Results for “HfIr” — Page 14

DOE OSTI2023

The Recovery of Medical Isotope 188 W from Irradiated W Metal Target - A New Approach

Tungsten-188 is in widespread use in 188 W(t 1/2 = 69 d )/ 188 Re(t 1/2 = 16.9 h ) biomedical generators. Oak Ridge National Laboratory has been providing this product to the world since 1999. At ORNL, 188 W is produced via irradiation in ORNL’s High Flux Isotope Reactor (HFIR). Enriched 186 W targets in the form of sintered metallic pellets or rings achieve a compact loading in the irradiation vessel, providing a high yield per unit target. The enrichment of the target is >90% 186 W, and this isotope undergoes double neutron capture to produce the desired 188 W product. While 188 W is produced by neutron bombardment, 191 Os(t 1/2 = 15.4 d ) is simultaneously produced as a by-product and expected to be separated from 188 W by postirradiation treatment.In the current processing pathway, the irradiated W metal rings are first converted into an oxide form of WO 3 by heating the irradiated W metal target at 750°C in a quartz reaction vessel inside a vertical furnace under a constant flow of air. During heating, W metal reacts with oxygen in the air to produce WO 3 , which is soluble in 6 M NaOH for preparation of 188 W product. This oxidation process also converts 188 Os (the decay daughter of 188 W) and 191 Os (15.4 d , the irradiation produced byproduct) into OsO 4 , a highly volatile and toxic gas. The gaseous effluents driven from the quartz reaction vessel are passed through a scrubbing array to remove OsO 4 before the air is discharged from the process. This heterogeneous oxidation method simultaneously achieves goals of (1) converting metal target to a soluble oxide form and (2) removing volatile OsO 4 away from the solid WO 3 product by air flow and absorbing the harmful Os species by the scrubbing array. But this method has two potential problems as well: (1) O 2 reacts with only W metal at high temperatures, not with W alloyed with other elements. The O 2 –W reaction will be retarded when formation of WRe or WC occurs, or even when a layer of non-W materials on the surface of the irradiated W rings.; (2) 100% absorption of OsO 4 of high yield (>90%) from the reaction of Os + O 2 is a strict requirement to the OsO 4 scrubbing system--so NaOH scrubbers of a redundant size (2x 1.5 L) are in use for safety reasons.To resolve above two potential problems, direct dissolution of the irradiated W metal target by a selected reagent is a preferred pathway to avoid heating step with generation of tremendous amount of volatile OsO 4 . Hydrogen peroxide (H 2 O 2 ) is such a candidate to dissolve W in forms of either metal or alloys, although literature lacks information of solubilities of Re or Os in H 2 O 2 . With experimental results of dissolving non-radioactive W, Re and Os in H 2 O 2 under various conditions, this report illustrates a method of H 2 O 2 dissolution for irradiated W target, with a complete dissolution of W and Re, but ≤10% dissolution of Os (converted into gaseous OsO 4 and carried out into a scrubbing for absorption) during processing irradiated W target. The portion of undissolved Os can be separated from W solution by a follow up filtration step. Solubilities of W, Re and Os in H 2 O 2 at a temperature range from 14° to 50°C are presented. And a dissolution rate of W metal per surface area of W metal in H 2 O 2 is calculated based on results of dissolving a W metal cylinder of known surface area in H 2 O 2 at room temperature without stirring.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2021

Building Neutron Scattering Infrastructure in Louisiana for Advanced Materials (Final Report)

The main objective of the Louisiana Consortium for Neutron Scattering (LaCNS) is to build a major neutron scattering infrastructure capable of treating both soft and hard materials. The goal is to create a sustainable effort having the quality, breadth, and depth necessary to produce competitive proposals including collaborative and center type proposals. Our scientific aim is to understand the role of coupling in emergent complex materials and its impact on the structure/property relationship and to explore how to tune the key couplings to guide the design of materials with the desired properties. This naturally includes building a base of users of the Spallation Neutron Source (SNS) and the High Flux Isotope Reactor (HFIR) in Louisiana; to train highly talented graduate and post-doctoral students in synthesis, neutron scattering, and simulation and modeling techniques, thereby helping to produce the next generation of scientist who use neutron scattering techniques as a crucial part of their research. The goal of our hard matter program is to understand the interplay between spin, charge, orbital, and lattice degrees of freedom in carefully selected complex materials. We have made considerable progress on number of complex systems including the oxide Sr3(Ru1-xMnx)2O7 where short-range magnetic ordering with anisotropic spin texture is initiated at the metal-insulator transition that clearly indicates a strong spin-charge coupling. Another critical area is in quantum materials. For example, in the topological semimetal BaMnSb2, we found a 3D canted antiferromagnetic Weyl semimetal with a 2D electronic structure and a nontrivial Berry phase. In addition, in the hexagonal chiral Mn1/3NbS2 system, we found soliton/soliton and soliton/antisoliton domain walls where the application of small fields or small currents can be used to control nanoscopic magnetic domains where the control of domain walls is crucially important for information storage. In addition, chemical transformation investigations were performed on the VISION instrument at Spallation Neutron Source (SNS). The soft matter effort was focused on understanding the role of non-covalent interactions on the structure and dynamics of fluid-based soft matter. One key focus was on sequence-defined (SD) amphiphilic peptoid polymers that allow encoding of molecular interactions and thereby systematic investigations of how charge directs the solution self-assembly of amphiphilic polymers in water. Another important area was on the dynamics of lipids self-assembled into membranes for exploring the permeability and mechanical using both neutron spin echo (NSE) spectroscopy and quasielastic neutron scattering (QENS) to distinguished between viscoelasticity and permeability at the molecular scale. Overall, the LaCNS project was quite successful, generating 145 publications and 245 presentations. Our graduate and post-doctoral students were well trained resulting in positions in national laboratories (Oak Ridge National Laboratory (ORNL), Argonne National Laboratory and Los Alamos National Laboratory), major research universities, and industry. We also developed a uniaxial pressure cell along with ORNL for SNS. A critical goal of this project was to establish a foundation for competing nationally in federally funded research programs. To this end, we were quite successful in generating over twenty-two federally and non-federally funded grants including awards from NSF, DOE, and DOD, and two early career awards. Equally important, we were able to secure a key major piece of instrumentation via a large ARO grant for a state-of-the-art electron microscope.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Mechanical Properties of Additively Manufactured 316L Stainless Steel Before and After Neutron Irradiation–FY23

This report presents the observed mechanical behavior of the additively manufactured (AM) 316L stainless steel (SS) before and after neutron irradiation. In the Advanced Materials and Manufacturing Technologies (AMMT) program, a variety of mechanical and physical property data are generated and accumulated to assess the AM austenitic alloy for nuclear reactor applications. The testing and evaluation task in the FY 2023 focused on elucidating the effects of sampling location and build size on the mechanical properties of AM 316L SS (in stress-relieved condition) before and after neutron irradiation. The laser powder bed fusion (LPBF) process produced 316L plates of three distinct sizes from which SS-J3 miniature tensile specimens were machined from six different locations. The tensile specimens were irradiated in the High Flux Isotope Reactor (HFIR) normally to 2 and 10 dpa at the target temperatures of 300 °C and 600 °C. Post-irradiation tensile testing was performed at room temperature, 300 °C, and 600 °C. The mechanical properties of AM 316L SS were significantly influenced by the characteristic microstructures of printed materials, which include fine grains and high-density dislocations. Compared with the traditional 316L SS, AM 316L showed higher initial strength and lower ductility. Regardless of sampling location, the AM 316L steel retained relatively high strength and ductility to the highest irradiation dose. A prompt necking at yield (with little uniform ductility) was observed after irradiation at 300 °C but no embrittlement was observed up to 10 dpa. Ductilization by irradiation–the radiation-induced increase of ductility–was observed for the 600 °C irradiation only and it occurred in low dose range only. The neutron irradiation increased the data variation in many tensile property datasets, particularly after 600 °C irradiation, and no clear dependence of tensile properties on build thickness or sampling location was observed.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Characterization of Aluminum Metal Powders for Plutonium-238 Program

As part of radioisotope thermoelectric generator (RTG) production for power sources in deep space exploration, Oak Ridge National Laboratory (ORNL) produces plutonium-238 ( 238 Pu). To produce 238 Pu, neptunium-237 ( 237 Np) targets are fabricated at ORNL and subsequently irradiated at the High Flux Isotope Reactor (HFIR) at ORNL and the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL). Specifically, current flowsheets utilize neptunium dioxide ( 237 NpO 2 ) targets. Aluminum (Al) powder is blended with 237 NpO 2 target material to improve thermal conductivity during irradiation. The current composition of 237 NpO 2 /Al pellets (i.e., cermets, or ceramic–metallics) is 20% 237 NpO 2 , 70% Al, and 10% void space. Al powders utilized by the 238 Pu program are high-fired under vacuum before blending into targets. The primary objective of this work is to measure the physical, chemical, and thermal properties of Al before and after the high-firing process. Properties of interest include the morphology, surface texture, particle size, crystal phase(s), and thermal conductivity of the material. These properties are measured with existing materials characterization equipment at ORNL, including powder x-ray diffraction (pXRD), scanning electron microscopy (SEM) with energy-dispersive spectroscopy (EDS), laser flash analysis (LFA), and thermogravimetric analysis (TGA). A secondary objective of this work is to compare the Al powders before and after the high-firing procedure to determine the effects of high-firing on chemical, physical, and thermal properties and to determine the efficacy of the high-firing process.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

High Data Rate Detector for Neutron Reflectometer

Neutron reflectometers are a class of instruments that employ neutron diffraction for measuring the structure of thin films. The technique provides valuable information over a wide variety of scientific and technological applications including chemical aggregation, polymer and surfactant adsorption, structure of thin film magnetic systems, biological membranes, etc. Such instruments are considered to be one of the most important in the neutron science field. Newer facilities place growing demands on the count rate capability of the specialized neutron detectors required. Proportional Technologies completed the Phase I effort successfully with a fully operational prototype detector built at PTI and tested at the CG1A neutron beam of the High Flux Isotope Reactor (HFIR, Oak Ridge, TN). The prototype incorporated 3 panels of 14 copper-walled cells each (total of 42 cells), each lined with 1.3 μm of 10B4C. The detector was tested for efficiency, spatial resolution, count rate linearity, uniformity, overlap and scatter. Testing revealed stable operation, uniform response across cells, and successful resolution of individual cells. The maximum count rate tested in the 3 panels combined was 590 kHz, limited by a deadtime of about 1 μs in the digital electronics. The local rate measured in a single cell showed no deadtime losses up to 810 cps/mm2, indicating that a rate of 20 Mhz can be supported in the 308-cell detector planned for Phase II.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2023

WIRE-21 Experiment Irradiation Conditions and In-Situ Data Collection

This report summarizes the in situ data collected during three cycles of irradiation (~75 days) of the Wireless Instrumented Removable Beryllium Experiment 2021 (WIRE-21) in the removable beryllium (RB) positions of the High Flux Isotope Reactor (HFIR). The experiment was designed primarily to evaluate the effects of high neutron flux and fluence on the performance of wireless temperature and pressure sensors being developed by Westinghouse Electric Company (WEC). WEC’s sensors could provide critical data regarding the evolution of centerline temperatures and pressurization due to fission gas release during fuel operation in light-water reactors (LWRs) or various advanced reactor applications. In addition to WEC’s wireless sensors, many other sensors were interrogated, including thermocouples, self-powered neutron detectors (SPNDs), distributed fiber optic temperature sensors, and passive neutron flux wires and silicon carbide thermometry.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

UCO TRISO Minifuel FY23 NSUF-Kairos Power Post-Irradiation Examination Status Report

Irradiation of miniature tristructural isotropic (TRISO)–coated particle fuel compacts at high-power particle was performed in the Oak Ridge National Laboratory’s (ORNL’s) High Flux Isotope Reactor (HFIR) using the MiniFuel irradiation capability. Each compact comprised 20 TRISO particles with a low-enriched uranium carbide uranium oxide (UCO), natural UCO, or low-enriched UO 2 kernel within a graphitic matrix. After irradiation, the MiniFuel targets and subcapsules were disassembled to recover the irradiated fuel specimens and pursue post-irradiation examination (PIE) to inform Kairos Power on the fuel specimen performance. This report describes the PIE results collected to date, including dilatometry on the passive thermometry to confirm the irradiation temperature, fission gas release measurements, and gamma counting. This work was funded by the Nuclear Science User Facilities program.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Report on the Analysis of Plutonium-238 Oxide, Campaign #P5PO

Oak Ridge National Laboratory (ORNL) is currently producing Plutonium-238 oxide for NASA space programs. Through the irradiation of NpO 2 pellets in the High Flux Isotope Reactor (HFIR), the production of Pu-238 oxide will be used for electrical power and heat on NASA spacecraft such as the Curiosity Mars Rover and the Voyager 1 and 2. The Transuranium Analytical Laboratory (TAL) leads the analytical effort for this project, which includes the dissolution of plutonium product oxide (PUP) and the analysis of the dissolved product solution using both radiological and inductively coupled plasma mass spectrometry (ICP-MS) techniques that are required to meet product specifications. The Transuranic Analytical Laboratory received three samples of Pu-238 oxide for analysis in January of 2022. This report documents the analytical protocols performed by the TAL along with the results produced from said analytical protocols. This report also includes a comparison with the general-purpose heat source (GPHS) specifications.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2024

Reduced Geometry for the NB5 Velocity Selector Shielding Box

This report details the reduced NB5 velocity selector shielding box that has been isolated from the complete HFIR CGH model in order to speed up detailed calculations of the velocity selector shielding. This shielding model is intended for outsourcing shielding optimization calculations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Road to PROSPECT-II

The Precision Reactor Oscillation and SPECTrum (PROSPECT) experiment is based in a segmented liquid scintillator antineutrino detector situated approximately 7 meters from the highly enriched High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory. Its main goal is to investigate short-baseline antineutrino oscillations. The first phase of data collection, known as PROSPECT-I, was held from 2018 to 2019 and was used for several high-precision analyses, including multiple measurements of the $^{235}U$ antineutrino spectrum and searches for $eV$-scale sterile antineutrino oscillations. The collaboration is now preparing for the second phase, PROSPECT-II, which features an upgraded detector design. This advancement will enhance sensitivity and statistical power, allowing for a broader range of analyses beyond those achieved in PROSPECT-I. As we transition into this new phase, new questions have arisen concerning background simulation and its potential differences from those conducted during the initial phase of the experiment. Moreover, it is essential to ascertain, through simulations, the positive effects that an improved detector could have on the study of oscillations. This information is crucial for justifying the proposed enhancements, and I will cover all of this in the talk.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2024

Mini-99 Experiment Design and Target Assembly

Qualification of nuclear fuels requires an understanding of a myriad of fuel performance variables, which requires time-consuming irradiations in test reactors. Accelerating burnup accumulation to reduce the irradiation time has historically been accomplished by increasing the 235 U enrichment in integral fuel tests, which inherently couples the fuel’s temperature and fission heat generation. Separate effects irradiation testing of nuclear fuel, using the MiniFuel target in the Oak Ridge National Laboratory’s (ORNL’s) High Flux Isotope Reactor (HFIR), offers an approach for decoupling fuel temperature and fission rate by reducing the quantity of the fuel and relying primarily on gamma heating in the surrounding components to drive fuel temperatures. However, if the fission rate is high enough, the fuel temperature will still vary over time as the fission heating changes, primarily due to poor heat conduction between the fuel and the surrounding components. This work details the design, analysis, and fabrication of a MiniFuel target which utilizes sodium bonding to improve the heat rejection from the fuel specimen, enabling the testing of higher 235 U enrichments (~8wt.%) to further accelerate burnup accumulation without prohibitively large temperature variations throughout the course of the irradiation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Oak Ridge National Laboratory's Strategic Research and Development Insights for Digital Twins

Oak Ridge National Laboratory (ORNL) is pleased to provide our response to the NITRD RFI on Digital Twins Research and Development. Digital twins are virtual representations of physical systems, leveraging real-time data to simulate and predict behaviors. ORNL is advancing digital twin technology across various disciplines, including neutron scattering, networking, science ecosystems, supercomputing, secure facilities, mobility technologies, materials design and discovery, power systems, fusion reactors, biological sciences, and earth observation. These efforts aim to enhance scientific research, operational efficiency, and decision-making processes. ORNL facilities, such as the High Flux Isotope Reactor (HFIR), Grid-C, Spallation Neutron Source (SNS), and Oak Ridge Leadership Computing Facility (OLCF), provide the infrastructure to develop and demonstrate these digital twin technologies. In this document, we lay out key challenges, research gaps, and future opportunities based on our experience with digital twins that aim to serve as useful contributions towards a National Digital Twins R&D Strategic Plan. In the remaining document, we address nine of the thirteen topic areas specified in the RFI.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2024

ROADRUNNER MiniFuel Experiment: Irradiation Target Design and Sample Characterization

High-density uranium nitride (UN) is a fuel candidate for several advanced nuclear reactor designs currently under development. Because there are limited UN performance data relative to fuel fabrication impurity and density variation, an irradiation campaign has been developed as part of a collaborative effort among the University of Texas at San Antonio (UTSA), Westinghouse Electric Company, Oak Ridge National Laboratory (ORNL), and Los Alamos National Laboratory (LANL) under the Nuclear Science User Facilities program. This project, entitled ROADRUNNER, or Research On ADvancing the peRformance of UraNium Nitrides in Extreme enviRonments, aimsto support UN fuel qualification for advanced reactors by investigating the impact of density and impurity variations on UN performance as a function of irradiation temperature and burnup. The MiniFuel experiment vehicle developed by ORNL, which leverages the High Flux Isotope Reactor, was selected to perform this accelerated separate-effects irradiation testing. The experiment test matrix consists of six MiniFuel targets containing miniature UN fuel disks, and targets three distinct burnup levels (37.5, 60, and 75 MWd/kg U) and three distinct temperatures (600, 900, and 1200°C). Neutronics and thermal analyses were performed to determine the experimental parameters needed to meet the desired irradiation conditions and to predict the experiment components temperatures. UN pellets were fabricated at LANL with tightly controlled parameters to produce specimens with three distinct densities and three levels of carbon content. The pellets were then thinned down by UTSA to the experiment-required thickness. The pre-characterization of the specimens includes density measurements, carbon and oxygen contents, microstructure analysis, and x-ray computed tomography. The selected specimens will be assembled into the MiniFuel experiment, and the first ROADRUNNER MiniFuel targets are intended for HFIR insertion during the Fall of 2024. After irradiation, the targets will be shipped to ORNL’s hot cell facility for disassembly. The post-irradiation examination on the fuel specimens includes fission gas release measurements, visual inspection, fuel swelling measurements, gamma spectroscopy, and microstructure analysis. The data collected post-irradiation will be used to develop fuel performance models.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Continued Evaluation of the Use of a Raman Spectrometer for H-Canyon Dissolver Monitoring

Remote monitoring of dissolver activities in H-Canyon can help operators avoid delays associated with excessive levels of fuel fragments remaining after a run. SRNL has proposed that effective monitoring can be achieved by using a Raman spectrometer to measure NO 2 concentrations in the offgas stream sampled from the facility stack. Prior work (SRNL-STI-2021-00451) measuring the offgas from one dissolution batch of High Flux Isotope Reactor (HFIR) fuel suggested a relationship between %NO 2 levels and fragment height. Herein, we report the results of monitoring and analysis of the dissolution of four batches of Material Test Reactor (MTR) fuel. A rigorous quantitative relationship between %NO 2 measurements and fragment heights could not be established, due to high uncertainties associated with both measurements. Uncertainties with gas measurements are associated with the %NO 2 levels in the offgas being close to the detection limit for the analyzer. Alternative gas measurement strategies are discussed which could improve sensitivity and reduce uncertainty. Limitations to the precision of the probe measurements are also discussed. It is also noted that the offgas is an average of the products from simultaneous dissolution of elements in multiple wells. Detection of a high fragment height level in an individual well may be hindered by low levels in other wells.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Fabrication and Characterization of MiniFuel Specimen

Burnable absorbers (BAs) are used in UO 2 fuels to tune the reactivity in a light water reactor (LWR) particularly at the beginning of life of the fuel. BAs are elements that have high neutron absorption cross sections and because of this property can prevent power peaking. The addition of BAs reduces the reactivity at the beginning of life, and this in turn allows for the increase of enrichments from > 5 % 235 U up to ~ 10 %. This also enables the increase of the burnup limit to 75 GWd/MTU and the cycle length to 24 months. The BA are eventually consumed under irradiation, and their concentration is diminished at roughly 10-20 GWd/MTU. The objective of this report is to fabricate UO 2 fuels that have been doped with BAs (Gd 2 O 3 in this case) and subsequently irradiate them in the high flux isotope reactor (HFIR) at Oak Ridge National Laboratory. The test specimen that are fabricated include 4 and 8 weight % Gd 2 O 3 doped UO 2 to investigate the influence of the BAs on the thermophysical properties and microstructure of the fresh and irradiated fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Testing and Characterization to Develop a Mechanistic Explanation for Unsaturated Drift of Fiber Optic Sensors during High-Dose Irradiation

The primary limitation for any optical fiber-based sensor for nuclear reactor applications is radiation-induced attenuation (RIA) of the transmitted and/or reflected signals. Based on several recent studies, RIA is tolerable for some fused silica optical fibers with the proper choice of sensing wavelength and fiber dopants. For extreme temperature applications (> 1000°C), sapphire optical fibers have been proposed; however, recent optical transmission measurements performed on bulk sapphire samples showed prohibitively large RIA. For some sensors, radiation-induced dimensional changes in the fiber materials can also cause significant drift. Moreover, the drift that was observed in numerous experiments performed in the High Flux Isotope Reactor (HFIR), the Advanced Test Reactor, the Massachusetts Institute of Technology Reactor, and other international facilities far exceeded what would be expected based on compaction of fused silica glass. Clearly, additional work is needed to better understand the origins of both RIA and radiation-induced drift in both silica and sapphire optical fiber-based sensors before these sensors can be reliably deployed for nuclear applications. This work evaluated the underlying mechanisms that may be responsible for RIA and drift in silica and sapphire materials. First, detailed characterization was performed on bulk fused silica glass samples that were previously irradiated to different neutron fluences at different temperatures to better understand the structural changes that drive radiation-induced drift in the absence of coating effects that are discussed later. Results show that the non-monotonic compaction that occurs with increasing neutron fluence continues up to fast neutron fluences approaching 10 22 n/cm 2 , which has important implications for physics-based models that may be used to compensate for the sensor drift. Initial Raman spectroscopy and synchrotron x-ray diffraction provide insights into the nature of the structural changes. Next, detailed characterizations were performed on silica fibers with various coatings that were subjected to several different thermal treatments. The hypothesis is that the coatings convert to carbon-rich materials that compact under irradiation, putting a large compressive strain on the fiber. Out-of-pile testing confirms that both polyimide and acrylate fiber coatings convert to glassy carbon (GC) materials when heated under inert conditions, and the degree of order (i.e., graphitization) increases with increasing temperature. The results provide increasingly strong evidence that the combination of polymeric coatings and inert (or vacuum) conditions render fiber optic sensors susceptible to significant radiation-induced drift that would not otherwise exist in uncoated fibers. Finally, transmission electron microscopy was performed on bulk sapphire samples that were irradiated to two neutron fluences at different temperatures to gain insights into the potential mechanisms driving the prohibitive RIA at higher neutron fluences and temperatures. Contrary to previous hypotheses, results show that scattering from radiation-induced voids cannot explain the observed RIA. Similarly, models for scattering losses from dislocation loops also do not agree with the experimental results. Instead, fitting to the experimental data shows that increased absorption from aluminum vacancy centers is the most likely explanation for the the prohibitively large RIA that was observed at high irradiation temperature and dose. In addition, the voids that formed in these single-crystal samples were found to align along the basal plane (a-axis) as opposed to that seen in previous observations of c-axis alignment in polycrystalline samples, which could have important implications for anisotropic swelling and other phenomena that could affect sensor performance at high neutron fluence.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2025

Neutron Scattering in High Magnetic Fields: Community Recommendations to Seize the Moment for Scientific Breakthroughs

Oak Ridge National Laboratory (ORNL) operates the world’s two most powerful neutron sources: the High Flux Isotope Reactor (HFIR) and the Spallation Neutron Source (SNS). These form a national user facility that provides neutron scattering instruments to probe and image static and dynamic properties of materials down to the atomic scale. Because the neutron carries a magnetic moment and the energies and wavelengths of neutrons match energy and length scales associated with magnetic materials, these facilities provide unique sensitivity to magnetism.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Testing and Characterization to Develop a Mechanistic Explanation for Unsaturated Drift of Fiber Optic Sensors during High-Dose Irradiation

The primary limitation for any optical fiber-based sensor for nuclear reactor applications is radiation-induced attenuation (RIA) of the transmitted and/or reflected signals. Based on several recent studies, RIA is tolerable for some fused silica optical fibers with the proper choice of sensing wavelength and fiber dopants. For extreme temperature applications (> 1000°C), sapphire optical fibers have been proposed; however, recent optical transmission measurements performed on bulk sapphire samples showed prohibitively large RIA. For some sensors, radiation-induced dimensional changes in the fiber materials can also cause significant drift. Moreover, the drift that was observed in numerous experiments performed in the High Flux Isotope Reactor (HFIR), the Advanced Test Reactor, the Massachusetts Institute of Technology Reactor, and other international facilities far exceeded what would be expected based on compaction of fused silica glass. Clearly, additional work is needed to better understand the origins of both RIA and radiation-induced drift in both silica and sapphire optical fiber-based sensors before these sensors can be reliably deployed for nuclear applications. This work evaluated the underlying mechanisms that may be responsible for RIA and drift in silica and sapphire materials. First, detailed characterization was performed on bulk fused silica glass samples that were previously irradiated to different neutron fluences at different temperatures to better understand the structural changes that drive radiation-induced drift in the absence of coating effects that are discussed later. Results show that the non-monotonic compaction that occurs with increasing neutron fluence continues up to fast neutron fluences approaching 10 22 n/cm 2 , which has important implications for physics-based models that may be used to compensate for the sensor drift. Initial Raman spectroscopy and synchrotron x-ray diffraction provide insights into the nature of the structural changes. Next, detailed characterizations were performed on silica fibers with various coatings that were subjected to several different thermal treatments. The hypothesis is that the coatings convert to carbon-rich materials that compact under irradiation, putting a large compressive strain on the fiber. Out-of-pile testing confirms that both polyimide and acrylate fiber coatings convert to glassy carbon (GC) materials when heated under inert conditions, and the degree of order (i.e., graphitization) increases with increasing temperature. The results provide increasingly strong evidence that the combination of polymeric coatings and inert (or vacuum) conditions render fiber optic sensors susceptible to significant radiation-induced drift that would not otherwise exist in uncoated fibers. Finally, transmission electron microscopy was performed on bulk sapphire samples that were irradiated to two neutron fluences at different temperatures to gain insights into the potential mechanisms driving the prohibitive RIA at higher neutron fluences and temperatures. Contrary to previous hypotheses, results show that scattering from radiation-induced voids cannot explain the observed RIA. Similarly, models for scattering losses from dislocation loops also do not agree with the experimental results. Instead, fitting to the experimental data shows that increased absorption from aluminum vacancy centers is the most likely explanation for the the prohibitively large RIA that was observed at high irradiation temperature and dose. In addition, the voids that formed in these single-crystal samples were found to align along the basal plane (a-axis) as opposed to that seen in previous observations of c-axis alignment in polycrystalline samples, which could have important implications for anisotropic swelling and other phenomena that could affect sensor performance at high neutron fluence.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗