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At least 235 records · Page 13

Impact of Radiolysis on Iodine Speciation in a Variety of Matrices

This report details the work conducted in fiscal year 2023 with the aim of providing a better understanding of the speciation of iodine in support of domestic 99 Mo production Shine who uses a sulfate matrix in their process. Laboratory experiments to study the behavior of iodine speciation were conducted using spectroscopic methods including UV-vis and Raman as well as electrochemical studies. Radiolysis occurring in solution presents a unique challenge that is largely unaddressed with thermodynamic modeling, therefore a kinetic model was developed to address these issues. The focus of the studies conducted this year used surrogate radiolytic conditions induced by hydrogen peroxide for comparison to radiolytic conditions from direct gamma irradiation and neat acid solutions. For each case a model incorporating the kinetics was used to predict iodine speciation in the defined conditions where the output was directly compared to the experimental conditions. Further modeling was conducted incorporating the process conditions that are specific to Shine with incorporation of radiolysis and gas sparging.

07 ISOTOPE AND RADIATION SOURCES↗

The Institute for Nuclear Science to Inspire the next Generation of a Highly Trained workforce (INSIGHT) at FRIB

The proposed INSIGHT Center at FRIB has two objectives: (1) provide a center to support and coordinate a nationwide traineeship effort; and (2) offer traineeships at FRIB by leveraging its scientific opportunities. This will provide an environment to: (i) recruit and retain undergraduate students in (nuclear) physics and sustain and/or increase their interest, confidence, and enthusiasm in this field; (ii) provide participants with a toolset to become effective independent researchers who pursue further research opportunities as undergraduates; and (iii) encourage participants to pursue graduate studies and potential careers in nuclear science, or related STEM fields.

07 ISOTOPE AND RADIATION SOURCES↗

Liquid centrifugation-based isotope separation of 7 Li, 37 Cl and D

Liquid centrifugation is an emerging method to separate isotopes. By spinning a liquid containing target isotopes (e.g., pure chemical or solution), the heavier isotope will be enriched at the outer part of a centrifuge, and the lighter ones will be enriched at the inner part of a centrifuge. The separation capability is positively correlated with rotation speed, outer radius and mass difference between isotopes to separate. This award targets to understand whether liquid centrifugation is effective in separating isotopes important for nuclear fission technologies. The results include the following three sections: 1) Effects of solute concentration on isotope separation; 2) Preliminary progress of building a low-speed countercurrent centrifuge, and 3) Analysis on possible candidates for 7 Li and 37 Cl. The award trained one research scientist, one Ph.D. student, one master student, and one undergraduate on liquid centrifugation and isotope measurements.

07 ISOTOPE AND RADIATION SOURCES↗

Method for producing thorium-226

Disclosed herein are embodiments of a method for producing thorium-226. The method comprises separating thorium-226 from uranium-230 to produce a solution of thorium-226 in a solvent, such as a chelating buffer, suitable for direct labeling by a chelate. The thorium-226 may be separated from the uranium-230 using extraction chromatography. The extraction may be repeated multiple times as additional thorium-226 is produced by uranium-230 decay.

07 ISOTOPE AND RADIATION SOURCES↗

Recovery of Neptunium-236g from Photon and Proton-Irradiated Actinide Targets

Neptunium-236g is a rare radionuclide used as a tracer for neptunium-237 analyses. The availability of 236gNp is limited and the viable production routes are costly, time consuming, and only produce trace quantities of the desired product. For this work, two known production methods were tested to determine product recovery, purity, and viability for use as a tracer. The first method utilizes a photon-irradiated 237Np target to produce 236gNp by the 237Np(?,n)?236Np reaction. The second method utilizes the 238U(d,4n) ?236Np reaction. These production routes were evaluated previously, and the former was considered ineffective without isotope separation and the latter was not well-characterized for the 236mNp/236gNp production ratio. Recent resurgence of electromagnetic isotope separation technology has enabled at least partial recovery of 236gNp from part-per-million abundance feeds produced by the photonuclear reaction. To address the lack of production data for the second method, a deuteron-irradiated depleted uranium target was chemically processed to recover and purify the Np for abundance and ratio analyses. The status and current analytical results for each production method are presented.

07 ISOTOPE AND RADIATION SOURCES↗

OpenSn: A massively parallel, open-source simulation environment for discrete ordinates radiation transport

OpenSn is an open-source, massively parallel deterministic radiation transport code for solving the discrete-ordinates ( S N ) form of the Boltzmann transport equation on unstructured, arbitrary polyhedral meshes. It supports high-fidelity simulations involving steady-state, eigenvalue, and adjoint problems for neutral particles (e.g., neutrons, photons, multi-particles), using the multigroup approximation in energy. OpenSn combines angular discretization via discrete ordinates with a discontinuous Galerkin finite element method (DGFEM) in space, enabling accurate resolution of transport physics on arbitrary polyhedral cells, included locally refined spatial grids. It includes multiple angular quadrature types, including locally refined angular quadratures. Written in modern C++ with a Python API, OpenSn runs efficiently on platforms ranging from laptops to supercomputers. The transport sweep algorithm is implemented using a task-based, directed-acyclic-graph (DAG) approach for each angle and supports asynchronous parallelism across thousands of MPI ranks. Group-set aggregation improves compute intensity, and synthetic acceleration techniques (e.g., diffusion synthetic acceleration, second-moment method) enhance solver convergence. OpenSn has been verified on reactor physics problems and demonstrated excellent weak and strong scaling performance on more than 32,768 processes, making it a versatile and robust platform for large-scale transport simulations in complex geometries.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Production of NBL PO plutonium isotopic standards CRM 136A, CRM 137A, and CRM 138A

Lawrence Livermore National Laboratory (LLNL) produced approximately 1 mg units of purified Pu from the parent New Brunswick Laboratory (NBL) certified reference materials (CRM) 137, 136 and 138 isotopic standards for the NBL Program Office (NBL PO) as detailed in the revised project plan. As stated in the plan, three representative units of each material were dispensed at the same time to be characterized at LLNL and provide informational values for the quantity of Pu and progeny nuclides in each unit. NBL PO intends to collect and evaluate isotopic measurement data from multiple laboratories and certify these materials as new isotopic standards C137A, C136A, and C138A, respectively. Soon after production eleven units of each analytical standard were shipped to other analytical laboratories for the certification effort, and 121, 119, and 119 units of C137A, C136A and C138A, respectively were shipped to Mickey Finch at Y12 NBL distribution center in November 2024 (30-gallon drum, TID 003777 PRL 7000005043). Residual purified Pu from the effort is being stored indefinitely in B332 at LLNL. Detailed methods can be found in the production plan, and this report describes and documents aspects of the production effort that are not in or were modified from the original production plan.

and nuclear chemistry↗

Point Source Likelihood Framework (psl) v1.0

PSL is a software framework for localizing radiation point sources in a 3D environment using a freely moving radiation detector system. The framework assumes a single point source of radiation is in the environment and uses known detector positions and orientations along with their radiation measurements to find the most likely location of the point source. This approach to the problem enables analyses that improve upon the capability of a standard Maximum Likelihood Expectation Maximization (MLEM) approach, such as setting a source detection threshold, finding a likelihood interval for the position of the source, finding a likelihood interval for the activity (intensity) of the source, determining whether more than one point source may be present, and generating a map of Minimum Detectable Activity (MDA) for a given source type. Applications include radiological and nuclear security, consequence management, decontamination and decommissioning of nuclear facilities, and radiological emergency response.

Joshi, Tenzing↗

In situ deformation of antigorite-olivine two-phase mixtures: Implications for dynamics and seismic anisotropy in the mantle wedge

Water released from hydrous minerals in subducting slabs reacts with the overlying plate, resulting in widespread serpentinization in the mantle wedge. Deformation of serpentinized peridotites has been invoked to explain forearc seismic anisotropy, yet studies of the mechanical properties and deformation behaviors of serpentine-bearing multiphase aggregates remain limited. Here we deformed olivine-antigorite mixtures containing 70, 50, and 20 vol.% of antigorite at 2.5 – 7.6 GPa, 673 K and strain rates of ∼10 –5 –10 –4 s –1 . Elasto-viscoplastic self-consistent simulations, constrained by synchrotron X-ray diffraction (XRD) data, were used to estimate lattice strain, stress–strain partitioning, crystallographic preferred orientations (CPO) development, and aggregate strength. Selected run products were also analyzed by electron backscatter diffraction for comparison with the CPO results obtained from XRD experiments. We found olivine transitions from A- or B-type to C-type when antigorite fraction drops to 20 vol.%, coinciding with a microstructural change from interconnected weak layers to a load-bearing framework (LBF). An additional run on a sample Atg50/Ol50 with preexisting microstructures suggested the formation of LBF was promoted by these microstructures, although the preexisting antigorite CPO has been overprinted at 20.8 % strain and could be erased completely by subsequent deformation in nature. Estimated viscosity of the two-phase mixtures suggests that low-degree serpentinization (≤20 %) in the mantle wedge may increase the strength of olivine-rich peridotite and hinder slab-mantle decoupling, whereas high-degree serpentinization (≥50–70 %) weakens the peridotite and favors decoupling if sufficient viscosity contrast (>10) develops. Seismic anisotropy shows a nonlinear dependence on antigorite fraction: antigorite CPO governs the anisotropy of the mixtures with ≥50 vol.% antigorite, whereas olivine CPO dominates at low fractions (∼20 vol.%). The presence of pre-existing microstructures reduces seismic anisotropy of the deformed mixtures, however the persistence of pre-existing CPO in actively subducting slabs remains uncertain, making their significance over geological timescales questionable.

Crystallographic preferred orientation↗

Connectivity-Dependent Exciton–Phonon Coupling in Cesium Bismuth Halide Quantum Dots

Metal halide octahedra form the fundamental functional building blocks of metal halide perovskites, dictating their structures, optical properties, electronic structures, and dynamics. Here, in this study, we show that the connectivity of bismuth halide octahedra in Cs 3 Bi 2 Br 9 and Cs 3 Bi 2 I 9 quantum dots (QDs) changes with different halide elements. We use first-principles calculations to reveal the key role of the connectivity of bismuth halide octahedra on the wave function symmetry, Huang-Rhys factor, and exciton-phonon interaction strength. Following QD synthesis via a ligand-mediated transport method, the effect of connectivity is verified with transient absorption spectroscopy, where we contrast Cs 3 Bi 2 Br 9 and Cs 3 Bi 2 I 9 QD exciton dynamics. In photoexcited Cs 3 Bi 2 I 9 QDs, phonons related to the vibrational motions of face-sharing [BiI 6 ] 3- bioctahedra couple strongly to the electronic state and drive rapid carrier relaxation. Equivalent signals are not observed for photoexcited Cs 3 Bi 2 Br 9 QDs, implying a lack of phonon involvement in band-edge absorption and subsequent exciton relaxation. Our findings suggest that structural engineering can effectively tune the exciton-phonon coupling and therefore influence exciton relaxation and recombination in perovskite nanomaterials.

TDDFT↗

Radiation Simulation using Wi-Fi Signal Strength and Frequency

For routine radiological operations, lost radioactive sources, decommissioning and cleanup of nuclear facilities, and radiological terrorist events such as Radioactive Dispersive Devices (RDDs) or Radiological Exposure Devices (REDs), individuals are tasked with accurately locating both point and distributed sources of radiation. Radiation workers must often practice these tasks, whether part of initial training or periodically as part of formal or informal exercises or drills. In such circumstances, it is desirable to have an accurate recreation of a radioactive source, including a method of detecting it, which does not include dangerous amounts of radiation. The goal of this research was to develop a radiation simulation technology that uses IEEE 802.11x W-LAN protocol, i.e. Wi-Fi sources and detectors for these, as an inexpensive, precise and accurate method of replicating sources of gamma radiation. For this work, existing 802.11x sources were used. Software was developed for use with an Android smartphone to detect the presence of these sources. The measurements followed the expected behavior as a function of distance from the sources, mimicking that of gamma radiation, thus demonstrating the fundamental principle of operation. The ultimate system will be used in an outreach program to interest students in the radiation protection field.

07 ISOTOPE AND RADIATION SOURCES↗

Idaho National Laboratory CY 2024 National Emission Standards for Hazardous Air Pollutants Analysis, Methodology, and Results for Radionuclides

This report documents the methodology and results for calculating the effective dose equivalent (EDE) to the maximally exposed individual (MEI) from atmospheric radionuclide emissions from Idaho National Laboratory (INL) sources in Calendar Year (CY) 2024. The calculations were performed in accordance with requirements in Code of Federal Regulations (CFR), Title 40, “Protection of the Environment,” Part 61, “National Emission Standards for Hazardous Air Pollutants (NESHAPs),” Subpart H, “National Emission Standards for Emissions of Radionuclides Other than Radon from Department of Energy Facilities” (40 CFR 61, Subpart H). UDFs were calculated using the computer model CAP88-PC for unit (1 Ci/yr) emission rates at INL Site facilities and INL in-town (Idaho Falls) facilities and stored in Microsoft Access databases. The UDFs—in this case, mrem/Ci—were then combined with radionuclide-specific release (emission) rates for each facility-specific source to compute doses at predetermined public receptor locations, including the MEI locations. This report contains the dose results and a description of the methodology and tools used to compute the doses.

07 - ISOTOPES AND RADIATION SOURCES↗

A transcriptome software comparison for the analyses of treatments expected to give subtle gene expression responses

Background: In this comparative study we evaluate the performance of four software tools: DNAstar-D (DESeq2), DNAstar-E (edgeR), CLC Genomics and Partek Flow for identification of differentially expressed genes (DEGs) using a transcriptome of E. coli. The RNA-seq data are from the effect of below-background radiation 5.5 nGy total dose (0.2nGy/hr) on E. coli grown shielded from natural radiation 655 m below ground in a pre-World War II steel vault. The gene expression response to three supplemented sources of radiation designed to mimic natural background, 1952 – 5720 nGy in total dose (71–208 nGy/hr), are compared to this “radiation-deprived” treatment. In addition, RNA-seq data of Caenorhabditis elegans nematode from similar radiation treatments was analyzed by three of the software packages. Results: In E. coli, the four software programs identified one of the supplementary sources of radiation (KCl) to evoke about 5 times more transcribed genes than the minus-radiation treatment (69–114 differentially expressed genes, DEGs), and so the rest of the analyses used this KCl vs “Minus” comparison. After imposing a 30-read minimum cutoff, one of the DNAStar options shared two of the three steps (mapping, normalization, and statistic) with Partek Flow (they both used median of ratios to normalize and the DESeq2 statistical package), and these two programs identified the highest number of DEGs in common with each other (53). In contrast, when the programs used different approaches in each of the three steps, between 31 and 40 DEGs were found in common. Regarding the extent of expression differences, three of the four programs gave high fold-change results (15–178 fold), but one (DNAstar’s DESeq2) resulted in more conservative fold-changes (1.5–3.5). In a parallel study comparing three qPCR commercial validation software programs, these programs also gave variable results as to which genes were significantly regulated. Similarly, the C. elegans analysis showed exaggerated fold-changes in CLC and DNAstar’s edgeR while DNAstar-D was more conservative. Conclusions: Regarding the extent of expression (fold-change), and considering the subtlety of the very low level radiation treatments, in E. coli three of the four programs gave what we consider exaggerated fold-change results (15 – 178 fold), but one (DNAstar’s DESeq2) gave more realistic fold-changes (1.5–3.5). When RT-qPCR validation comparisons to transcriptome results were carried out, they supported the more conservative DNAstar-D’s expression results. When another model organism’s (nematode) response to these radiation differences was similarly analyzed, DNAstar-D also resulted in the most conservative expression patterns. Therefore, we would propose DESeq2 (“DNAstar-D”) as an appropriate software tool for differential gene expression studies for treatments expected to give subtle transcriptome responses.

59 BASIC BIOLOGICAL SCIENCES↗

Gamma-radiation-induced negative nonlinear absorption in quartz glass

The effect of ionizing radiation on the nonlinear optical properties of materials needs to be considered for applications that employ high-power laser pulses in extreme radiation environments. The Heraeus Infrasil302 optical quartz glass was irradiated by gamma rays, and its nonlinear absorption was measured using the open-aperture Z-scan technique with nanosecond laser pulses. Irradiation results in a negative nonlinear absorption coefficient whose magnitude increases with irradiation dose. Nonlinear absorption coefficients of -0.78, -1.14, -1.29, and -1.88~ × ~10 -13 m/W are measured for gamma doses of 600 krad, 1.2 Mrad, 3.6 Mrad, and 10 Mrad, respectively. Thermal annealing restores the optical properties of quartz-glass to their unirradiated values. It is suggested that metallic impurities introduced by the manufacturing process have a role in inducing saturated absorption in irradiated quartz glass, which manifests as negative nonlinear absorption coefficient, and is demonstrated by comparing Infrasil302 quartz results to equivalent irradiated measurements for Spectrosil2000 quartz.

07 ISOTOPE AND RADIATION SOURCES↗