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Laboratory Directed Research and Development Program Activities (LDRD 2021 Annual Report)

Each year, Brookhaven National Laboratory (BNL) is required to provide a report of its completed Laboratory Directed Research and Development Program (LDRD) projects to the Department of Energy (DOE) Office of Scientific and Technical Information in accordance with DOE Order 413.2C Chg1 (MinChg) dated August 2, 2018. This report provides a detailed look at the scientific and technical activities for each of the LDRD projects funded by BNL in FY 2021, in fulfillment of that requirement. In FY 2021, the BNL LDRD Program funded 68 projects, 24 of which were new starts, at a total cost of $17.1M. The investments that BNL makes in its LDRD program support the Laboratory’s strategic goals. BNL has identified six scientific initiatives that define the Laboratory’s scientific future and that will enable it to realize its overall vision. This requires simultaneous excellence in all aspects of BNL’s work – from science and operations, to external partnerships with the local, state, and national communities, and beyond. This is enabled by safe, efficient, and secure operations; by an unwavering commitment to a diverse, equitable, and inclusive environment, including workforce development, both with staff and reaching out to the community; and by a strong focus on renewed infrastructure. The six scientific initiatives are: (1) Nuclear Physics: The Electron Ion Collider, (2) Clean Energy and Climate, (3) Quantum Information Science and Technology, (4) Discovery Science Driven by the Human-AI-Facility Integration, (5) High Energy Physics: Building for Discovery, and (6) Accelerating Isotope Production: Ensuring the Nation’s Supply is Secure. The funded projects support BNL’s six scientific initiatives and priority programs as well as new areas of research and competencies at the Laboratory that are consistent with the Laboratory’s vision and mission. In total, these LDRD investments supported 80 postdoctoral researchers and graduate students in whole or in part and resulted in 136 publications and 3 awards. This Program Activities Report represents the future of BNL science; it is an impressive body of exploratory work that investigates many scientific and technical directions in support of the DOE and BNL missions.

07 ISOTOPE AND RADIATION SOURCES↗

Complex software dedicated for design and simulation of LPCE process for heavy water detritiation

The main purpose of this paper is to present a comprehensive software, SICA, designed to be used in water-hydrogen liquid phase catalytic exchange process (LPCE). The software calculates the water-gas catalytic isotopic exchange process, following the transfer of any H, D or T isotope from water to gas and vice versa. This software is useful for both design and laboratory-based research; the type of the catalytic filling (ordered or random) can be defined for any of these 2 cases, the isotopic calculation being specific to the package type. For the laboratory-based research, the performance of a catalytic packing can be determined by knowing the type and by using experimental results. Performance of the mixed catalytic packing is defined by mass transfer constants for each catalytic and hydrophilic package in that specific arrangement, and also for the isotope whose transfer is studied from one phase to another. Also, it has been established a link between these constants and commonly used parameters for the fillings performance defined by HETP (Height Equivalent of Theoretical Plate). To demonstrate the performance of the software, we present a comparative analysis of water-gas catalytic isotopic exchange on a column equipped with 3 types of filling: successive layers, random and structured (ordered package filled with catalyst). The program can be used for the LPCE process calculation, process used at detritiation facilities for CANDU reactors or fusion reactors. (authors)

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Comparison of Light-Weight Radioisotope Heater Unit (LWRHU) Historical Testing to Special Form Testing Requirements

This paper compares the Light-Weight Radioisotope Heater Unit (LWRHU) historical testing to Department of Transportation (DOT) Special Form criteria per 49 CFR Part 173, Shippers-General Requirements for Shipments and Packages, Section 469, Tests for special form Class 7 (radioactive) materials as specified in DOE-STD-1027, Hazard Categorization of DOE Nuclear Facilities. Compliance with the aforementioned criteria allows for the exclusion of radioactive sources from the facility’s nuclear material inventory. As part of a new program at Los Alamos National Laboratory (LANL), LWRHUs are planned to be moved into TA-55, PF-5 Power Source Assembly Area (PSAA) for assembly and testing activities. The PSAA Facility is categorized as a low hazard, non-nuclear facility per DOE STD-1027 and is described in TA55-PF-5-FHC-11-001, Facility Hazard Categorization of the PSAA at PF-5, TA-55. The Facility Hazard Categorization document states, there must be documentation that radioactive sources are engineered to pass the special form testing specified by DOT in 49 CFR 173.469, Tests for special form Class 7 (radioactive) materials or ANSI N43.6, Sealed Radioactive Sources - Classification. This paper documents the extensive historical environmental safety testing of the LWRHU and demonstrates its ability to survive potential launch safety accident scenarios. The testing results are used herein to demonstrate through a comparative analysis that the robust design of the LWRHU meets or exceeds the special form testing specifications in 49 CFR 173.469, enabling the LWRHU to be transported and handled in PF-5 in support of testing and assembly program.

07 ISOTOPE AND RADIATION SOURCES↗

National‐Scale Assessment of Total Gaseous Mercury Isotopes Across the United States

Abstract With the 2011 promulgation of the Mercury and Air Toxics Standards by the U.S. Environmental Protection Agency, and the successful negotiation by the United Nations Environment Program of the Minamata Convention, emissions of mercury (Hg) have declined in the United States. While the declines in atmospheric Hg concentrations in North America are encouraging, linking the declines to changing domestic and global source portfolios remains challenging. To address these research gaps, the U.S. Geological Survey initiated the first national‐scale effort to establish a baseline of total gaseous mercury stable isotope values at 31 sites distributed across the United States. Results indicated that unique Hg sources, such as Hg evasion from an elemental Hg contaminated site or free tropospheric intrusions in high altitude sites, were distinguishable from background atmospheric values. Minor gradients were observed across the nation, with regions of heavy industrial activity demonstrating lower δ 202 Hg, but no consistent changes in other isotopes such as Δ 199 Hg and Δ 200 Hg were observed. Furthermore, δ 202 Hg was impacted by foliar uptake and senescence but trends varied between forested regions in the northeastern and midwestern United States. These data demonstrate regional emission sources and other environmental variables can impact total gaseous Hg (TGM) isotope values, highlighting the need to characterize atmospheric Hg isotopes over larger geographical areas to evaluate changes related to national and international Hg regulations.

Tate, Michael T.↗

Developing a Facility NMAC Plan

The table presented below suggests the basic information that should be covered in a facility NMAC Plan for an NMAC program that is designed for nuclear security. The topics are appropriate for and should be addressed by all facilities in their NMAC Plans. They are appropriate for NMAC Plans for nuclear power plants, research reactors, fuel manufacturing facilities, facilities that produce medical isotopes, and other facilities. The difference is in the intensity with which the various measures are applied and the thoroughness of the description of the application (i.e., the program requirements). The robustness of a facility NMAC program and the content of its NMAC Plan should be graded in accordance with the type of facility and the category of its nuclear material.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Post-irradiation Examination of Eurofer-97 Steel Irradiated to 20 dpa at 200–400°C in HFIR under the EUROfusion (ORNL-KIT) Collaboration Program

The Oak Ridge National Laboratory/Karlsruhe Institute of Technology (ORNL/KIT) collaboration focuses on research involving irradiation experiments and post-irradiation examinations (PIE) of isotopically modified Eurofer-97 steels for fusion reactor applications. This collaboration capitalizes on ORNL’s expertise in radiation effects on materials and its capabilities in irradiation and PIE. The research aims to qualify Fe-9Cr-based Eurofer-97 steel under simulated fusion conditions, which include high doses and high transmutation rates. A unique isotopic modification technique is utilized in the research, wherein high-transmutation isotopes such as Fe-54 and Ni-58 are alloyed into the Eurofer steel to align with the expected helium production rates in fusion reactor conditions. This report presents the results of post-irradiation mechanical testing activities for the EUROFER-97/2 specimens after irradiation to ~20 dpa at various irradiation temperatures. The irradiation doses and temperatures for the ES capsules ranged from 18.4–20.4 dpa and 202–256°C, respectively. The mechanical property datasets, obtained through baseline testing and PIE of the tensile and fracture specimens, include microhardness data from 93 irradiated and non-irradiated tensile specimens and 28 irradiated bend bar specimens, uniaxial tensile property data from 45 irradiated and non-irradiated tensile specimens, and fracture toughness data from the bend bar specimens. Further data analyses provide statistical information on the microhardness values and tensile properties, as well as the reference ductile-brittle transition temperature (T 0 ) data.

36 MATERIALS SCIENCE↗

Proceedings for the Workshop on Applied Nuclear Data Activities 2024

The Workshop for Applied Nuclear Data Activities (WANDA) is designed to increase communication among nuclear data (ND) users in multidisciplinary federal programs, ND producers, ND funders, and other ND experts. It also presents an opportunity to cross-pollinate ideas as well as introduce ND gaps identified by federal programs to ND experts and ND capabilities to the various federal ND users. WANDA 2024 included five technical sessions, three of which focused on Fusion Energy Sciences (FES)—FES Fusion Neutronics, FES Tritium Production, and FES Material Damage—and two stand-alone sessions—Isotopes and Targetry for Nuclear Data and Uncertainty Quantification. The FES sessions successfully brought new voices to the WANDA discussions, expanding the application space in which nuclear data are critical. FES programs need accurate nuclear data with realistic uncertainty quantification to properly estimate, for example, shielding, activation, tritium production, helium production, structural material integrity, and superconducting magnet operation. This includes a variety of projectile (neutrons, photons, charged particles) and target atoms. One of the action items common to all the FES sessions was a need to perform sensitivity studies to identify the prioritization of nuclear data needs. The Isotopes and Targetry session highlighted the many capabilities available to produce high-quality targets for nuclear data measurements, including 3D printing with spherical powders, combustion synthesis coupled with spin coating & electrospraying, inkjet printing, and isotopic doping. These new methods open doors for more accurate measurement, but it was also stressed that sample characterization following any method of fabrication is of the highest importance to accurately interpret nuclear data measurement results that used that sample. The Uncertainty Quantification (UQ) session was broken into two categories: nuclear data uncertainty quantification and the use of that uncertainty quantification. Thematic to the UQ session was the loss of information when going from nuclear data measurement, to evaluation, to evaluated file, and finally to neutron transport calculations. Current evaluated ND libraries typically only contain covariances, which assume that the probability distributions are Gaussian. Beyond being a simplified assumption for many evaluations, this can lead to negative values on many observables when attempting to sample the covariance. The covariance format, however, is very efficient in that a simple set of linear equations can transform uncertainty from parameters or cross sections to the application of interest. Focused collaboration is needed between nuclear data evaluators and nuclear data users to ensure that needs are being met.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Fluid geochemistry at the Raft River geothermal field, Idaho, USA: New data and hydrogeological implications

Following a period of exploration and development in the mid-late 1970’s, there was little activity at the Raft River geothermal field for the next ~20 years. U.S. Geothermal Inc. acquired the project in 2002, and began commercial power generation in January 2008. From mid-2004 to present, U.S. Geothermal Inc. has collected geochemical data from geothermal and monitoring wells in the field, as well as other shallow wells in the area. An additional sampling program was completed in July 2010 to measure a wider range of trace elements and key water isotopes (δ 18 O, δD, and 3 H (Tritium)) in the field. The data indicate that the fluid geochemistry in the field is spatially variable and complex, with two distinct deep geothermal fluid types (high vs. low K, Na, Cl, Ca, Li, F concentrations) and two groundwater fluid types. These differences have been interpreted to reflect deep structural controls on fluid pathways in the field, which has compartmentalized the fluids and limited the degree of mixing between them.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Understanding the effect of specimen size on the properties of fine-grain isotropic nuclear graphite for irradiation studies: Mechanical properties

Programs at Oak Ridge National Laboratory are investigating the effects of neutron irradiation in the High Flux Isotope Reactor (HFIR) on properties of fine-grain isotropic nuclear graphites. Specimens were irradiated in the HFIR flux trap, which requires using specimens that are smaller than the sizes recommended by ASTM standards. Here, this work has investigated whether subsized specimens can be used to reliably predict strength behavior. The results show that (1) tensile strength was loosely coupled to specimen volume, (2) the compression specimens had a slightly higher strength for larger volumes, (3) the uniaxial flexural strength was nearly independent of specimen effective area for one orientation whereas the other orientation showed a slight strength–size scaling Weibull behavior, and (4) equibiaxial flexural strength followed traditional strength–size scaling Weibull behavior. These results suggest that fine-grain graphite is more similar to ceramics than to medium- and large-grained graphite with respect to both the strength-limiting flaws (Griffith theory) and the effect of machining on the strength behavior. This work shows that using specimens that are smaller than ASTM recommendations are suitable for investigating the strength changes caused by neutron irradiation because the primary interest is the relative change in the strength distribution parameters rather than their absolute values.

36 MATERIALS SCIENCE↗

Understanding the effect of specimen size on the properties of fine-grain isotropic nuclear graphite for irradiation studies: Physical, electrical, thermal properties

Programs at Oak Ridge National Laboratory are investigating the effects of neutron irradiation in the High Flux Isotope Reactor (HFIR) on properties of fine-grain nuclear graphites. Specimens were irradiated in the HFIR flux trap, which required using specimens that are smaller than the sizes recommended by ASTM standards. Here, this work has investigated whether subsized specimens can be used to reliably determine the measured physical (density, elastic moduli, and electrical resistivity) and thermal properties (coefficient of thermal conductivity and thermal conductivity). The results show the specimen sizes in this investigation had a minimal influence on any of the measured properties. Even for the properties where size influenced the measured value (density and thermal conductivity), an explanation is provided, and the consequences can be accounted for in post-irradiation results. This work demonstrated that using subsized specimens for physical and thermal property measurements is suitable when necessary for fine-grain isotropic graphite.

36 MATERIALS SCIENCE↗

Baseline Hypothetical Facility for the Production of 131 I and 99 Mo using Activation Targets

This report describes a hypothetical facility for production of medical radioisotopes via activation under the Proliferation Resistance and Optimization (PRO-X) program. The facility uses neutron activation of non-special nuclear material (SNM) to produce the medical isotopes 131 I and 99 Mo at a throughput of 60 Ci/week of 131 I and 5 Ci/week of 99 Mo. The hypothetical design was carried out using a 10 MWt research reactor. The precursors used for the activation process were TeO2 for 131 I and MoO 3 for 99 Mo. The processes are performed in 3 hot cells used for target receipt, extraction, purification low specific activity (LSA) generator introduction, and packaging. A fourth hotcell is used for waste processing. The hot cell processing area takes up a footprint of 15.4 m 2 with the total footprint of the facility, including space for administrative offices, non-rad labs, quality assurance, and radiation buffer areas set at 763 m 2 . Waste is produced at a weekly rate of 257.8 g low activity solid waste and 8032.7 mL of low activity liquid waste, 8032 mL of which is water. This baseline hypothetical facility for production of medical isotopes via activation was then compared and contrasted to the hypothetical facility for production of medical isotopes via fission products to show the differences in approach for the two production modes. The two production modes had several highlighted differences including the overall facility and hot cell layout, the type and amount of waste produced by the respective facilities, and economic factors impacting production mode. Finally, a decision tree for which production mode might be more beneficial for an entrant into medical isotope production was developed based on the differences examined and the desired output of medical isotopes desired by the entrant.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Characterization of Fresh Nuclear Fuel using Time-Of-Flight Neutrons

Neutrons offer excellent characterization capabilities for nuclear fuels and can provide non-destructive insight on micro structure, chemistry and crystallographic phase. Measurements are possible at reactors or pulsed sources, but the inherent energy resolution implicit at pulsed sources offers unique opportunities. Recent advances in 2D neutron detection enabled new capabilities of material characterization using neutron imaging and tomography for nuclear materials. Moreover, time-of-flight (TOF) neutron measurements can enable isotope specific tomography by deriving isotope densities from transmission spectra exhibiting neutron resonances, which are recorded for each pixel. Tomographic algorithms allow 3D reconstructions of the spatial distribution of isotopes, density and features in typical fuel pellet samples. The ability to select radiographs for different energies allows characterizing samples which are opaque for thermal neutrons, such as enriched fuels or fuels containing plutonium, by selecting epi-thermal neutron energies and by knowledge of the total neutron cross sections of the constituents, isotopic enrichment levels can be determined. Nuclear cross sections are typically not calculated directly and databases such as the Evaluated Nuclear Data File (ENDF) database provide this information with cross sections determined by standardized experimental measurements, such as neutron transmission measurements for individual isotopes. Utilizing the information in the ENDF database, the 'inverse' problem can be solved by assuming cross section parameters to be known parameters and areal densities can be determined. This work presents recent advances at the Los Alamos Neutron Science Center (LANSCE) facility at Los Alamos National Laboratory (LANL), which provides the infrastructure to handle radioactive samples, in the development of fuel characterization with TOF neutrons. Examples include recent work on prototype accident tolerant nuclear fuels (ATF). The potential application of these techniques for nondestructive examination of irradiated fuel is under consideration. Non-destructive access to materials features for specimens embedded in containers, particularly for hazardous samples, such as a radioactive nuclear fuel, is indispensable to characterize and ultimately license new fuel forms. Energy-resolve neutron imaging is a new tool for this research field. The results reported here present a new imaging technique, setting a milestone in the capabilities of measuring non-destructively absolute quantities of physical properties. The enabling physics behind this new technique are nuclear resonances. We have demonstrated how absolute areal densities can be extracted from radiographs utilizing pulsed neutron sources. This technique provides information that is otherwise difficult and costly to obtain. In the case of nuclear fuels, the results from energy-dispersive neutron imaging may guide destructive examination of irradiated fuel. This summery does not describe recent analysis, which is ongoing. Particularly, the implementation of calibration standards has improved the determination of enrichment levels without additional calibration. The analysis of the samples was performed with full tomographic reconstructions for isotope specific data and presents a first approach in absolute isotope specific 3D reconstruction. This work was predominantly funded by and received substantial support from the Fuel Cycle R and D program at Los Alamos National Laboratory. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Measurement of isotopic separation of argon with the prototype of the cryogenic distillation plant Aria for dark matter searches

The Aria cryogenic distillation plant, located in Sardinia, Italy, is a key component of the DarkSide-20k experimental program for WIMP dark matter searches at the INFN Laboratori Nazionali del Gran Sasso, Italy. Aria is designed to purify the argon, extracted from underground wells in Colorado, USA, and used as the DarkSide-20k target material, to detector-grade quality. In this paper, we report the first measurement of argon isotopic separation by distillation with the 26 m tall Aria prototype. We discuss the measurement of the operating parameters of the column and the observation of the simultaneous separation of the three stable argon isotopes: ${}^{36}\hbox {Ar}$, ${}^{38}\textrm{Ar}$, and ${}^{40}\textrm{Ar}$. We also provide a detailed comparison of the experimental results with commercial process simulation software. This measurement of isotopic separation of argon is a significant achievement for the project, building on the success of the initial demonstration of isotopic separation of nitrogen using the same equipment in 2019.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

SU-E-T-234: Modulated Photon Radiotherapy (XMRT):The Impact of Incorporating Energy Modulation Into Intensity Modulated Radiotherapy (IMRT) Optimization

Purpose: To develop a new radiotherapy plan optimization technique that, for a given organ geometry, will find the optimal photon beam energies and fluences to produce a desirable dose distribution. This new modulated (both in energy and fluence) photon radiotherapy (XMRT) was compared with intensity modulated radiotherapy (IMRT) for a simple organ geometry. Methods: The XMRT optimization was formulated using a linear programming approach where the objective function is the mean dose to the healthy organs and dose-point constraints were assigned to each organ of interest. The organ geometry consisted of a target, two organs at risk (OARs), and normal tissue. A seven-equispaced-coplanar beam arrangement was used. For conventional IMRT, only 6 MV beams were available, while XMRT was optimized using 6 and 18 MV beams. A prescribed dose (PD) of 72 GY was assigned to the target, with upper and lower bounds of 110% and 95% of the PD, respectively. Both OARs were assigned a maximum dose of 64 Gy, while the normal tissue was assigned a maximum dose of 66 Gy. A numerical solver, Gurobi, generated solutions for the XMRT and IMRT problems. The dose-volume histograms from IMRT and XMRT solutions were compared. Results: The maximum, minimum, mean, and homogeneity of the dose to the target were comparable between IMRT and XMRT. Though IMRT had improved dose conformity relative to XMRT, XMRT reduced the mean dose to both OARs by more than 1 Gy. For normal tissue, an increase of 5 Gy in mean dose and 27 percent in integral dose was seen for IMRT relative to XMRT. Conclusion: This work demonstrates the benefits of simultaneously modulating photon beam energy and fluence using our XMRT approach in a given phantom geometry. While target coverage was comparable, dose to healthy structures was reduced using XMRT.

07 ISOTOPE AND RADIATION SOURCES↗

140,142 Cerium Resolved Resonance Region Evaluation [Slides]

The presentation covers an overview of 140,142 Ce Isotopes, including new evaluations of 140,142 Ce that were requested by the Hanford Plutonium Finishing plant to the Nuclear Criticality Safety Program. It also discusses current ENDF/B-VIII.0 evaluation, which has an error in the 1-2 keV range. It was evaluated using multi-level Breit-Wigner and 142Ce has room for extending resolved resonance region current upper limit from 13 keV. The presentation also discusses new transmission and capture measurements of nat Ce and 142 Ce from Klaus Guber. It also states that no known integral experiments prominently feature Cerium.

07 ISOTOPE AND RADIATION SOURCES↗

Advanced Multiphysics Thermal-Hydraulics Models for the High Flux Isotope Reactor

Engineering design studies to determine the feasibility of converting the High Flux Isotope Reactor (HFIR) from using highly enriched uranium (HEU) to low-enriched uranium (LEU) fuel are ongoing at Oak Ridge National Laboratory (ORNL). This work is part of an effort sponsored by the US Department of Energy (DOE) Reactor Conversion Program. HFIR is a very high flux pressurized light-water-cooled and moderated flux-trap type research reactor. HFIR s current missions are to support neutron scattering experiments, isotope production, and materials irradiation, including neutron activation analysis. Advanced three-dimensional multiphysics models of HFIR fuel were developed in COMSOL software for safety basis (worst case) operating conditions. Several types of physics including multilayer heat conduction, conjugate heat transfer, turbulent flows (RANS model) and structural mechanics were combined and solved for HFIR s inner and outer fuel elements. Alternate design features of the new LEU fuel were evaluated using these multiphysics models. This work led to a new, preliminary reference LEU design that combines a permanent absorber in the lower unfueled region of all of the fuel plates, a burnable absorber in the inner element side plates, and a relocated and reshaped (but still radially contoured) fuel zone. Preliminary results of estimated thermal safety margins are presented. Fuel design studies and model enhancement continue.

COMSOL↗

Delayed Critical and Subcritical Experiments with Polyethylene Moderated Unreflected Thin 15 in. Diameter HEU Metal Plates

The thin ~15 in. diameter highly enriched uranium (HEU) metal plates were assembled to delayed criticality at the Oak Ridge Critical Experiments Facility (ORCEF) in 1969 with various thicknesses of polyethylene (varying from 1/16 to 2$\frac{3}{8}$ inches) between uranium metal plates. The average 235 U enrichment was 93.27 wt. %. These unreflected critical configurations contained 4$\frac{2}{3}$ to 20$\frac{5}{6}$ thin 15 in. diameter HEU metal plates (on loan from Los Alamos National Laboratory [LANL] and shipped to Oak Ridge National Laboratory [ORNL] on June 3, 1969). Depending on the thickness of polyethylene, the enriched uranium masses varying from 28,053 to 135,148 grams. Fractional plate sections consisted of the appropriate number of 60° pie sections. In addition to the measurement at delayed criticality, subcritical measurements were also performed by the inverse kinetic rod drop method. Prompt neutron decay constant measurements were also performed by the Rossi alpha and randomly pulsed neutron method using a time-tagged spontaneous fission californium neutron source; these are briefly reported here. At the time of these measurements in 1969, the thin HEU metal plates were in near-pristine condition with extremely little oxidation, allowing better descriptions of the uranium plates than the use of these plates in a heavily oxidized and deteriorated condition in recent reflected benchmark experiments at the LANL facility at the Nevada Test Site with these same thin highly enriched uranium metal plates. This report documents the experimental information for the measurements performed so that later researchers can perform the required uncertainty and calculational analyses and documentation to use these data for an International Nuclear Criticality Safety Benchmark Evaluation Program (ICSBEP) or a Nuclear Energy Agency (NEA) benchmark. Data from the experiments described should be acceptable for use as criticality safety benchmark experiments for the ICSBEP and the NEA nuclear criticality safety benchmark program once the uncertainty analysis on the measured neutron multiplication factors is completed. Additional data—such as the dimensional inspection reports, uranium isotopic information, and other relevant particulars—should be retrieved from the Y-12 Plant or LANL and incorporated in the final ICSBEP benchmark. Based on previous ICSBEP benchmarks with this enriched uranium metal at ORCEF, the uncertainties in $k_{eff}$ could be as low as ± 0.0002 for some configurations. Other experiments with smaller-diameter than 15 in. diameter HEU metal plates have been benchmarked in HEU-METFAST-001. The prompt neutron time decay measurements could be the basis for an International Reactor Physics Benchmark Program. Preparation of the present report is part of an effort at ORNL to document more than 15 undocumented critical and subcritical experiments enumerated in ORNL/TM-2019/18 and performed by ORNL at ORCEF and other US Department of Energy critical experiments facilities using more than 500 operational days of critical facility time. This work for this report publication was supported by the Nuclear Criticality, Radiation Transport and Safety NCSP Program at ORNL.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Improvements to the operational efficiency of the Portsmouth 'Blue Box' Assay system - 15162

The 'Blue Box' in Building 326 at Portsmouth comprises a dual cargo container lined with high density polyethylene with 5% (elemental) boron that acts as a neutron shield. This construction provides a low environmental neutron background to support the capability to attain low values of minimal detectable activity (MDA). A Non-destructive Assay (NDA) measurement platform known as the Fluor B and W Portsmouth Slab Counter (FBPSC) is housed inside the Blue Box. This comprises four neutron slab detectors supported with an electronic system supplying power and associated signal processing. The system is operated by a laptop computer which has data acquisition and analysis capabilities. Each slab contains five {sup 3}He proportional counters embedded in polyethylene. The system is designed to measure the mass of U-235 in coolers from the Portsmouth site using passive neutron counting. The system was calibrated by taking measurements with {sup 252}Cf sources attached to various positions on the outside surfaces of a surrogate cooler. In addition, Monte-Carlo N-Particle (MCNP) simulations were performed to extend the baseline calibration for coolers of various sizes used in the gaseous-diffusion process. The basic principle of operation is to measure the total neutron emission from the item and determine the mass of {sup 235}U using the system efficiency (determined from MCNP calculations combined with the calibration measurements) combined with known isotopic information ({sup 235}U enrichment and U-235/U-234 ratio), assumed chemical composition, and gross cooler mass. The FBPSC analysis program calculates the mass of U-235 within the cooler being assayed, together with the associated Total Measurement Uncertainty (TMU). A background correction is performed that accounts for the measured environmental background with a cosmic-ray spallation correction (based on the cooler's gross weight). The software suite developed for the system also includes the capability to track and trend measurement control data in order to quickly identify conditions where the system has drifted outside of its quality control envelope. The MDA of the system has been determined to be less the 15 g of U-235 for count times that are typically less than 5 minutes (depending on the uranium isotopics). This is primarily the result of the low neutron background rate inside the Blue Box (approximately 3 times lower than at nearby locations outside the box). Additionally, various software features have been designed to yield optimum counting performance for the system including count time adjustment and interval filtering to reject statistical outliers that are usually associated with cosmic spallation events. The operation of the system has proven to be very efficient, with the short measurement time providing a high throughput rate of coolers through the Blue Box NDA system. Significant operational benefits and improved data traceability have been yielded compared to the previous measurement process, which involved operators taking measurement with counter/scalers and manually entering data into spreadsheets. As of August 2014, this system successfully measured all coolers required to support completion of a contractually-required Performance Milestone. There are approximately 1900 coolers available for measurement. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗