigated groundwater samples can be used to establish a baseline for radioactivity levels in groundwater around the WIPP site.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

Conceptual Designs for Irradiation Creep Testing of SiC in HFIR

Understanding irradiation creep of nuclear fuel cladding is important to properly size the initial fuel-cladding gap and understand when pellet-cladding contact is expected to occur due to a combination of fuel swelling and cladding creep-down. Irradiation creep also plays a role in relaxing stresses that develop in-pile. Silicon carbide fiber–reinforced silicon carbide matrix (SiC/SiC) composites are the leading long-term accident-tolerant fuel cladding concept for light-water reactors (LWRs). Although some limited data are available regarding irradiation creep of the individual constituents (fibers, matrix), data regarding irradiation creep of SiC/SiC composites are currently insufficient. Additional data regarding irradiation creep compliance and the rupture lifetime (combination of creep and slow crack growth) are needed to understand material limitations. This work describes the design and development of two irradiation vehicles that are being pursued for testing SiC/SiC concepts in the High Flux Isotope Reactor (HFIR). The first is a passive experiment, referred to as the PRECISE experiment, that leverages the constant coolant pressure of HFIR to compress a metallic bellows and provide a well-characterized load to drive creep in a SiC/SiC dog bone specimen. The total creep strain would be quantified post-irradiation by measuring dimensional changes of the specimen length as well as local dimensional changes within the gauge region. Non-stressed specimens would also be irradiated under the same conditions to provide an indication of dimensional changes due to radiation-induced swelling in the absence of creep. A second, more complex experiment, referred to as the INSITE experiment, is being designed in parallel that would use pneumatics to pressurize a metal bellows and linear variable differential transformers (LVDTs) to measure the specimen displacement in situ during irradiation. Such an experiment would provide significantly more data regarding the evolution of the creep compliance as a function of dose and applied stress within a single experiment but would require significantly more development time and cost to execute. The primary concern with the INSITE experiment is the accuracy, reliability, and expected lifetime of the LVDTs during irradiation at elevated temperatures. Efforts are being made to adjust the experiment design and operating procedure to limit LVDT temperatures and mitigate or otherwise compensate for uncertainties due to factors such as temperature fluctuations, creep in the surrounding structural materials, and drift of the LVDTs. This work describes the experiment designs, thermal and structural analysis that were performed to ensure that the desired temperature and stress conditions can be achieved, some initial sensitivity analyses to predict the evolution of the radiation-induced specimen displacements, and potential sources of uncertainty in the measurements. Out-of-pile testing is being performed in parallel to confirm that the test trains achieve the expected stress states in the specimens and do not result in prohibitive stress concentrators (e.g., in the grip regions) that might risk pre-mature failure. The PRECISE experiments are proceeding toward fabrication and assembly with HFIR insertion planned during fiscal year 2026. The INSITE experiment is progressing toward out-of-pile demonstrations, which will provide more conclusive evidence regarding the feasibility of executing these tests in HFIR or whether alternative displacement monitoring techniques may need to be considered.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Direct Measurements with Neutron Sources [Slides]

The majority of heavy elements are produced through neutron capture. This presentation discusses progress in measurements for the Weak s-Process, how measurements are done, and future capabilities for direct measurement at LANSCE. Conclusion: Major advances have been made in improving neutron capture rates for the weak s process in the last 15 years. Coupling these measurements to stellar simulations is key to understanding where the next opportunities lie. New capabilities for performing measurements, particularly on unstable isotopes are being developed around the world

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗