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Experiment Design and Preparation for a Shielding Benchmark Utilizing Godiva-IV

An experiment is currently being designed to provide a high-quality shielding benchmark for Criticality Accident Alarm System (CAAS) modeling. Previous benchmarks have suffered from uncertainty primarily due to two factors. The first factor is radiation that is not directly coming from the source, also known as room return. Room return is notoriously difficult to account for in experimental data and to model in benchmarks. The second factor is uncertainty associated with the source term itself. In order to reduce these two sources of uncertainty, this experiment will utilize a room return shield [1] that will reduce the effect of room return and previous work performed to ensure the reproducibility of the source term. The experiment will use the Godiva IV [2] assembly located at the National Criticality Experiments Research Center (NCERC) to provide a neutron source representative of a criticality accident. Previous experiments [3]-[4] have shown that Godiva IV is capable of producing both bursts and steady-state emissions of equal magnitude which will allow for reduced uncertainty in the source term. The room return shield will house and isolate the shielding samples, neutron activation foils, and other detectors. Data collected will provide a comparison of the neutron and gamma dose for shielded and unshielded configurations. This data will be used to validate shielding data used for modeling criticality accident alarm systems. Shielding samples included in this benchmark are C, Fe, NaCl, Pb, high density polyethylene, and SiO 2 . This paper details the design of the room return shield, the experimental plan, challenges, and mitigation strategies.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

International Intercomparison for Nuclear Accident Dosimetry Using Godiva-IV

During the week of August 22, 2022, Integral Experiment Request (IER) 538, an international blind intercomparison for nuclear accident dosimetry (NAD) exercise, was completed using the Godiva-IV critical assembly at the National Criticality Experiments Research Center (NCERC) located in the Device Assembly Facility (DAF) at the Nevada National Security Site (NNSS). This exercise builds upon a series of experiments that include the characterization the radiation fields around Godiva (IER-147) and Flattop (IER-252) and follow up intercomparisons of dosimetry around both Godiva IV and Flattop (IER-148 and IER-253, respectively). The participants consisted of seven Department of Energy laboratories and one laboratory each from the US Navy, United Kingdom, and France. The participants of the exercise were Lawrence Livermore National Laboratory (LLNL); Los Alamos National Laboratory (LANL); Sandia National Laboratory (SNL); Savannah River Site (SRS); Hanford Site, Missions Support and Test Services (MSTS); Y-12 National Security Complex (Y-12); Naval Dosimetry Center (NDC); Atomic Weapons Establishment (AWE); and Institut de Radioprotection et de Sûreté Nucléaire (IRSN). MSTS dosimeters were included in the irradiations but not reported for evaluation. This report primarily discusses the performance of the 24 hour results submitted by participants, though available final results are briefly discussed. Information for each irradiation performed is provided for participating laboratories to produce their own final report which will be incorporated into the CED-4a report.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

National Criticality Experiments Research Center (NCERC) - capabilities and recent measurements

The National Criticality Experiments Research Center (NCERC) located at the Device Assembly Facility (DAF) at the Nevada National Security Site (NNSS) and operated by Los Alamos National Laboratory (LANL) is home to four critical assemblies which are used to support of range of missions, including nuclear criticality safety and nuclear nonproliferation. Additionally, subcritical systems can also be assembled at NCERC. NCERC is providing critical and subcritical experiments valuable to the nuclear data community and experiments performed at NCERC are often published as benchmarks in the International Criticality Safety Benchmark Evaluation Project (ICSBEP) Handbook. This manuscript will give a broad overview of recent experiments performed at NCERC, upcoming experiments, and why integral measurements are important and useful to the nuclear data community. The four critical assemblies are GODIVA IV, FLATTOP, COMET, and PLANET. GODIVA IV is a cylindrical metal fast burst reactor, the fourth in the GODIVA series that dates back to the 1950’s. FLATTOP is an highly enriched uranium (HEU) or Pu core reflected by natural uranium. COMET and PLANET are vertical lift assemblies, where one half of the reactor can be lifted to the upper half of the reactor to create a critical system. Some recent experiments include various critical intermediate energy assemblies with lead, and subcritical measurements of plutonium reflected by copper, tungsten, and nickel. Work is also underway to make a better measurement of the critical mass of neptunium, using a neptunium sphere surrounded by nickel shells. Additionally, measurements will be performed next year with HEU shells from Rocky Flats. These HEU shells will be stacked together to make larger systems, allowing for a large range of criticality (from subcritical to delayed critical). Other upcoming measurements include an HEU critical assembly sensitive to intermediate energy neutrons.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Godiva-IV Dosimetry Exercise 2022 Preliminary Results

Integral Experiment Request (IER) 538 is part of a series of dose characterization and nuclear accident dosimetry (NAD) exercises performed under the Department of Energy (DOE) Nuclear Criticality Safety Program (NCSP). This is the second NAD exercise using the Godiva-IV critical assembly and the third NAD exercise overall. The participating laboratories provided their own dosimeters that were mounted on the Lawrence Livermore National Laboratory (LLNL) BOttle Manikin ABsorption (BOMAB) phantoms and aluminum plates. The BOMABs and plates were placed at two, three, and four meters away from the center of Godiva. Alongside the NADs, there was a LLNL Passive Neutron Spectrometer (PNS), Atomic Weapons Establishment (AWE) PNS, and Y-12 Sphere present to measure the neutron dose from Godiva. Two irradiations were conducted to test the NAD performance from each laboratory and assesses their performance to the DOE-STD-1098-2017 part 515 criteria. Neutron and gamma doses were measured prior to this exercise. This work presents a model for the neutron and gamma dose respectively to serve as the reference value. A code written in C/C++/ROOT was used to fit the measured neutron and gamma dose with the new models. It was assumed that the neutron and gamma doses are proportional to the change in temperature of Godiva after a burst irradiation. Uncertainties for the reference values were calculated using error propagation of the model’s parameters. Preliminary results (within twenty-four hours) and final results were compared for each laboratory. On average of all the participating laboratories, 32% of neutron doses and 78% of gamma doses were outside the DOE standards. One laboratory did not report their dose readings and were not included in this average. There is a bias for a lower neutron dose and a higher gamma dose based on the distribution of results. In comparison with the past Godiva-IV NAD exercise, there is an improvement in neutron dose readings by 20%.

BOttle Manikin ABsorption (BOMAB)↗

Improved Cumulative Fission Yield Measurements with Fission Spectrum Neutrons on 238U

Two isotopically-characterized targets of high-purity (99.961±0.002%) 238U metal and a neutron dosimetry package were exposed to a pulsed neutron irradiation using the Godiva IV critical assembly at the National Criticality Experiments Research Center to measure the integral fission product yields produced in a Watt fission neutron-energy spectrum. Following irradiation, the fissioned targets were counted with two broad energy germanium detectors. Estimates of the total fissions for each target were made using measurements of well-known fission products. The total number of fissions in each target were then used to measure the fission yields of 33 fission products, 18 of which are published as new measurements. Twelve of the 18 isotopes were in agreement with ENDF/B- VIII.0 using the zeta test and treating ENDF/B-VIII.0 as the true mean: 84mBr, 93Y, 94Y, 104Tc, 134I, 135I, 138Xe, 141Ba, 142Ba, 142La, 146Ce, and 149Nd. The ENDF/B-VIII.0 fission yield for 139Ba was only slightly outside of 1-s relative to the uncertainty measured in this work. Uncertainties for 5 fission product yields were markedly improved over those reported in ENDF/B-VIII.0: 128Sn, 129Sb, 130gSb, 131mTe, and 133I. The fission yields measured for 128Sn, 131mTe, and 133I were in good agreement with the ENDF/B-VIII.0 predicted fission yields. However, fission yields measurements of the isotopes 129Sb, and 130gSb deviated from the ENDF/B-VIII.0 value. Both of these isotopes reside near the doubly magic nuclear shell closures of 50 protons and 82 neutrons. These fission yields may be suppressed because of the odd-odd nuclear structure of 130gSb and the odd-even structure of 129Sb and isomer splitting. Comparisons to other recent work and a brief review with citations are included to support this conclusion.

Fission Yields↗

NCERC Capabilities [Slides]

NCERC is our nation’s only generalpurpose critical experiments facility and is one of only a few that remain operational throughout the world. The mission of the National Criticality Experiments Research Center (NCERC) is to conduct experiments and training with critical assemblies and fissionable material at or near criticality in order to explore reactivity phenomena, and to operate the assemblies in the regions from subcritical through delayed critical. One critical assembly, Godiva-IV, is designed to operate above prompt critical.

61 RADIATION PROTECTION AND DOSIMETRY↗

Integral Measurement of the 237 Np($n$, γ) 238 Np Cross Section with Fast Neutrons

Accurate knowledge of the 237 Np($n$; γ) 238 Np cross section at fast neutron energies is important for applied nuclear science. The presently available experimental data has large disagreements in the fast neutron region. A measurement of the 237 Np($n$; γ) 238 Np cross section was performed using a well characterized fast neutron source and the results was compared with previous measurements and current nuclear data evaluations. This will provide an integral measurement that can be used as a benchmark for current evaluations. Multiple samples of 237 Np were irradiated in the Godiva-IV critical assembly. Following the irradiation, the samples placed in a γ-ray counting setup and the γ-rays emitted from the decay of 238 Np were measured over a time period of approximately 7 days. Multiple γ-ray decay branches of 238 Np were observed. The observed activity of 238 Np was used to calculate the amount of 238 Np produced during the irradiation via the 237 Np($n$; γ) 238 Np and an integral cross section of 359(10) mb was measured. The 238 Np half-life has been measured with a result of 50.34(7) hours. An integral measurement of the 237 Np($n$; γ) 238 Np cross section has been measured. This result has been compared to the calculated integral cross section using the ENDF/BVIII.0 and JENDL-4.0 evaluated cross sections and found to be in good agreement with ENDF/BVIII.0 value of 367 mb. The JENDL-4.0 evaluation yields a value of 312 mb, which is significantly lower than the measured cross section.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

IER 557: Godiva Pulse Repeatability and Characterization (CED-3A Report)

Godiva IV is a fast burst critical assembly constructed of approximately 65 kg of highly enriched uranium (HEU) fuel alloyed with 1.5% molybdenum for strength. Godiva IV is proposed as the radiation source for IER 498: Design a Shielding Benchmark with a Metal Critical Source. IER 498 proposes a two-burst method to determine the performance of shielding samples, comparing the transmission of the source radiation to detectors with and without a shielding sample present. This eliminates the need for an absolute calibration and allows many uncertainties to cancel. However, the source term variability must be low compared to other sources of experimental uncertainty to ensure the overall uncertainty meets acceptable levels to provide useful measurements. The primary goal of this experiment is to quantify the source term variability, or reproducibility, of Godiva bursts, focusing on the 70 °C bursts planned for IER 498 measurements. Discussions during IER 498 noted that a number of bursts (on the order of six to ten) as identical as possible would be performed and that a 5-7% standard deviation in source intensity would be acceptable.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

IER 268 CED-3b Report

The goal of IER 268 was to collect information from the operation of the Godiva IV super-prompt critical assembly to support multi-physics modeling efforts. There were two types of systems deployed. One was a Photo-Doppler Velocimetry (PDV) system which used the reflection of laser light on the surface of the Godiva IV core. The other consisted of an MHD 240 detector with two other detectors (an MHD-241 and an Eljen EJ-325A) used for reference as the MHD-240 detector was moved. The collection is referred to as the MHD Detector in the narrative log. There were two types of Godiva operations performed to gather data. A series of super-prompt critical bursts were performed and data collected on both systems, tied to a common trigger. Separately, a series of delayed critical operations at various power levels was performed for a combination of MHD detector distances from Godiva and the presence and absence of a shield in the line of sight between Godiva and the MHD detector. This data was collected to determine the contribution of room return during the burst measurements.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

A New Era of Nuclear Criticality Experiments: The First 10 Years of Godiva IV Operations at NCERC

The work presented in this paper focuses on the first 10 years (2011–2020) of Godiva IV operations at the National Criticality Experiments Research Center (NCERC). Godiva IV is a fast burst critical assembly constructed of approximately 65 kg of highly enriched uranium fuel alloyed with 1.5% molybdenum for strength. Godiva is one of the last such critical assemblies in the United States and can be used for studies of super-prompt-critical behavior as well as irradiations and demonstrations. An overview of the startup of Godiva IV at NCERC is given followed by a summary of the experiments performed utilizing Godiva IV over the first 10 years of operation at NCERC.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Criticality Accident Alarm System Shielding Benchmark: Integral Experiment Request 498, Critical Engineering Decision 2 Report

A workable design to perform a CAAS benchmark experiment is detailed herein. Key dimensions, materials, source intensity levels, and detectors are listed in this report. Sensitivity to 21 perturbations was determined to be acceptable. The next step will be for NCSP management to determine whether procurement should occur and if the experiment should proceed. The perturbation study suggests that the room return shield cavity radius and runout should be maintained to within a millimeter, the room return shield should be positioned carefully (perhaps with a laser range finder), and that the detectors should be mounted in a lightweight fixture such as aluminum, so their positioning is assured. Using a 3D scanner or photogrammetry to record part shapes may be beneficial. Further work is also needed to verify source reproducibility.

36 MATERIALS SCIENCE↗

Godiva Experiments for the Nuclear Criticality Safety Program (NCSP)

Godiva IV is a fast burst critical assembly constructed of approximately 65 kg of highly enriched uranium (HEU) fuel alloyed with 1.5 percent molybdenum for strength. Godiva is one of the last such critical assemblies in the United States, and can be used for studies of super-prompt critical behavior as well as irradiations and demonstrations. A demonstration of a Godiva burst is usually performed as a highlight of the hands-on portion of the Criticality Safety Training Classes taught at the National Criticality Experiment Research Center (NCERC). The Godiva burst is used to demonstrate the concept of super-prompt critical and the time-scale of a criticality accident. In addition, several NCSP projects have been conducted on Godiva IV over the past two years. One experiment focused on collecting data to support multiphysics simulations using Photo-Doppler Velocimetry (PDV) to measure surface movement and gamma detectors to measure the burst output as the burst develops from background to peak over ten orders of magnitude. Another experiment was performed to demonstrate the functionality of the Criticality Accident Alarm System (CAAS) system developed for installation in the Y-12 Uranium Processing Facility (UPF). The system must not only respond to a criticality event and alarm, but must also be shown to operate in a high dose environment.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

193 mIr/ 192 Ir ratio from irradiation with various NCERC critical assemblies

Eight irradiations of K 2 IrCl 6 pellets were carried out with three critical assemblies: Flattop-Oy, Flattop-Pu and Godiva IV. One of the irradiations was performed with three pellets at different locations of the critical assembly, while the other irradiations with pellets at the center, but operating the critical assembly at different power and, respectively, different neutron flux. Counting samples were prepared from the irradiated pellets and X-ray spectra measured with silicone drift detectors. The 193 mIr/ 192 Ir ratio is reported for each irradiation.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Godiva IV Burst Reproducibility and Diagnostic Testing

Godiva IV is a fast burst critical assembly located at the Nation Criticality Experiment Research Center (NCERC) in the Nevada National Security Site (NNSS). It is constructed of approximately 65 kg of highly enriched uranium (HEU) fuel alloyed with 1.5% molybdenum for strength. The assembly can be operated at delayed critical or can be used to perform super-prompt critical bursts with temperature rises of up to 250 °C. Several projects with the objective of characterizing Go diva IV are ongoing including characterizations of its radiation emission and thermomechanics. One of the characterization projects is a study of the variability in the relative source emission (or fluence in absolute terms) between bursts that are nominally the same size. There is some inherent variation in the number of fissions, or "size" of the burst, even for bursts where the operators perform identical processes. The source of the variation can be attributed to several factors. The largest contributor is the precision with which the operators are able to determine delayed critical (DC). Operators find DC for every burst operation. The impact of being slightly above or below DC can change the super-prompt critical reactivity and therefore the source term. The temperature of the fuel is another factor. Establishing delayed critical prior to performing a burst act as a control of the bulk temperature coefficient of reactivity.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

The National Criticality Experiments Research Center: Capability Expansion and Experiments in the Last Three Years

The National Criticality Experiments Research Center (NCERC) is a general purpose criticality experiments facility located inside the Device Assembly Facility (DAF) at the Nevada National Security Site (NNSS). Critical experiments containing any special nuclear material, any enrich ment/separation, most physical forms, and any configuration are possible within the constraints of the defined safety basis. NCERC draws upon physical assets and experimental knowledge to solve some of the most difficult problems with respect to criticality safety, reactor physics, and reactor kinetics. In terms of physical assets, NCERC houses hundreds of kilograms of special nuclear material with a majority consisting of highly enriched uranium (HEU) and weapons grade plutonium (WGPu). NCERC is home to four critical assembly machines: Comet, Planet, Flattop, and Godiva IV. To support various derivative diagnostics on fissioning systems, NCERC houses a count room to measure irradiated samples and dosimeters. This paper will step through each of these capabilities explaining recently completed work and upgrades.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Godiva IV Simulated Radiation Field Characterization and Variance Reduction

Godiva IV is a system comprised of highly enriched uranium alloyed with molybdenum in the form of fuel plate rings. The reactor, along with its predecessors, was designed with the unique ability to satisfy interests in the super-prompt-critical reactor operation space. Originally, the reactor was part of the Los Alamos Critical Experiments Facility (LACEF) at Technical Area-18 (TA-18). The radiation field around Godiva at this facility was well characterized and understood. As a fast neutron system, the neutron spectrum in and around Godiva was close to a Watt Fission spectrum. The Kiva where Godiva IV was located at LACEF was made of thin, sheet metal walls which did not contribute significantly to the neutron spectrum. Following the transition of LACEF to the National Critical Experiments and Research Center (NCERC) in Nevada, Godiva-IV was moved from TA-18 to the Device Assembly Facility (DAF) at the Nevada National Security Site (NNSS). Part of this move brought renewed interest in radiation field characterization. The new facility introduced significant changes to the environment surrounding Godiva, and preliminary foil irradiation results suggested that the room contribution to the neutron spectrum was significant. Unlike at TA-18, a large thermal neutron signature was added to the fast spectrum from Godiva due to significant room return. A primary goal due to the additional complexity that the room return adds to the Godiva IV radiation emission spectrum was the development of an efficient Monte Carlo N-Particle (MCNP) calculation capable of characterizing the neutron spectrum anywhere in the room around Godiva. A campaign of activation foil irradiations and analysis were completed to support the validation of the MCNP model. The modeling of these foils in MCNP can be easily done with a standard volumetric neutron flux tally. However, given the multitude of locations and reaction rates to be modeled, further steps must be taken to increase the efficiency of these calculations in MCNP. During this study, a benchmark model currently under development for Godiva IV was used. A qualitative assessment of the thermal neutron contributors was performed using spatial neutron distribution plots. Additional detail was added to the model based on the qualitative results showing the thermal spectrum’s large sensitivity to hydrogenous material. Neutron energy spectra was evaluated at discrete locations in the room around Godiva to quantify the relative contribution of various components. It was discovered that the concrete walls are the largest contributor to the thermal signature, with minor contributions from plastic components surrounding Godiva. Following these results, two different variance reduction techniques were implemented to improve the problem efficiency in these calculations. In the first approach, an F5 point detector tally was implemented in the standard Godiva IV criticality problem. The second approach involved a weight-window generator implementation with an F5 point detector tally in a fixed source problem. The weight window implementation reduced the runtime from 42739.55 minutes to 1803.34 minutes (computer time), compared to the F5 KCODE implementation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

NCERC 2024 Highlights

The National Nuclear Security Administration (NNSA) is entrusted with ensuring the safety, security, and reliability of the nation’s nuclear weapons stockpile while advancing programs aimed at reducing global nuclear proliferation. These critical mission objectives are achieved through the expertise of a highly skilled team of professionals. The operations at the National Criticality Experiments Research Center (NCERC) play a vital role in developing and enhancing knowledge and expertise in advanced nuclear technologies. NCERC supports a wide range of mission areas, including nuclear criticality safety, nuclear emergency response, and nuclear nonproliferation, safeguards, and arms control. It also provides support to the Department of Homeland Security, advances stockpile stewardship science, and delivers scientific expertise to other government agencies, such as NASA and the Defense Threat Reduction Agency. NCERC conducts experiments utilizing diverse nuclear materials, from small neutron-emitting sources for testing radiation detection equipment to larger quantities of uranium and plutonium for criticality experiments. A cornerstone of NCERC's mission portfolio includes the operation of four critical mass assembly machines—Planet, Comet, Flattop, and Godiva-IV—which are instrumental in advancing nuclear science and ensuring the nation’s nuclear security objectives.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Investigating Fission Reaction Rate Ratio Sensitivities [Abstract]

Reaction rate ratios are a measurable parameter for reactor and criticality applications. A number of foil irradiations and fission chamber measurements have been performed for critical assemblies at Los Alamos National Laboratory starting in the 1950’s including (i) Godiva, a bare HEU spherical assembly; (ii) Flattop-25, a spherical assembly consisting of an HEU core and a natural uranium reflector; (iii) Jezebel, a bare 239 Pu assembly; and (iv) Flattop-Pu, a spherical assembly consisting of a 239Pu core and a natural uranium reflector. Fission ratio data for 238 U(n,f)/ 235 U(n,f), 237 Np(n,f)/ 235 U(n,f), 233 U(n,f)/ 235 U(n,f) and 239 Pu(n,f)/ 235 U(n,f) were obtained and reported. The EUCLID (Experiments Underpinned by Computational Learning for Improvements in nuclear Data) project at Los Alamos National Laboratory (LANL) aims to constrain nuclear data by using a suite of measurement types beyond k-effective. Recent investigations include the use of pulsed spheres for nuclear data validation and other measurement methods of interest. One focus of the work is to determine if other methods are complimentary to the critical experiments utilized for nuclear data validation. It is anticipated the investigations will help inform methods that may be utilized in machine learning algorithms for nuclear validation. In order to use a measurement type for nuclear validation, it is necessary to obtain cross-section sensitivities for parameters. This work looks at reaction rate ratio sensitivities with SENSMG and Monte Carlo N-Particle R Code Version 6.21.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗