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Fission Product and Actinide Distribution in the SiC Layer of Fissioned Triso Fuel Particles

Tri-structural Isotropic (TRISO) encapsulated fuel particles are used in next generation high-temperature gas-cooled nuclear reactors. The integrity of the fuel over a wide range of temperatures is integral to the safety of an operating nuclear reactor. It has been observed that fission products are released at high temperatures that simulate hypothesized accident scenarios. The particles under study were from the AGR-1 fuel development and qualification program. They consist of an enriched UCO fuel kernel surrounded by a dense carbon buffer layer (100 {mu}m), an inner pyrolytic carbon (IPyC) layer (40 {mu}m), a silicon carbide (SiC) layer (35 {mu}m), and an outer pyrolytic carbon (OPyC) layer (40 {mu}m). The SiC layer acts as the main diffusion barrier to fission products, but has been demonstrated to fail due to release of Ag through intact particles and local corrosion from metallic fission products such as Pd. In this work, we use transmission electron microscopy and diffraction techniques to study the structure and dispersion of release products within the SiC of TRISO particles as a function of annealing temperature used to simulate margin temperatures for in-reactor accident scenarios. In order to improve our understanding of fission product retention as a function of temperature, we have the unique opportunity to examine irradiated, fissioned TRISO particles to study post-irradiation effects on these materials. This data will contribute to current models used to predict the behavior of fission products in the SiC layer of TRISO fuels.

07 ISOTOPE AND RADIATION SOURCES↗

Project 57 Air Monitoring Report: January 1 through December 31, 2017

On April 24, 1957, the Atomic Energy Commission (AEC) (now the Department of Energy [DOE]) conducted the Project 57 safety experiment in western Emigrant Valley northeast of the Nevada National Security Site (NNSS, formerly the Nevada Test Site) on lands withdrawn by the Department of Defense (DOD) for the Nevada Test and Training Range (NTTR). The test was undertaken to develop (1) a means of estimating plutonium distribution resulting from a non-nuclear detonation; (2) biomedical evaluation techniques for use in plutonium-laden environments; (3) methods of surface decontamination; and (4) instruments and field procedures for prompt estimation of alpha contamination (Shreve, 1958). Although the test did not result in the fission of nuclear materials, it did disseminate plutonium across the land surface. Following the experiment, the AEC fenced the contaminated area and returned control of the surrounding land to the DOD. Various radiological surveys were performed in the area and in 2007, the DOE expanded the demarked Contamination Area (CA) by posting signs 200 to 400 ft (60 to 120 m) outside of the original fence. Plutonium in soil attaches preferentially to smaller particles (Tamura, 1985; Friesen, 1992; Murarik et al., 1992; and Misra et al., 1993). Therefore, redistribution of soil particles by wind (dust) and water are the mechanisms most likely to transport plutonium beyond the boundary of the Project 57 CA. Monitoring was implemented in 2011 by Desert Research Institute (DRI) to determine if radionuclide contamination was detectable in samples of airborne dust and to characterize meteorological and environmental parameters that influence dust transport. Initially, two monitoring stations consisting of radiological, meteorological, and dust sampling equipment were installed near the southeast and northeast corners of the CA. In January 2015, the original monitoring stations were dismantled and moved farther to the west along the CA boundary. This move was made to place the monitoring stations downwind of ground zero and the High Contamination Area (HCA) during the dominant northerly and southerly winds. Samples of particles suspended in the air are collected every two weeks and submitted for laboratory assessments of gross alpha and gross beta radioactivity, and for determinations of gamma-emitting radionuclides. In calendar year (CY) 2017, the mean gross alpha concentration at monitoring station P57-4 was approximately 4.25 times the value at monitoring station P57-3. In CY2015 and CY2016, the difference in mean gross alpha concentration at the two stations was approximately 1.5. The mean gross alpha concentrations at P57-3 and P57-4 were approximately 1.9 and 7.9 times, respectively, the mean gross alpha concentrations at the surrounding Community Environmental Monitoring Program (CEMP) stations. The minimum gross alpha concentrations reported for the Project 57 stations are in the range of the minimum values observed at the CEMP stations. However, maximum gross alpha concentrations are greater than the maximum concentrations observed at the surrounding CEMP stations. Gamma spectroscopy analyses resulted in the detection of seven radionuclides. Except for americium-241 (Am-241), all reported radionuclides occur naturally in the environment. The Am-241 detection by gamma spectroscopy was confirmed by alpha spectroscopy. During each quarter of CY2017, four suspended particulate matter samples were selected for alpha spectroscopy analysis. Two were selected each quarter from the regular biweekly samples collected at each of the two monitoring stations. Of the eight samples from P57-3, one was reported to have plutonium-238 (Pu-238) above the minimum detectable activity (MDA) and five were reported to have plutonium 239/240 (Pu-239/240) above the MDA. Of the eight samples from P57-4, three were reported to have Pu-238 above the MDA and six were reported to have Pu-239/240 above the MDA. Soil material is also transported by saltation, which is a wind driven phenomena that bounces sand-sized soil particles across the land surface because they are too heavy to be suspended in the air. Samples of particles transported by saltation were collected downwind and upwind of the CA at both monitoring stations in May 2017 after a 190-day deployment and again in September 2017 after a 114-day deployment. Mass of the saltation samples was determined after oven drying. The September sample had greater mass than the May sample. The same relationship was observed for the suspended particulate matter samples during periods of saltation sample collection. The difference in the collected mass appears to be because of the amount of soil moisture. Higher soil moisture exerts additional isotopic bonds between soil particles and water molecules, and between water molecules that envelop soil particles, making it more difficult for wind to raise the particles as dust. In general, samples collected from saltation traps facing south contained more material than samples collected from traps facing north. This suggests that although saltation material may have been moving back and forth in conjunction with the two dominant wind directions, there was a net trend for saltation material to be transported toward the north. Radiological analyses of the saltation samples show that the smaller particle size faction (<63 μm) generally produced the highest activity levels of Am-241, Pu-238, and Pu-239/240. In general, the isotope activity levels decreased as the particle size increased. These results are consistent with the expectation that the greatest potential for transport of radiological contamination is with the smaller particles. Thermoluminescent dosimeters (TLDs) indicated that the average annual external radioactivity dose at the monitoring stations is slightly higher than the dose determined at the surrounding CEMP stations, but approximately half of the estimated national average dose received by the general public from exposure to natural sources. The TLDs at the Project 57 monitoring stations are exposed to both natural sources (terrestrial and cosmic) and radioactive releases from the Project 57 CA. Winds in excess of approximately 15 mph (24 km/hr) begin to generate dust movement by saltation or suspension, as determined by the monitoring instruments. Saltated particles, PM10 (i.e., inhalable dust), and PM2.5 (i.e., fine particulate dust) exhibit an approximately exponential increase with increasing wind speed. The greatest concentrations of dust occurred for winds exceeding 20 mph (32 km/hr). When the wind/dust analysis was performed for winds separated into the dominant northerly and southerly wind directions, it was evident that the northerly winds generated the higher PM10 concentrations and had the dominate influence on the PM10 concentration determined for all wind speeds when all wind directions were evaluated together. During the year, winds in excess of 20 mph (32 km/hr) occurred approximately one percent of the time. Although winds sufficient to generate dust occur at the Project 57 site, they are infrequent and of short duration. A preliminary assessment of individual wind events suggests that dust generation in response to specific wind conditions is highly variable. Wind speeds that would be expected to generate noticeable dust may not do so in every instance. Additionally, saltation transport in response to wind conditions was less common than expected. These variations were likely because of the influence of meteorological and environmental parameters other than wind.

54 ENVIRONMENTAL SCIENCES↗

Evaluating Optical Techniques to Characterize Solid State Samples for the Pu-238 Supply Program

This report documents steps that have been taken to establish advanced characterization capabilities for solid-state samples to support the 238 Pu Supply Program. The program has already invested significantly in spectroscopy and online monitoring development for liquid processes. Many of the data, analytical methods, and equipment could also be leveraged for the analysis of Np/Pu oxides and Np pellets to help classify material properties and link them to operations. The techniques described in this work include diffuse reflectance spectroscopy (DRS), Raman spectroscopy, and laser-induced breakdown spectroscopy (LIBS). Each technique is sensitive to various chemical and/or elemental species and can provide complimentary information to more standard methods such as powder x-ray diffraction and scanning electron microscopy. These options are remotely deployable via fiber-optic cables. DRS and Raman spectroscopy are already approved for glove box and hot cell work, but LIBS requires US Department of Energy approval for incorporation. Raman spectroscopy does require laser shielding, which means that DRS is the easiest method to implement. However, each technique provides complimentary data, and the most robust sample characterization could be achieved when all three, among other methods, are harnessed together. This report documents some of the progress made testing these capabilities, some of the challenges, and next steps to optimize the technology and integration strategies.

07 ISOTOPE AND RADIATION SOURCES↗

MO-DE-BRA-01: Flipped Physics Courses Within a Radiologic Technologist Program: Video Production and Long Term Outcomes

Purpose: To determine if the flipped class format has an effect on examination results for a radiologic technologist (RT) program and discuss benefits from creating video resources. Methods: From 2001–2015, students had taken both a radiological physics and quality control (QC) class as a part of their didactic training. In 2005/2006, the creation of videos of didactic lectures and QC test demonstrations allowed for a flip where content was studied at home while exercises and reviews were done in-class. Final examinations were retrospectively reviewed from this timeframe. 12 multiple choice physics questions (MCP) and 5 short answer QC questions (SAQC) were common to pre and post flip exams. The RT program’s ARRT exam scores were also obtained and compared to national averages. Results: In total, 36 lecture videos and 65 quality control videos were created for the flipped content. Data was ∼2.4GB and distributed to students via USB or CD media. For MCP questions, scores improved by 7.9% with the flipped format and significance (Student’s t-test, p<0.05) was found for 3 of the 12 questions. SAQC questions showed improvement by 14.6% and significance was found for 2 of the 5 questions. Student enrollment increased from ∼14 (2001–2004) to ∼23 students (2005–15). Content was continuously added post-flip due to the efficiency of delivery. The QC class in 2003 covered 45 test setups in-class while 65 were covered with video segments in 2014. Flipped materials are currently being repurposed. In 2015, this video content was restructured into an ARRT exam review guide and in 2016, the content was reorganized for fluoroscopy training for physicians. Conclusion: We believe that flipped classes can improve efficiency of content delivery and improve student performance even with an increase in class size. This format allows for flexibility in learning as well as re-use in multiple applications.

07 ISOTOPE AND RADIATION SOURCES↗

Westinghouse Accident Tolerant Fuel Phase 2B with Higher Enriched and Higher Burnup Add-On Project Final Technical Report Deliverable Volume 1

The Westinghouse Electric Company LLC (Westinghouse) accident tolerant fuel (ATF) program funded by Westinghouse and the US Department of Energy (DOE) utilized chromium (Cr) coated zirconium alloy cladding with doped UO 2 (ADOPT(TM)) and uranium silicide (U 3 Si 2 ) high density/high thermal conductivity fuel for its lead test rod (LTR) program with irradiation beginning in 2019. ADOPT is a Cr 2 O 3 +Al 2 O 3 doped UO 2 pellet with increased oxidation resistance and density, and increased resistance to fission gas release. Due to the issues with U 3 Si 2 fuel reaction in pressurized water reactor (PWR) environments, uranium nitride (U 15 N) has been substituted for U 3 Si 2 as a long-term fuel option. Cr coated cladding with ADOPT fuel is the near-term Westinghouse EnCore fuel product. The long-term EnCore ® fuel product is SiGA ® SiC/SiC composite cladding with high density/high thermal conductivity UN fuel. In 2020, the higher burnup and higher enriched and (HBHE) program was integrated into the ATF program. The objective of this expanded program is to extend ATF burnups to at least 75 MWd/kgU to economically facilitate 24-month cycles in PWRs. The ATF program now includes ADOPT fuel with enrichments >5% 235 U. Over the past several years, Westinghouse has tested the Cr coated zirconium (Zr) and silicon carbide (SiC) claddings in Westinghouse Churchill autoclaves and the Massachusetts Institute of Technology (MIT) reactor. Additionally, the Cr coated cladding has been tested in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) and in LTR programs at the Doel 4 and Bryon 2 commercial reactors. High temperature tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried out to determine the time and temperature limits for the Cr coated zirconium claddings. These tests indicate that Cr coated Zr cladding can take temperatures up to about 1500°C for short periods of time without becoming totally oxidized. The main issue is the formation of the Cr-Zr eutectic at 1333°C resulting in the migration of this eutectic inward with the formation of ZrCr 2 which rapidly oxidizes to ZrO 2 on the outside of the tube. The Cr coated Zr cladding also delays the bursting of the tube, reduces the burst area, and reduces hydriding and embrittlement of the Zr which is a major benefit for reducing fuel fragmentation, redistribution, and dispersal (FFRD), the major licensing issue faced by HBHE. The manufacturing parameters for the SiC have been found to have a significant effect on the corrosion rate of the SiC in light water reactor (LWR) conditions and significant improvements have been made in the yield, quality, and oxidation resistance of the SiC cladding by identifying and tightening manufacturing process parameters. Current autoclave results for SiC composite claddings indicate that a corrosion rate of fewer than 2 micrometers per year can be achieved which meets corrosion requirements under normal operating conditions. High temperature steam oxidation tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried and determined that SiC cladding can withstand temperatures up to about 1800°C to 1900°C before excessive corrosion reactions begin, and that the SiC will not balloon and burst. ADOPT fuel pellets were incorporated into the Westinghouse ATF program because of their increased density and oxidation resistance. A topical report supporting the use of ADOPT pellets has been submitted to the NRC and will be approved shortly. ADOPT pellets have been a product in Europe for over 15 years. The additives work to make larger grain sizes which appear to reduce fission gas release during transients as well as increase the density of the pellet. Fuel rod and assembly design in preparation for the lead test rod (LTR) and lead test assembly (LTA) programs is underway as well as licensing efforts with the Nuclear Regulatory Commission (NRC). Finally, accident analyses coupled with economic evaluations for both operating savings as well as fuel savings have been initiated. Modular Accident Analysis Program 5 (MAAP5) calculations indicate that both Cr coated cladding and SiC composite cladding can increase the time to fuel rod loss of geometry for up to two hours longer than current Zr based cladding in a station blackout scenario. This additional time is due to the much higher oxidation resistance of the SiC and Cr coated cladding. These two hours can be used to implement additional response options instituted through the Diverse and Flexible Mitigation Capability (FLEX) program by reactor operators. Both ATF cladding options also reduce hydrogen production which dramatically reduces primary system and containment pressure and the risk of fission product release beyond containment in the unlikely event of an accident. The lower pressure in the system allows more time to feed cooling water to the core, resulting in the avoidance of fuel melting. The coping time is extended indefinitely if the modest water flow provided by FLEX continues. Experimental work on methods to rapidly fabricate SiC composite structures with high density and reduce the fabrication price of SiC fibers while maintaining a high level of performance is needed. Methods for mitigating or stopping the Cr-Zr eutectic are also needed to further improve the oxidation resistance of Cr coated Zr. Minimal (<1%) swelling of U 3 Si 2 and subsequent fission gas release has been demonstrated up to 20 MWd/kgU. Irradiation experiments with U 3 Si 2 fuel in ATR to determine these properties at 40 MWd/kgU were completed but post irradiation examinations were not done since U 3 Si 2 has been replaced by UN. UN has three issues that are being addressed. The first is increasing the oxidation resistance so that there is not excessive reaction up to ~1500°C. While UN increases the pellet density and additives to the UN postponed the temperature at which rapid oxidation occurred by ~100°C to 200°C, this is not enough, and pellet coating options are now being pursued. The second is developing a method to manufacture that does not require the multi-step process of UF 6 to UO 2 to UC to UN. Efforts are underway looking at UF 6 to UN 2 to UN and UF 6 to UF 4 to UN 2 to UN reactions. Finally, an economically acceptable process for potentially enriching the 15 N content of the nitrogen used to make UN to >95% 15N was identified though not experimentally validated. In addition to the work supported by the DOE, research and testing activities are being carried on in a world-wide effort funded by many countries such as Sweden, United Kingdom, Belgium, Netherlands, Spain, Germany, Japan, and France. This work is being facilitated through the Westinghouse led Collaboration for Advanced Research on Accident Tolerant Fuel (CARAT) program. Annual meetings were organized in 2018 and 2019 by Westinghouse as a venue for presentation of this work and to provide for the cross-fertilization of ideas among the many outstanding researchers in the ATF area. No meetings were held in 2020 and 2021 due to the COVID-19 related restrictions on traveling and gatherings. Since SiC, coated cladding, and high-density fuel options are not currently used in the nuclear industry; support from the government and industry members is needed to further the significant effort of setting new standards. The same is true for the Nuclear Regulatory Commission (NRC) which must review and approve the commercial use of these new fuels since all current regulations are oriented toward Zr/UO 2 fuel. Several meetings have been held with the NRC to generate a fast-track approach to licensing ATF using a combination of atomic modeling, in-rod sensors, and in-reactor testing. This approach was memorialized in an “Accelerated Fuel Qualification White Paper” prepared by the Accelerated Fuel Qualification Working Group lead by General Atomics.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Westinghouse Accident Tolerant Fuel Phase 2B with Higher Enriched and Higher Burnup Add-On Project Final Technical Report Deliverable Volume 2

The Westinghouse Electric Company LLC (Westinghouse) accident tolerant fuel (ATF) program funded by Westinghouse and the US Department of Energy (DOE) utilized chromium (Cr) coated zirconium alloy cladding with doped UO 2 (ADOPT(TM)) and uranium silicide (U 3 Si 2 ) high density/high thermal conductivity fuel for its lead test rod (LTR) program with irradiation beginning in 2019. ADOPT is a Cr 2 O 3 +Al 2 O 3 doped UO 2 pellet with increased oxidation resistance and density, and increased resistance to fission gas release. Due to the issues with U 3 Si 2 fuel reaction in pressurized water reactor (PWR) environments, uranium nitride (U 15 N) has been substituted for U 3 Si 2 as a long-term fuel option. Cr coated cladding with ADOPT fuel is the near-term Westinghouse EnCore ® fuel product. The long-term EnCore fuel product is SiGA ® SiC/SiC composite cladding with high density/high thermal conductivity UN fuel. In 2020, the higher burnup and higher enriched and (HBHE) program was integrated into the ATF program. The objective of this expanded program is to extend ATF burnups to at least 75 MWd/kgU to economically facilitate 24-month cycles in PWRs. The ATF program now includes ADOPT fuel with enrichments >5% 235 U. Over the past several years, Westinghouse has tested the Cr coated zirconium (Zr) and silicon carbide (SiC) claddings in Westinghouse Churchill autoclaves and the Massachusetts Institute of Technology (MIT) reactor. Additionally, the Cr coated cladding has been tested in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) and in LTR programs at the Doel 4 and Bryon 2 commercial reactors. High temperature tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried out to determine the time and temperature limits for the Cr coated zirconium claddings. These tests indicate that Cr coated Zr cladding can take temperatures up to about 1500°C for short periods of time without becoming totally oxidized. The main issue is the formation of the Cr-Zr eutectic at 1333°C resulting in the migration of this eutectic inward with the formation of ZrCr 2 which rapidly oxidizes to ZrO 2 on the outside of the tube. The Cr coated Zr cladding also delays the bursting of the tube, reduces the burst area, and reduces hydriding and embrittlement of the Zr which is a major benefit for reducing fuel fragmentation, redistribution, and dispersal (FFRD), the major licensing issue faced by HBHE. The manufacturing parameters for the SiC have been found to have a significant effect on the corrosion rate of the SiC in light water reactor (LWR) conditions and significant improvements have been made in the yield, quality, and oxidation resistance of the SiC cladding by identifying and tightening manufacturing process parameters. Current autoclave results for SiC composite claddings indicate that a corrosion rate of fewer than 2 micrometers per year can be achieved which meets corrosion requirements under normal operating conditions. High temperature steam oxidation tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried and determined that SiC cladding can withstand temperatures up to about 1800°C to 1900°C before excessive corrosion reactions begin, and that the SiC will not balloon and burst. ADOPT fuel pellets were incorporated into the Westinghouse ATF program because of their increased density and oxidation resistance. A topical report supporting the use of ADOPT pellets has been submitted to the NRC and will be approved shortly. ADOPT pellets have been a product in Europe for over 15 years. The additives work to make larger grain sizes which appear to reduce fission gas release during transients as well as increase the density of the pellet. Fuel rod and assembly design in preparation for the lead test rod (LTR) and lead test assembly (LTA) programs is underway as well as licensing efforts with the Nuclear Regulatory Commission (NRC). Finally, accident analyses coupled with economic evaluations for both operating savings as well as fuel savings have been initiated. Modular Accident Analysis Program 5 (MAAP5) calculations indicate that both Cr coated cladding and SiC composite cladding can increase the time to fuel rod loss of geometry for up to two hours longer than current Zr based cladding in a station blackout scenario. This additional time is due to the much higher oxidation resistance of the SiC and Cr coated cladding. These two hours can be used to implement additional response options instituted through the Diverse and Flexible Mitigation Capability (FLEX) program by reactor operators. Both ATF cladding options also reduce hydrogen production which dramatically reduces primary system and containment pressure and the risk of fission product release beyond containment in the unlikely event of an accident. The lower pressure in the system allows more time to feed cooling water to the core, resulting in the avoidance of fuel melting. The coping time is extended indefinitely if the modest water flow provided by FLEX continues. Experimental work on methods to rapidly fabricate SiC composite structures with high density and reduce the fabrication price of SiC fibers while maintaining a high level of performance is needed. Methods for mitigating or stopping the Cr-Zr eutectic are also needed to further improve the oxidation resistance of Cr coated Zr. Minimal (<1%) swelling of U 3 Si 2 and subsequent fission gas release has been demonstrated up to 20 MWd/kgU. Irradiation experiments with U 3 Si 2 fuel in ATR to determine these properties at 40 MWd/kgU were completed but post irradiation examinations were not done since U 3 Si 2 has been replaced by UN. UN has three issues that are being addressed. The first is increasing the oxidation resistance so that there is not excessive reaction up to ~1500°C. While UN increases the pellet density and additives to the UN postponed the temperature at which rapid oxidation occurred by ~100°C to 200°C, this is not enough, and pellet coating options are now being pursued. The second is developing a method to manufacture that does not require the multi-step process of UF 6 to UO 2 to UC to UN. Efforts are underway looking at UF 6 to UN 2 to UN and UF 6 to UF 4 to UN 2 to UN reactions. Finally, an economically acceptable process for potentially enriching the 15 N content of the nitrogen used to make UN to >95% 15 N was identified though not experimentally validated. In addition to the work supported by the DOE, research and testing activities are being carried on in a world-wide effort funded by many countries such as Sweden, United Kingdom, Belgium, Netherlands, Spain, Germany, Japan, and France. This work is being facilitated through the Westinghouse led Collaboration for Advanced Research on Accident Tolerant Fuel (CARAT) program. Annual meetings were organized in 2018 and 2019 by Westinghouse as a venue for presentation of this work and to provide for the cross-fertilization of ideas among the many outstanding researchers in the ATF area. No meetings were held in 2020 and 2021 due to the COVID-19 related restrictions on traveling and gatherings. Since SiC, coated cladding, and high-density fuel options are not currently used in the nuclear industry; support from the government and industry members is needed to further the significant effort of setting new standards. The same is true for the Nuclear Regulatory Commission (NRC) which must review and approve the commercial use of these new fuels since all current regulations are oriented toward Zr/UO 2 fuel. Several meetings have been held with the NRC to generate a fast-track approach to licensing ATF using a combination of atomic modeling, in-rod sensors, and in-reactor testing. This approach was memorialized in an “Accelerated Fuel Qualification White Paper” prepared by the Accelerated Fuel Qualification Working Group lead by General Atomics.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Analysis of Synergistic Fuel Cycle Options with Thorium and Heavy Water Reactors

Fuel cycle options (FCOs) with thorium-based fuels have characteristics that may have benefits for meeting certain objectives, such as transuranic actinide inventory management and overall natural resource utilization. Neutron irradiation of thorium and uranium-233 results in negligible production of transuranic actinides. This advantage is compromised, to a degree, when thorium fuels are used in conjunction with uranium-238; however, strategic reprocessing and fuel use (e.g., recycle of plutonium and/or minor actinides) can be used to manage this problem. Furthermore, thorium FCOs with reprocessing can extend the availability of natural nuclear resources by breeding new fissile material, recovering and recycling unused material, and achieving high burnups. In instances where natural thorium is more readily available than uranium, FCOs which use thorium may be preferable from sustainability and energy security perspectives. However, many hybrid uranium-thorium FCOs struggle to perform well in this regard, since large amounts of external fissile material (and therefore natural uranium) are required to breed the required uranium-233. DOE's evaluation and screening effort reports that for every metric ton (MT) of U-233 bred in a light water reactor for reuse, about 1000 MT of natural uranium are required to support such breeding, much of which is used inefficiently due to enrichment. The combination of HWRs and thorium-based fuels has the potential to reduce this consumption of natural uranium resources. Because heavy water moderates neutrons without significant absorption, fissile material requirements are lower compared to those of LWRs. This has enabled conventional 'once-through' HWRs to operate with only slightly-enriched or even natural uranium. Also, HWRs can be combined with LWRs in multistage FCOs where used LWR fuel can be processed and the remaining fissile content is sufficient to support use as fuel in HWRs in spite of the presence of neutron poisons (e.g., uranium-236); this concept has been demonstrated at a research scale in Korea. Thus, additional energy is extracted from the same initial natural uranium feed and uranium enrichment effort. Another consideration with using thorium-based fuels in HWRs is the current limited operational experience of the reactors and associated fuel cycle facilities using these fuels. However, work continues internationally towards gaining further experience. For example, at equilibrium the third stage of India's planned Three-Stage Nuclear Power Program uses thorium/uranium-233 or thorium/plutonium fuels with a fissile supply from second-stage fast reactors. Further, China plans to experiment with low-enriched uranium (LEU)-Th CANFLEX fuel bundles in a once-through configuration in its HWRs and a long-term objective is to transition to thorium use in a closed HWR FCO. Vanderbilt University (VU) and Oak Ridge National Laboratory (ORNL) are characterizing multi-stage, thermal-reactor FCOs that incorporate thorium and examining their potential performance. This paper presents insights from the examination of FCOs which consider the synergy of HWRs and thorium. Two multi-stage FCOs which incorporate thorium-based fuels in HWRs have been examined for their potential, one which uses recycled PWR uranium oxide fuel in conjunction with thorium in an HWR, and another that uses recycled HWR fuel in an MSR which also includes thorium. Both of the systems studied offer resource utilization improvements as compared to a once-through LWR fueled with low-enrichment uranium and highlight the potential synergy of thorium and HWRs. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A Verification of Flux Sensitivity Estimates Using the MCNP Tally Perturbation Tool

Nuclear data is commonly used in applications such as nuclear nonproliferation, safeguards, and criticality safety. More specifically, nuclear data is used in predictive simulation codes like the Monte-Carlo N-Particle (MCNP ® ) transport code, Serpent, and similar radiation transport codes. The improvement of nuclear data enables more precise and accurate simulations, which result in higher fidelity designs and reduced operational/procedural costs. Therefore, the improvement of nuclear data is of paramount importance across the nuclear community. Nuclear data is improved and validated through integral benchmark experiments. The design of benchmark experiments is an extensive process; therefore, these experiments are often optimized on multiple characteristics, including sensitivity to the nuclear data, during the design process. Sensitivity is a measure of how much a quantity changes due to changes in independent variables such as experimental configuration. An experimental design that has a larger sensitivity to the nuclear data of interest will have a larger impact on the accuracy and precision of the validated data. Past integral benchmark experiments have primarily used the effective multiplication factor ($k_{eff}$) as the predominant measured quantity; however, experiments designed with other quantities in mind would be able to optimize on validating different areas of the nuclear data. A primary goal of the EUCLID project is to design, constrain, and reduce compensating errors in experiments focused on quantities other than $k_{eff}$ to better validate nuclear data across the board. Currently, there is a capability in MCNP to easily calculate the sensitivity of $k_{eff}$ to specific nuclear data of numerous reactions types and isotopes (KSEN card); however, the sensitivity of other quantities must be estimated in more strenuous manners. For example, the perturbation feature (PERT card) of MCNP can be used to estimate first-order sensitivities of some response in fixed source simulations. A recent announcement revealed that the first- and second-order perturbation features in previous releases of MCNP contained a bug. It was identified that particles were being scored into the wrong energy bin. The bug is in the most recent public release (MCNP6.2); however, a patch has been added to the most up to date version (MCNP6.2.2) that has not been released publicly. A direct comparison of the PERT card results for an F4 (neutron flux averaged over a cell) tally before and after the patch are shown in figure 1. All simulations used in the sensitivity estimates in this report were performed with MCNP6.2.2. This work verifies the patched MCNP perturbation tool by comparing first order sensitivities made using the PERT card to estimates made using manual perturbation of the compact ENDF (ACE) files.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Evaluating Age Effects on HEPA Filter Performance

Nuclear grade high efficiency particulate air (HEPA) filters are routinely employed as the final control element in confinement ventilation systems. The traditional HEPA filter utilizes a pleated filter medium of fibrous glass that has been produced in a manner analogous to manufacturing paper. These filters are the physically weakest element in a containment ventilation system. Containment ventilation systems are designed to condition the air-stream (temperature, relative humidity, moisture, particle size distribution of aerosols, and aerosol concentration) to levels/conditions that fibrous glass HEPA filters can handle. Approximately 6000 nuclear grade HEPA filters are purchased each year for use in the DOE/NNSA complex. Additional filters are purchased for use in commercial nuclear power generation and ventilation systems of other nuclear applications. These filters are designed and tested in accordance with the American Society of Mechanical Engineers (ASME) AG-1 Code Nuclear Air and Gas Treatment. This code establishes design requirements and qualification procedures. Qualification testing of axial flow filters is described in paragraphs 5000 and following of AG-1. The series of qualification tests are intended to describe the operating envelope of HEPA filters and verify the reliability of a filter design. AG-1 qualification also confirms the pedigree of components used in manufacture for that filter design. The collective set of qualification tests establishes the assumed operating envelope for AG-1 filters. The effects of age on HEPA filter performance have been a concern for at least two decades. A combination of physical evaluation of aged filter media and a review of filter failure records resulted in Appendix C of the Nuclear Air Cleaning Handbook (NACH), Determination of HEPA Filter Life. This states that HEPA filters are not to be used beyond 10 years from the date of manufacture. Additionally, filters put into service in locations where they may become wet are to be taken out of service five years from date of manufacture. Filters that have become wet are to be taken out of service immediately. Finally, it should also be pointed out that filters held in Level B storage are subject to the same 10-year service life. Very limited bench-scale testing in the 1990's raised concern that aging HEPA filters do not have the strength to withstand an accident scenario. In May of 1999, the DNFSB released a Technical Report 23 entitled HEPA Filters Used in the Department of Energy's Hazardous Facilities. This report expressed concerns for the potential vulnerability of HEPA filters in vital safety systems. Concerns and uncertainty associated with degradation of HEPA filter performance over time led the DOE sites to limit HEPA filter service life to 10 years from the date of manufacture or five years in cases where filters may become wet. Establishment of a conservative service life needs to be based on data from a structured series of tests comparing the performance envelope of new and aged full-scale filters. A service life that is insufficiently conservative endangers workers and the public. One that is excessively conservative costs can cause hundreds of otherwise unnecessary filter changes. This increases exposure of employees, disrupts facility operations, and increase disposal costs by millions of dollars annually. Conclusive data are needed to resolve uncertainty associated with the damaging effects of aging on durability of HEPA filters. Therefore, this study needs to provide a sufficient body of evidence to allow DOE and site professionals to make prudent decisions. An updated version of ASME AG-1 Section FC included a non-mandatory appendix that would include the DOE guidance for service life of HEPA filters. Balloting of this revision generated significant resistance to inclusion of any kind of service life language citing the lack of supporting experimental data. Efforts to resolve negative votes failed and resistance to acceptance of the language increased. The result has been to not include service language in Section FC and requests to remove it from sections that already include such language. The recent activity of the ASME AG-1 Committee on Nuclear Air and Gas Treatment effectively de-emphasizes following DoE's service life guidelines. The DOE Office of Nuclear Safety under its NSR and D program provided the Mississippi State University Institute for Clean Energy Technology (ICET) finding to initiate a study to determine the effects of aging on AG-1 axial flow filters just prior to actions taken within the AG-1 committee regarding service life. The NSR and D funding facilitated timely development of a national technical working group comprised of members from the regulatory community, DOE complex, and commercial power to resolve uncertainty associated with effects of aging. The Department of Energy Office of Environmental Management (DOE-EM) has been funding the ICET to evaluate the performance envelope for AG-1 HEPA filters. ICET is one of DOE-EM's qualified suppliers. Synergy has been achieved by associating the NSR and D aged filter activities to testing activities evaluating the performance envelopes of separator and separator-less AG-1 HEPA filters funded by DOE-EM. The DOE-EM funded activities establish baseline data for the aged filter study and future EM funding will provide long term support for testing additional aged filters. EM funding of new filters includes analytical evaluation of media tensile strength by thermal analysis to establish baseline values and determine mass loss of moisture resistance and acrylic binders due to use. All of these values can be used for comparison of test results for aged filters. (authors)

07 ISOTOPE AND RADIATION SOURCES↗

SU-G-TeP2-15: Feasibility Study of Fiber-Optic Cerenkov Radiation Sensors for in Vivo Measurement: Dosimetric Characterization and Clinical Application in Proton Beams

Purpose: To evaluate the possibility of a fiber-optic Cerenkov radiation sensor (FCRS) for in vivo dose verification in proton therapy. Methods: The Cerenkov radiation due to the proton beam was measured using a homemade phantom, consisting of a plastic optical fiber (POF, PGSCD1001-13-E, Toray, Tokyo, Japan) connected to each channel of a multianode photomultiplier tube (MAPMT:H7546, Hamamatsu Photonics, Shizuoka, Japan). Data were acquired using a multi-anode photomultiplier tube with the NI-DAQ system (National Instruments Texas, USA). The real-time monitoring graphic user interface was programmed using Labview. The FCRS was analyzed for its dosimetrics characteristic in proton beam. To determine the accuracy of the FCRS in proton dose measurements, we compared the ionization chamber dose measurements using a water phantom. We investigated the feasibility of the FCRS for the measurement of dose distributions near the superficial region for proton plans with a varying separation between the target volume and the surface of 3 patients using a humanoid phantom. Results: The dose-response has good linearity. Dose-rate and energy dependence were found to be within 1%. Depth-dose distributions in non-modulated proton beams obtained with the FCRS was in good agreement with the depth-dose measurements from the ionization chamber. To evaluate the dosimetric accuracy of the FCRS, the difference of isocenter dose between the delivery dose calculated by the treatment planning system and that measured by the FCRS was within 3%. With in vivo dosimetry using the humanoid phantom, the calculated surface doses overestimated measurements by 4%–8% using FCRS. Conclusion: In previous study, our results indicate that the performance of the array-type FCRS was comparable to that of the currently used a multi-layer ion chamber system. In this study, we also believe that the fiber-optic Cerenkov radiation sensor has considerable potential for use with in vivo patient proton dosimetry.

07 ISOTOPE AND RADIATION SOURCES↗

MO-FG-CAMPUS-IeP1-05: New Ionization Chamber Dosimetry of Absorbed Dose to Water in Diagnostic KV X-Ray Beams

Purpose: To develop new ionization chamber dosimetry of absorbed dose to water in diagnostic kV x-ray beams, by using a beam quality conversion factor, kQ, for Co-60 to kV x-ray and an ionization conversion factor for a water-substitute plastic phantom. Methods: kQ was calculated for aluminum half value-layers (Al-HVLs) of 1.5 mm to 8 mm which were generated by kV x-ray beams of 50 to 120 kVp. Twenty-two energy spectra for ten effective energies (Eeff) were calculated by a SpecCalc program. Depth doses in water were calculated at 5 × 5 to 30 × 30 cm{sup 2} fields. Output factors were also obtained from the dose ratio for a 10 × 10 cm{sup 2} field. kQ was obtained for a PTW30013 Former ion chamber. In addition, an ionization conversion factor of the PWDT phantom to water was calculated. All calculations were performed with EGSnrc/cavity code and egs-chamber codes. Results: The x-ray beam energies for 1.5 mm to 8 mm Al-HVLs ranged in Eeff of 25.7 to 54.3 keV. kQ for 1.5 mm to 8 mm Al-HVLs were 0.831 to 0.897, at 1 and 2 cm depths for a 10 × 10 cm2 field. Similarly, output factors for 5 × 5 to 30 × 30 cm{sup 2} fields were 0.937 to 1.033 for 25.7 keV and 0.857 to 1.168 for 54.3 keV. The depth dose in a PWDT phantom decreased up to 5% compared to that in water at depth of ten percent of maximum dose for 1.5 mm Al-HVL. The ionization ratios of water/PWDT phantoms for the PTW30013 chamber were 1.012 to 1.007 for 1.5 mm to 8 mm Al-HVLs at 1 cm depth. Conclusion: It became possible to directly measure the absorbed dose to water with the ionization chamber in diagnostic kV x-ray beams, by using kQ and the PWDT phantom.

07 ISOTOPE AND RADIATION SOURCES↗

Modernization efforts for the R -Matrix code SAMMY [Abstract]

The R-Matrix code SAMMY is a widely used nuclear data evaluation code focused on the resolved range, which includes corrections for experimental effects. The code is still mostly written in Fortran 77, and uses a memory management system suitable for the time of its initial writing (1984). A modernization effort is under way to bring the code in-line with modern software development practices. A continuous-integration testing framework was added, automating the large existing set of test cases. It is run on every commit. The memory management was updated to current standard practices suitable for modern software analysis tools. The code can be obtained from https://code.ornl.gov/RNSD/SAMMY. The resonance parameters and covariance information are now stored in C++ objects shared by SAMMY and AMPX, the processing code that generates nuclear data libraries for SCALE. This allows for easier maintenance and access to the resonance parameters inside and outside of SAMMY. This feature is already used by accessing and changing parameters in memory in the Bayesian Monte Carlo Evaluation Framework for Cross Sections Nuclear Data and Integral Benchmark Experiments project, Further plans include the switch to the ENDF reading and writing routines in AMPX, as these routines are more robust, easier to maintain, and support more features. Of note here is support for the new GNDS format. Previously it wasn’t easy to share the full covariance matrix for evaluations containing more than one isotope due to limitations on the ENDF format; this is now supported in GNDS. The data are currently available in a binary SAMMY format and can be exported to GNDS to make them more widely available and sharable. The next step will be to use the same resonance processing code at 0K in AMPX and SAMMY as one of the available Reich-Moore R-Matrix formalism. The first step toward this goal is to isolate the reconstruction into a module that takes resonance parameters as its input and does not depend on SAMMY global parameters. This goal has been achieved and it should now be possible to more easily change the resonance formalism and add enhancements as the Phenomenological R-Matrix parameterization of direct, doorway, and compound nuclear reactions discussed elsewhere on this conference. This concerted modernization and enhancement effort provides multiple advantages to the nuclear data community. It will allow parameter optimization using enhanced formalisms, including experimental effects, that better match complex experimental data. Then those evaluated parameters can immediately be passed off to AMPX to be reconstructed with the exact same cross section model and be put into a data library for subsequent testing using SCALE and the Valid Benchmark suite or other suitable benchmark suites.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Validation of Jezebel Reactivity Coefficients and Sensitivity Analysis

Nuclear data validation is often performed today using criticality measurements. The gold standard for criticality measurements is the International Criticality Safety Benchmark Experiment Project (ICSBEP). The validation specifically focuses on the effective multiplication factor ($k_{eff}$). $K_{eff}$ is a relatively easy parameter to infer and has reduced uncertainty due to being at or above critical. However, while $k_{eff}$ is the most documented parameter and its uncertainties and sensitivities have been evaluated in great detail, it cannot be used as a standalone metric to determine inaccuracies in nuclear data (e.g., cross section data, PFNS, nu), which is based on theory, physics, and differential measurements. The Experiments Underpinned by Computational Learning for Improvements in nuclear Data (EUCLID) project aims to identify compensating errors in specific isotope nuclear data by optimally designing experiments that are, or are not sensitive to a suite of measurement parameters beyond $k_{eff}$. By identifying parameters that are sensitive to each other, oppositely sensitive, or have substantial magnitude differences in sensitivity, experiments can be designed to constrain questionable nuclear data. One sensitivity that is of particular interest to this project includes the sensitivity of reactivity coefficients. Reactivity coefficients compare reactivity, which is related to $k_{eff}$ at two different states therefore being sensitive to small changes in the system. The most common type of reactivity coefficient measurements is comparison to void for a small sample within the assembly. It is key that the sample sizes are small enough to not affect the flux of the full system. Reactivity coefficients were evaluated for many early experiments to better understand transport corrected cross sections. In fact, ICSBEP includes reactivity coefficient results as “Supplemental Measurements” in appendices for a handful of older benchmarks. One of those benchmarks is Jezebel, the bare Pu critical assembly. This paper compares new simulations of reactivity coefficients for Jezebel, and explores the sensitivity of reactivity coefficients to small changes in nuclear data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Developing And Scaling an OpenFOAM Model to Study Turbulent Flow in a HFIR Coolant Channel

Improving the understanding of how computational fluid dynamics (CFD) direct numerical simulations (DNS) of flows in the High Flux Isotope Reactor (HFIR) perform when run in parallel using the high performance computing (HPC) platform Summit at the Oak Ridge Leadership Computing Facility (OLCF) is of particular importance to boost the computational tools used to support HFIR conversion to low enriched fuel (LEU). Evaluation of scaling performance was driven by the increasing importance of graphics processing unit (GPU) usage in HPC, which is becoming the standard for modern supercomputers such as Summit. The desired results are to obtain a strong positive correlation between the computational resources dedicated to a problem and the relative speed-up of the simulation in comparison to a benchmark. This capability will allow substantially improvement in HFIR flow analytical capabilities, specifically when predicting turbulence properties at high Reynolds numbers. The study leverages previous simulation results performed with code PHASTA (finite element) on HPC platforms Cori (NERSC) and Theta (ALCF) [1] with computing options provided in the computing platform OpenFOAM (finite volume) at OLCF. Transitioning from PHASTA to OpenFOAM will (1) eliminate dependence on third-party software for mesh generation and manipulation, (2) reduce resource needs by employing modern architectures, and (3) build expertise for future modeling of HFIR-specific problems like heat transfer in involute geometry, entrance effects, flow structure in channel corners, and so on—all important issues when defining the available thermal margins in the transition to LEU. CPUs and GPUs differ significantly in their architecture and utilization, as discussed in the literature [2]. The most important differences are in the approach to computations and their memory. A single GPU contains a large quantity of cores, enabling it to perform with a much higher throughput than a CPU, but execution requires a different approach. GPU codes execute instructions using the Single-Instruction Multiple-Thread (SIMT) approach in which a single instruction is used for groups of threads called warps. A warp typically consists of 32 threads which must execute the same set of instructions, although on separate threads. Alternately, a CPU has far fewer cores that are much more flexible in their operation, excelling at quickly performing more complex serial computations. This is why GPUs have greater throughput when properly utilized. The second important difference is seen when comparing their memory spaces. Limited memory allocations and CPU–GPU communications cause a significant bottleneck in GPU-accelerated programs. Further study was required to properly take advantage of GPU resources. A comprehensive analysis of code performance and the model-specific features of turbulence constitutes the core of this work. In this study, a DNS simulation of HFIR channel turbulence was performed with the finite volume CFD code OpenFOAM v2112 and CUDA v11.0 on Red Hat Enterprise Linux v8.2. The OpenFOAM installation had AMGx integrated to enable GPU acceleration and utilizes the PETSc4FOAM library. The computational resources and the problem size were scaled on CPU and CPU + GPU architectures to gain a better understanding of the performance of a DNS problem on modern computing hardware. The study aimed to analyze the scaling of the code exclusively on CPUs and then to examine the scaling of the codes with GPU acceleration enabled. Scaling studies included CPU and GPU acceleration on a mesh of varying resolution to analyze the impact of problem size relative to computational resources. In the course of preparing the GPU configuration on Summit, mainly using the AMGX solvers, difficulties were encountered stemming from constant changes resulting from extensive ongoing development activities and the changing environment. This resulted in the inability to complete the GPU portion of the work. The code was compiled and tested, but production runs to assess acceleration were not performed because the used discretional compute time allocation expired as year-end approached. The Summit HPC platform is scheduled for decommissioning in 2024, making it unattractive for future use with Nvidia-based GPUs. Therefore, the work will be moved onto NERSC machines in FY24. An application was prepared and submitted, and sufficient node-hours were awarded to continue the research in the next calendar year. This report summarizes work performed thus far, which mostly focused on CPU OpenFOAM computing.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Sum-of-Fractions Method

Sum-of-fractions is a method intended to make sure a subcritical margin for aqueous solutions and slurries of fissionable isotopes exists. The method indicates that a system is subcritical if the sum of the ratios of the mass of each isotope (in a mixture) to its individual minimum subcritical mass limit is less than or equal to one. Historically, the basis of the sum-of-fractions has been derived from allowances given in the American National Standards Institute (ANSI)/ American Nuclear Society (ANS)-8.15-1981. However, the allowance was removed in ANSI/ANS-8.15-2014 due to a lack of technical basis. A methodology was developed to assess the validity of using the sum-of-fractions for water- or polyethylene-moderated systems for the following nuclides: 232U, 233U, 234U, 235U, 237Np, 236Pu, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, 241Am, 242mAm, 243Am, 242Cm, 243Cm, 244Cm, 245Cm, 246Cm, 247Cm, 249Cf, and 251Cf. The methodology uses available benchmark data for mixtures of 233U, 235U, and 239Pu to establish the calculational margin, and a mass limit reduction to establish the margin of subcriticality. Water- or polyethylene-moderated and -reflected mixtures containing the nuclides are evaluated with the code system, SCALE 6.2.4. Including the calculational margin, subcritical mass limits for each nuclide were computed for optimally water- or polyethylene-moderated and fully reflected systems. These masses were used to create nuclide mixtures in which the sum of the mass to subcritical mass limit ratios is one. The various nuclide mixtures were modeled over a range of moderation and demonstrate the keff does not exceed the calculational margin. For additional assurance of subcriticality, a significant mass reduction is applied to each computed minimum critical mass of the nuclides without adequate benchmark data consistent with the method in ANSI/ANS-8.15-2014.

criticality safety, Actinide↗

Exome resequencing and GWAS for growth, ecophysiology, and chemical and metabolomic composition of wood of Populus trichocarpa

Populus trichocarpa is an important forest tree species for the generation of lignocellulosic ethanol. Understanding the genomic basis of biomass production and chemical composition of wood is fundamental in supporting genetic improvement programs. Considerable variation has been observed in this species for complex traits related to growth, phenology, ecophysiology and wood chemistry. Those traits are influenced by both polygenic control and environmental effects, and their genome architecture and regulation are only partially understood. Genome wide association studies (GWAS) represent an approach to advance that aim using thousands of single nucleotide polymorphisms (SNPs). Genotyping using exome capture methodologies represent an efficient approach to identify specific functional regions of genomes underlying phenotypic variation. We identified 813 K SNPs, which were utilized for genotyping 461 P. trichocarpa clones, representing 101 provenances collected from Oregon and Washington, and established in California. A GWAS performed on 20 traits, considering single SNP-marker tests identified a variable number of significant SNPs ( p -value < 6.1479E-8) in association with diameter, height, leaf carbon and nitrogen contents, and δ 15 N. The number of significant SNPs ranged from 2 to 220 per trait. Additionally, multiple-marker analyses by sliding-windows tests detected between 6 and 192 significant windows for the analyzed traits. The significant SNPs resided within genes that encode proteins belonging to different functional classes as such protein synthesis, energy/metabolism and DNA/RNA metabolism, among others. SNP-markers within genes associated with traits of importance for biomass production were detected. They contribute to characterize the genomic architecture of P. trichocarpa biomass required to support the development and application of marker breeding technologies.

09 BIOMASS FUELS↗

Which nuclear data can be validated with LLNL pulsed-sphere experiments?

It is shown here that 14-MeV D+T LLNL pulsed-sphere experiments bring complementary information into the process of validating nuclear data compared to experiments that are traditionally used for this purpose—such as critical assemblies. To be more specific, the 14-MeV D+T LLNL pulsed-sphere neutron-leakage spectra enable to validate scattering and fission nuclear data up to 15 MeV (compared to approximately up to 5 MeV when using criticality experiments) and employ to this end simple compound targets containing only few isotopes. In this work, sensitivity profiles of the spectra to nuclear data are calculated in order to understand in detail which isotopes, observables, and energy ranges of nuclear data contribute significantly to their simulation. These profiles are presented for a few selected spheres containing 16 O, 12 C, 56 Fe, and 239 Pu. It is shown that the neutron-leakage spectra of spheres containing light elements are mostly sensitive to elastic- and inelastic-scattering cross sections on discrete levels and corresponding angular distributions. Spheres of structural materials are sensitive to elastic- and inelastic-scattering cross sections, including scattering on discrete levels and the continuum, and double-differential cross sections. Actinide spheres are also strongly sensitive to the fission observables, in particular to the total-fission neutron spectrum. Thin spheres (in which neutrons experience on average less than one scatter) are mostly sensitive to data near the elastic peak, in the energy range from 12–15 MeV, while thicker ones can be sensitive to data at lower incident-neutron energies due to multiple-scattering effects. This information is brought together with simulations of 71 pulsed-sphere neutron-leakage spectra using the ENDF/B-VII.1 and ENDF/B-VIII.0 nuclear-data libraries. This analysis highlights ENDF/B-VIII.0 data that could be further investigated for potential shortcomings ( 6 Li, 12 C, 16 O, 24-26 Mg, 27 Al, 48 Ti, 56 Fe, and 208 Pb) or are likely reliable ( 1,2 H, 7 Li, 9 Be, 14 N, 235,238 U, and 239 Pu) as indicated by validating with LLNL pulsed-sphere experiments.

14-MeV D+T LLNL pulsed-sphere neutron-leakage spec↗

Machine Learning to Select Experiments Driven by Fundamental Science and Applications for Targeted Nuclear Data Improvement

This work describes a blueprint for a process that accelerates progress in science by quantitatively answering the following question: What is the optimal combination of fundamental-science and application-driven experiments to maximally reduce pertinent data uncertainties? Answering this question entails solving a high-dimensional and complex optimization problem that is best solved with advanced statistic techniques often classified as machine learning. We apply this process within the framework of nuclear data with the aim to select an experiment combination that will reduce uncertainties in 239 Pu nuclear data for neutron energies between 1 and 600 keV. In this field, fundamental-physics driven data, called differential, look at one nuclear physics observable at a time. They are contrasted to application-driven, integral, data where one or few resulting values inform a broad set of nuclear data across several nuclides and energies. The candidates for integral experiments are criticality measurements that were refined by a genetic algorithm to be maximally sensitive to 239 Pu fission cross sections in the desired energy range. Twenty-three candidate differential experiments were investigated and span multiple nuclear physics observables (e.g., total, capture cross sections) for isotopes appearing in the integral experiments. The optimal combination among these candidate experiments was investigated via generalized least squares fitting, augmented with Gaussian processes to ameliorate statistical irregularities in data, and the D-optimality criterion. The latter evaluates for each pair of candidates the joint reduction in uncertainties of all 12200 nuclear data appearing in the integral experiments compared to the knowledge we have from 168 past experiments, theory, and nuclear data. We chose as differential measurements those that investigate 63 Cu and 239 Pu total cross sections, based on D-optimality rank and feasibility constraints. Two integral (criticality) experiments were selected: An experiment with Al 2 ⁢O 3 and graphite interleaved with Pu and a thick Cu reflector explores 1–30 keV, while we target the 30–600 keV range with an experiment that swaps boron in place of graphite with a different geometry.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗