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Microstructural characterization of the oxidation of nuclear graphite under chronic and accident conditions via XCT and synchrotron XCT

Graphite is a candidate material to moderate fast neutrons and for structural components in the US next-generation graphite-moderated reactors. A graphite core is conceived as a large formation of interconnected bricks that primarily serves as the moderator of fast neutrons, holds instrumentation, fuel elements, control rods, and is a receptacle for molten salts for Molten Salt Reactors (MSRs) designs. During the operation of a graphite-moderated power plant, graphite components might be subjected to chronic oxidation during normal operating conditions or aggressive oxidation as a result of accidental ingress of air that reacts vigorously with the graphite core. Using synchrotron, x-ray computed tomography (XCT), this research systematically characterized microstructural changes that accompanied these two oxidation scenarios. Chronic oxidation was studied by characterizing IG-110, PCEA, and NBG-18 specimens that were gradually oxidized in air at a low temperature (520°C). The accidental ingress of air into the graphite reactor was simulated by subjecting the grades mentioned above to high-temperature oxidation at approximately 750°C. This research is the first, in situ, systematic characterization of nuclear graphite microstructural evolution that can be associated with the two possible oxidation scenarios and provide insight into related repercussions. The results show that the microstructure and pore connectivity influence the rate of oxidation and evolution of the microstructure under the two oxidation regimes. These results are crucial to understanding which grades are more resilient to each type of oxidation and documenting the damage created in the graphite.

Arregui Mena, Jose'↗

A Fast Reactor Irradiation Experiment Design in the ATR

Modern modeling techniques were used to investigate a proposed method for fast neutron irradiations in an existing thermal-spectrum reactor, the Advanced Test Reactor (ATR). This method builds upon pre-existing ideas, where fast flux is increased by surrounding the specimens with fissionable “booster fuel” but diverges from historical approaches by using an already developed fuel element design used in the Belgian Reactor 2 (BR2) as the booster fuel while leveraging modern 3-D modeling and simulation techniques. Design evaluations and neutronics simulations were performed to evaluate the performance of a BR2 fuel element irradiated in an ATR flux trap with test pins in the central channel of the BR2 fuel element. These efforts have yielded promising results. Adding a BR2 fuel element in the northeast (NE) flux trap of ATR was predicted to result in a 150% increase to the incident fast neutron flux with a fast (>0.1 MeV) to thermal (<0.625 eV) neutron flux ratio ranging from approximately 50 to 150, dependent on the material used for thermal neutron filtering and volume of moderator within the central channel of the BR2 element. The predicted annual fast neutron fluence (>0.1 MeV) ranges from 7.9 × 1021 to 9.1 × 1021 n/cm2. Given the relatively large fast to thermal neutron flux ratio, the calculated radial power profiles within 4.3 mm outer diameter U10Zr fueled specimens irradiated within the BR2 booster fuel element are adequate representations of those within fast neutron reactors. The predicted radial power profiles are not flat, but they are more prototypic than those seen in advanced fuels tests which began in ATR in 2003. Another distinct advantage of this experiment design is that full-scale test pins can be irradiated to augment the ongoing series of reduced scale advanced fuels tests. The proposed experiment design irradiated within a BR2 fuel element in a flux trap of ATR offers an improved alternative to the current testing of advanced reactor fuels in ATR. Selected results from this design evaluation are presented.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Photon-to-Digital Converters for Neutron Imaging Instruments (Final Report)

Oak Ridge National Laboratory (ORNL) collaborated with the Université de Sherbrooke (UdeS) to design a modular and scalable tile of innovative digital photodetectors called Photon-to-Digital Converters (PDC) and the required subsystems to demonstrate the feasibility of large area single-photon detectors to support high-resolution, depth-of-interaction, fast neutron radiography based on scintillation detectors. The goal is to demonstrate the advantages of using PDC over conventional Silicon Photomultiplier (SiPM) for neutron imaging systems. The basic building blocks of analog SiPM and PDC are Single-Photon Avalanche Photodiodes (SPAD). The main difference between conventional SiPMs and PDCs, is in the fact that analog SiPMs sum the charge produced by individual SPAD passively, while in PDCs each SPAD is read out individually by an active electronic circuit. Hence, PDCs provide a direct photon-to-bit conversion where a logic “1” means that there was a detection in a given SPAD. Conversely, an analog SiPM requires a sophisticated preamplifier (current amplifiers or transimpedance amplifier) followed by a shaping amplifier and an analog-to-digital converter. Moreover, since the charge from each SPAD varies slightly, the passive sum of the analog SiPM will have signal fluctuations for the same amount of photon detected. This is one of many issues that is completely eliminated by individual one-to-one SPAD read out in PDCs. The large area required for scintillator readouts for neutron imaging is such that the output capacitance of a large area of SiPM arrays is very high. This creates a burden on the signal-to-noise optimization with respect to the power budget. For PDC, the power consumption is dictated by rate of the incident photon flux, or in photon-starved environments, the dark noise rate of the SPAD array. In other words, the power consumption in the absence of events is extremely low. Hence, the power consumption of a PDC read out system is much lower than its analog counterpart. Further, the large SiPM capacitance may introduce signal distortions on the scintillator fast rise or decay time with undesired effects on timing and pulse shape discrimination. The problem is absent in PDCs, as their readout is independent on device capacitance. UdeS is the world leader in 3D vertical integration of frontside illuminated SPAD arrays over CMOS readouts. These capabilities allow future production of “3D PDC” with maximum photosensitive fill factor and electronic functionalities tailored to the application. UdeS' vast knowledge of SPADs and CMOS design made the team an ideal collaborator in the development of large area high-resolution fast neutron radiography.

42 ENGINEERING↗

Impact of control blade insertion on the deformation behavior of SiC-SiC channel boxes in BWRs

This article describes the analysis of distortion of a silicon carbide fiber-reinforced, silicon carbide matrix (SiC-SiC) composite channel box under in-reactor conditions of a boiling water reactor (BWR). The BWR core has significant gradients in the fast neutron flux across the channel box due to the presence of water rods within the fuel assemblies, and these gradients increase further with the insertion of control blades. As a result of the temperature and neutron flux dependent irradiation-induced swelling of SiC, the SiC-SiC composite channel box can undergo distortion. In this work, we evaluate the SiC-SiC channel box distortion for three different control blade positions. This analysis is based on the neutron flux and temperature distributions in the BWR core calculated using the neutronics code MPACT and thermal-hydraulics code CTF. This calculation is coupled through temperature feedback. Subsequently, we have performed structural analysis based on the calculated neutron flux and temperature distributions to determine the deformation and stress development in the channel box. The structural analysis was performed using the fuel performance modeling code BISON and the commercial finite element analysis software Abaqus. The results indicate that large gradients in fast neutron flux (up to 35–40% across a single axial level) will develop across the channel box. Due to these gradients, the channel box will undergo time-dependent bending for all the control blade positions in the assembly. The time-dependent bowing behavior is dominated by the transient swelling of SiC-SiC material under non-uniform neutron flux, and changes with variation in the control blade position. The bending will cause temporary interference between the channel box and control blade, and the interference is expected to be most severe for the fully inserted control blade position. The developed stresses due to differential swelling in the channel box exceed the proportional limit stress of the material, which may cause matrix microcracking in the channel box. However, the stresses remain below the tensile strength of the material, and therefore, development of a full, through-thickness crack in the channel box is not expected. Finally, further work is recommended to explore and evaluate the mitigation strategies.

42 ENGINEERING↗

Irradiation of ultrasonic sensors and adhesive couplants for application in light water reactor primary loop piping and components

The Electric Power Research Institute (EPRI) Nuclear Sector and US Department of Energy Light Water Reactor Sustainability Program are committed to engaging in research and development endeavors to address materials aging issues specific to long term operation of light water power reactors. To this effect, EPRI launched an industry initiative to develop nondestructive evaluation systems for online monitoring of existing cracks in light water reactor primary coolant loop piping and components. One of the goals of this initiative is to develop a sensor system (or systems) that can determine nondestructively if cracks are growing or arrested and, in the case of the former, to characterize their growth rates. A missing component of this initiative is an experimental assessment of how sensors and adhesive couplants will perform in service when exposed to chronic energetic neutron radiation, particularly at the primary coolant loop hot and cold leg dissimilar metal welds, which join the primary loop piping to the reactor pressure vessel and reside in the vicinity of the reactor core. The objective of this experimental study was to determine how ultrasonic transducers and adhesive couplants perform when exposed to irradiation in a test reactor to simulate and accelerate in-service exposure. Further, to achieve this objective, the signal stability of piezoelectric transducers and performance of adhesive couplants as a function of accumulated fast neutron fluence were characterized by collecting ultrasonic data in-situ during irradiation. Of particular interest were the ultrasonic signal quality and time decay of the amplitude of acoustic reflections as a function of fast neutron fluence. The results of the study showed that, of the 8 transducer/substrate sample assemblies tested, only 3 generated usable ultrasonic signals through the conclusion of the irradiation campaign. It was found that high temperature epoxy tends to ultrasonically couple the sensors to the substrates better than three types of refractory ceramic cements studied, as is supported by post irradiation examination. The results obtained through this experimental study will be utilized in the achievement of the overall goal of development of a sensor system to perform online monitoring of primary loop components.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Assessment of CASL VERA for BWR analysis and application to accident tolerant SiC/SiC channel box

Application of the Virtual Environment for Reactor Applications (VERA) to BWR analysis is assessed in this paper by comparing results to those calculated using other widely-used modeling tools, namely the U.S. Nuclear Regulatory Commission’s PARCS/PATHS and the Serpent Monte Carlo particle transport code. Additionally, VERA is used to calculate 3-D temperature and fast neutron flux distributions in silicon carbide (SiC) fiber-reinforced, SiC matrix composite (SiC/SiC) BWR channel boxes, which are being studied as an Accident Tolerant Fuel core structural material concept. We found that the code-to-code comparisons were favorable, and the SiC/SiC channel box evaluation demonstrates the many advanced modeling features VERA provides while also highlighting the non-uniformity in fast neutron flux distributions that can play a role in potential SiC/SiC channel box deformation. Traditional BWR analysis tools do not have the calculation fidelity necessary for coupled assessment of flux and temperature gradients in a SiC/SiC channel box. VERA is a state-of-the-art modeling environment that was developed to increase the safety and economic competitiveness of nuclear power through improved modeling accuracy. While VERA has already been deployed in the nuclear industry for PWR applications, the current study is a vital initial step in the extensive development, validation, and verification that VERA must go through to be useful for BWR applications.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

HFIR SiC Bowing Test Ready to Insert

This report describes the successful assembly of a High Flux Isotope Reactor (HFIR) irradiation experiment designed to assess radiation-induced lateral bowing of silicon carbide fiber–reinforced, silicon carbide matrix composite (SiC/SiC) components under a radial fast neutron flux gradient. Excessive bowing of a SiC/SiC channel box in a boiling water reactor could potentially interfere with control blade movements. Similar concerns exist for SiC/SiC fuel cladding in light water reactors. The experiment described herein will provide experimental validation of the structural response of a miniature SiC/SiC channel box and tube specimens with pressurized water reactor diameters during irradiation. The significant radial fast neutron flux gradients that exist in the permanent reflector of HFIR were characterized using detailed three-dimensional neutronic calculations. The three-dimensional displacement damage dose rate profile and the resulting volumetric swelling in SiC were used as inputs to structural analyses that predicted the deformation and stresses in the channel box specimen. The specimens were thoroughly characterized prior to irradiation using traditional dimensional inspection and surface profilometry so that these measurements can later be compared with similar measurements that will be made post-irradiation to determine radiation-induced deformations. Furthermore, fine engraving markers were inscribed along all outer surfaces of the specimen and mapped using a digital microscope and a three-dimensional stage. This technique allowed for accurate measurements of the marker spacings, which can be compared with similar measurements that will be made post-irradiation to provide local radiation-induced strain mapping. The experiment was successfully assembled and is scheduled for insertion during HFIR cycle 492, which is currently scheduled to run from May 25, 2021 to June 18, 2021.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Sensitive Resources Assessment and Forest Analysis for the Proposed Versatile Test Reactor, Oak Ridge, Tennessee

The US Department of Energy’s (DOE’s) Oak Ridge National Laboratory (ORNL) is a leading institution in advanced materials, supercomputing, neutrons, and nuclear science. As a research laboratory managed by UT-Battelle, LLC for DOE, ORNL has national priorities in energy, security, and scientific discovery that necessitate facility improvements and expansions. DOE is also committed to environmental stewardship. The laboratory is located on the ~32,000-acre (~13,000-ha) Oak Ridge Reservation (ORR), much of which is categorized as a National Environmental Research Park (NERP) and a state Wildlife Management Area. DOE works with the Tennessee Wildlife Resources Agency (TWRA), Tennessee Department of Environment and Conservation (TDEC), US Fish and Wildlife Service (USFWS), US Department of Agriculture, and other agencies to serve as an effective steward of the ORR. Accordingly, project managers must conform to environmental regulations, agreements, and policies at the federal, state, and institutional levels. Per 40 CFR (Code of Federal Regulations) 1508.14, potential effects on research and science education also represent potential effects of federal actions on the NERP, and impacts on, e.g., deer harvest, must be considered on the Oak Ridge Wildlife Management Area when other aspects of the human environment are affected. The United States currently has no fast neutron testing capability to support advanced nuclear research and development. The proposed Versatile Test Reactor (VTR) will take advantage of current investments by the US government and private industry in nuclear reactors to expedite the design and construction process, using proven technology to create a world-class scientific infrastructure. The VTR will take advantage of fast neutrons provided by this proven technology, along with a capability to rapidly insert, conduct, and remove state-of-the-art experiments. An advantage of the VTR is that it can support future innovations in experimental capabilities without modifying the facility. The VTR will support progress in a variety of science and technology areas, including testing and qualification of advanced reactor fuels; testing and qualification of innovative structural materials; testing of innovative components and instruments; validation of advanced modeling and simulation tools; and versatility for future technical missions. Through proven technology, the VTR can take advantage of existing reactor designs and operating experience to reduce the risk, cost, and time for design and construction. The top available resources of DOE laboratories, industry, and universities will be used to expedite reactor design and construction toward developing the scientific infrastructure that affords a strong testing capability that can be sustained over many years. This report summarizes current knowledge of natural and cultural resources primarily within the VTR construction area. At the time of this report, the proposed VTR site design includes a construction area of ~150.4 acres (~69.9 ha), which contains an ~51.3-acre (~20.8-ha) operations area, located within forested natural areas of the ORR. The primary goal of the work presented here was to evaluate potential effects on sensitive resources that might result from development and construction activities associated with VTR. In addition to on-the-ground surveys during spring and summer 2020 by the ORNL Natural Resources Management Program and Aquatic Ecology Group staff, this report makes use of historical (pre-1995) and contemporary (1995 to present) data from additional confirmed sources (e.g., TDEC). Likewise, forest conditions were compiled from a 2011 forest inventory and supplemented with limited ground observations in 2020. The individuals who obtained and compiled the data presented here are familiar with and routinely assess sensitive resources on the ORR. Anyone who references this report must consider that the timing of surveys did not permit a complete delineation of the resources that will be affected. If the VTR project proceeds, additional surveys will be required to account for the seasonal patterns of various threatened and endangered species. Data deficiencies and potential resources that likely went undetected are indicated where possible. Accordingly, this report should facilitate more environmentally sound decisions during planning and 2 development of the VTR site, provide a foundation for further assessment of sensitive and cultural resources, and help project managers better address regulatory guidance and DOE policies on sustainable development in compliance with, for example, the US Endangered Species Act (ESA), Migratory Bird Treaty Act (MBTA), Tennessee Rare Plant Protection and Conservation Act of 1985, Tennessee Nongame and Endangered or Threatened Wildlife Species Conservation Act of 1974, several federal and state regulations regarding aquatic resource protection, and site-specific policies as outlined in various ORR management plans developed by ORNL and TWRA for DOE.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Efficient Prompt Scintillation and Fast Neutron-Gamma Ray Discrimination Using Amorphous Blends of Difluorenylsilane Organic Glass and in-situ Polymerized Vinyltoluene

High performance radiation detection materials are an integral part of national security, medical imaging, and nuclear physics applications. Those that offer compositional and manufacturing versatility are of particular interest. In this work, we report a new family of radiological particle-discriminating scintillators containing bis(9,9-dimethyl-9H-fluoren-2- yl)diphenylsilane (compound “P2”) and in-situ polymerized vinyltoluene (PVT) that is phase stable and mechanically robust at any blend ratio. The gamma-ray light yield increases nearly linearly across the composition range, to ~16,400 photons/MeV at 75 % wt. P2. These materials are also capable of γ/n pulse shape discrimination (PSD) and between 20-50 % P2 loading are competitive with the PSD quality of commercially-available plastic scintillators. The 137 Cs scintillation rise and decay times are sensitive to P2 loading and approach the values for “pure” P2. Additionally, the radiation detection performance of P2-PVT blends can be made stable in 60°C air for at least 1.5 months with the application of a thin film of poly(vinylalcohol) to the scintillator surfaces.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Effects of fast and thermal neutron irradiation on Ga-polar and N-polar GaN diodes

Studies of the radiation tolerance and electrical behavior of gallium nitride (GaN) based devices are important for the next generation of high-power and high-voltage electronics that may be subjected to harsh environments such as nuclear reactor and fusion facilities, particle accelerators, and post-denotation environments. Here, in this work, we study the behavior of Ga-polar and N-polar GaN Schottky diodes before and after exposure to fast and thermal + fast neutrons. Temperature-dependent current–voltage (I–V) and circular transmission line method (CTLM) measurements were used to study the electrical characteristics. A strong reduction in reverse leakage current and an increase in differential resistance in forward bias were observed after neutron irradiation. Thermionic emission (TE), Frenkel–Poole (FP) emission, and Fowler–Nordheim (FN) tunneling models were used to explain the forward and reverse I–V characteristics pre- and post-irradiation. The study confirms that Ga-polar and N-polar GaN Schottky diodes exhibit different electrical responses to fast and thermal neutron irradiations. The reverse bias characteristics of N-polar diodes are less affected after the fast neutron irradiation compared to Ga-polar diodes, while in the forward bias region, the electrical behavior after fast and thermal neutron irradiations is similar in Ga-polar and N-polar diodes. The results indicate that the role of orientation should be considered in the design of GaN-based radiation-tolerant electronics.

42 ENGINEERING↗

Periodic Fast Radio Bursts from Young Neutron Stars

Fast radio bursts (FRBs) are highly energetic radio pulses from cosmological origins. Despite an abundance of detections, their nature remains elusive. At least a subset of FRBs is expected to repeat, as the volumetric FRB rate surpasses that of any known cataclysmic event, which has been confirmed by observations. One of the proposed mechanisms to generate repeating FRBs is supergiant pulses from young and highly spinning neutron stars (NSs), in which case FRBs could inherit the periodicity of their parent NS. Here we examine the consequences of such a population of periodic fast radio bursts (PFRBs). We calculate the rate and lifetime of PFRB progenitors, and find that each newly born highly spinning NS has to emit a number ${N}_{\mathrm{PFRB}}\sim {10}^{2}$ of detectable bursts during its active lifetime of $\tau \sim 100$ yr, after which it becomes too dim and crosses a PFRB "death line" analogous to the pulsar one. We propose several tests of this hypothesis. First, the period of PFRBs would increase over time, and their luminosity would decrease, due to the NS spin-down. Second, PFRBs may show modest amounts of rotation measure, given the lack of expelled matter from the pulsar, as opposed to the magnetar-sourced FRBs proposed to explain the first repeater FRB 121102. As an example, we study whether the second confirmed repeater (FRB 180814) is a PFRB, given the preference for an inter-pulse separation of 13 ms within its sub-bursts. We show that, if confirmed, this period would place FRB 180814 in a different category as FRB 121102. We develop tests that would identify—and characterize—the prospective population of PFRBs.

79 ASTRONOMY AND ASTROPHYSICS↗

Baseline Postirradiation Examination of the FUTURIX-FTA Experiments

Postirradiation Examination (PIE) results from the baseline examination of the FUTURIX-FTA irradiation experiment are presented in this report. The FUTURIX-FTA irradiation was designed to study the fuel performance of candidate transmutation fuels. The FUTURIX-FTA experiment was conducted in the true fast neutron spectrum conditions of the Phénix sodium fast test reactor in France. FUTURIX-FTA contained several compositions that were also irradiated as part of the AFC-1 test in cadmium filtered positions in the Idaho National Laboratory (INL) Advanced Test Reactor (ATR) that approximate the neutron spectrum of a fast reactor. This experiment was a joint collaboration between the Department of Energy (DOE) in the U.S. and the Commissariat á l'Energie Atomique et aux Energies Alternatives (CEA) in France. A joint agreement between DOE and CEA was established in 2004 to conduct an irradiation experiment of metallic and nitride fuels in the Phénix reactor at CEA. Both the FUTURIX-FTA tests and the AFC-1 tests were conducted for the DOE Advanced Fuels Campaign (AFC) that is part of Fuel Cycle Research & Development (FCRD) program. These programs seek to develop and demonstrate the technologies needed to transmute long-lived transuranic actinide isotopes contained in spent nuclear fuel via fast reactor technology. The long term goal of this work is to reduce the radiotoxicity of future high level waste repositories. Post-irradiation examination of irradiated fuels experiments provides data related to in reactor fuel performance and input into future fuel design choices. The compositions of the FUTURIX-FTA pins were designed to test if minor actinides could be incorporated into the fuel of a fast reactor without significantly changing fuel performance observed for previously well studied fuels. The fuel performance of metallic fuel in fast reactors has been well documented. Likewise the irradiation performance of nitride fuels in fast reactors has also been documented. However the existing database for nitride fuels is much smaller than the database for metal fuels.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A revisitation of the ENEA TAPIRO Fast Source Reactor neutronic capabilities

This work is devoted to the analysis of the neutronic characterization of the ENEA-Casaccia center RSV TAPIRO fast neutrons source reactor performed during the 80's in the frame of a joint ENEA-SCK-CEN Mol collaboration. The Belgian scientist Albert Fabry, who was available to investigate a fast research reactor to perform a full characterization of the system neutron flux, led the TAPIRO experimental campaign. In particular, the paper is focused on the comparison between some 'recommended' Fabry experimental reaction rates traverses and nowadays MCNP Monte Carlo and ERANOS deterministic calculation results. It appears that the quality of the results depends on the penetration depth into the copper reflector. The influence of copper nuclear data are more evident in the ERANOS results. Massimo Salvatores has provided a great contribution to the interpretation of the TAPIRO neutronics: this humble work is dedicated to him.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

INL Report: Multiphysics Modeling and Simulation of Deimos, an Advanced Reactor Experiment

When designing a novel reactor, nuclear experiments are essential to validate the predictive capability of modeling/simulation tools and to justify the investment of a full-scale prototype. Being able to accurately predict temperature reactivity coefficients is of high importance to reactor designers as it impacts the safety and performance of the system. Deimos is a proposed graphite-moderated, beryllium-reflected, high assay low-enriched uranium (HALEU) tri-structural isotropic (TRISO) fueled experiment for NCERC. Deimos is a valuable experiment for validating the predictive performance of modeling and simulation tools since it comprises a relatively thermal energy spectrum with 84% thermal neutrons causing fission, 15% epithermal neutrons causing fission, and 1% fast neutrons causing fission. Additionally, by electrically heating the experiment, reactivity can be validated at various temperatures. Deimos will serve as a testbed for future advanced reactor concepts.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

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↗

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 ↗

Correlated Signal Analysis for Nuclear Emergency Response

In the context of nuclear emergency response (NER) scenarios, the critical task is to quickly identify a "black box" as a potential threat, as failing to do so could have catastrophic consequences. Techniques for passive assay of a “black box” typically include gamma-ray spectroscopy and neutron coincidence/multiplicity counting. However, there are significant challenges associated with these type of measurements. First, the presence of intervening materials can obstruct the detection of relevant signatures. Second, the presence of strong non-fission neutron sources, like (α, n) emitters, can add uncertainties to the neutron multiplicity analysis. In our LDRD-MFR Phase II work, a portable neutron spectrometer, called the Compact Fast Neutron Spectrometer (CFNS), was developed for NER applications. The CFNS system leverages information-rich neutron energy spectra to derive actionable information. This work investigates the use of correlated signals in the CFNS from special nuclear material (SNM) to characterize physical properties, such as intervening shielding material and fission to non-fission neutron contributions. In this report, the Phase II results from bulk SNM measurements at the National Criticality Experiments Research Center (NCERC) are briefly discussed along with the motivation for this work. Afterwards, simulations using the MCNPX-PoliMi transport code are discussed, which were used to expand our correlated signal study. Signal triggered analysis for neutron multiplicity extraction will also be discussed. Lastly, the use neutron-photon correlations for intervening material identification are shown, along with the use of correlated neutron energy spectra for α-ratio extraction.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Analysis of SPND Material Candidates for Real-Time Neutron Spectrum Monitoring Poster

The future of the nuclear industry will be shaped by advanced reactor designs requiring innovative instrumentation for safe operation. A key area of innovation is the ability to accurately and reliably monitor the neutron energy spectrum during operations, which would also enhance the experimental capabilities of existing research reactors. To address this need, our research focuses on the potential use of Self-Powered Neutron Detectors (SPNDs) for real-time neutron spectrum monitoring. We investigated various candidate materials for SPNDs by evaluating their energy-dependent reaction rates. Promising materials were further modeled using MCNP to determine the free electron production per neutron across the neutron energy spectrum, approximating their energy-dependent signal sensitivity. Our findings identified Samarium (Sm) and Gadolinium (Gd) as top candidates for thermal neutrons, Hafnium (Hf) and Thulium (Tm) for epithermal neutrons, and Tantalum (Ta) for fast neutrons. These materials will undergo future experimental validation to confirm the modeled responses and assess their feasibility for real-time neutron spectrum measurements.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗