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Nuclear Criticality Experiments Research Center Futures: A Report of a Workshop held September 6-9, 2022, Los Alamos, NM, November, 2022

Experiments and training with critical assemblies and fissionable material (at or near the critical state) that explore reactivity phenomena are central to a number of national security challenges. From fission energy to nuclear weapons to a broad suite of scientific challenges, it is clear that additional capacity and capability are needed. The National Criticality Experiments Research Center (NCERC) marked 10 years of operations in 2021. This anniversary was an opportune time to celebrate our successes and progress, and to evaluate the remaining and emergent challenges. Against this backdrop, a workshop of approximately 140 national and international leaders in nuclear research was convened in Los Alamos, New Mexico to explore “NCERC Futures.” Therefore, the present workshop focused specifically on needed capabilities and tools to meet the research challenges in eight topical mission areas served by NCERC. As each Topical Group summarized their discussions in the out brief, it was recognized that key challenges could be met through enabling infrastructure investments and new critical assemblies. Enabling infrastructure includes staffing, additional space/buildings, developing an agile bounding safety basis, the ability to keep pace with technological advances in detectors and data acquisition systems (allowing use of those with Bluetooth™ and similar technologies), an expanded set of materials options (especially plutonium), a “Plug and Play” design and implementation mindset, and a facility that enabled free-field measurements. The new critical assemblies that were identified as having the most impact were a bare plutonium (Pu) Critical Assembly, a Horizontal Split Table (HST), a Super Comet, and a Uranium Solution Burst Assembly. NECRC is a unique, one-of-a-kind facility in the United States. If all the improvements were to be made, NCERC would enable the United States and its partners to address many important research questions related to criticality. These include but are not limited to: (1) Covering the entire neutron energy spectrum for both highly enriched uranium (HEU) and Pu in configurations for virtually all conceivable applications; (2) Performing multi-physics solution experiments and irradiations with a Uranium Solution Burst Assembly, which more closely resembles actual criticality accidents; (3) Conducting free-field experiments to make basic fission physics measurements and much cleaner benchmarks with various experimental observables; and (4) Providing more training classes and more experiments annually at greater cost efficiency enabled by additional buildings and machines and an agile, bounding, risk-balanced Safety Basis. In the end, workshop attendees enthusiastically concluded that NCERC Futures are bright and the workshop helped to identify a roadmap of capability gaps that need to be addressed. This report documents the results of those efforts.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Neutron Absorber Plate Characterization Plan for Criticality Experiments Design

After being used in nuclear installations, depleted fuel can still be highly reactive and must be handled securely to prevent any radiological or criticality concerns. In particular, spent fuel from use in nuclear power reactors must be stored and transported in specifically designed containers using neutron absorber materials to prevent criticality. Various neutron absorber material types exist and are manufactured by various entities, as thoroughly described in the Handbook of Neutron Absorber Materials for Spent Nuclear Fuel Storage and Transportation Applications written by EPRI. Presently, one of the most modern and most widely used types of neutron absorber material contains particles of boron carbide, or B 4 C, embedded in aluminum matrix: Boralcan, manufactured by Rio Tinto. It is very important for the community to know as much as possible about such neutron absorber materials. Therefore, in the recent years, a US Department of Energy National Nuclear Security Administration–Nuclear Criticality Safety Program funded project initiated design of an experiment that places Boralcan neutron-absorbing plates in an established critical assembly using low-enriched uranium fuel at the Sandia Pulsed Reactor Facility/Critical Experiments (SPRF/CX) apparatus at Sandia National Laboratories. The goal of the experiment is to produce high-quality benchmark data to submit to the International Criticality Safety Benchmark Evaluation Project (ICSBEP), for use in validating calculational tools and nuclear data by criticality safety analysts. The project, named IER-554, is currently in its final design stage, following a successful preliminary design. In the work documented in the design study, ten critical configurations using Boralcan neutron absorber plates were designed, and the experiment was proven to be feasible, with a predicted low k eff uncertainty around 100 pcm. An overview of the modeled cutout of the critical assembly with a Boralcan plate is shown in Figure 1, representing one of the configurations planned for the critical experiments. Before the plates are inserted in the critical assembly, it is necessary to know more about their composition and uniformity. This summary focuses on the plate characterization plans. Each plate will undergo (1) neutron transmission measurements at different locations to determine the 10 B areal density and (2) an in-depth x-ray computed tomography (XCT) examination to obtain the exact Sizes and distribution of the B4C powder particles inside the plates. In parallel, plate modeling studies are performed with a goal to determine the validity of the currently used approximation of modeling the neutron absorber plates as a homogeneous mixture of Aluminum 1100 alloy and B4C— instead of explicitly modeling the B4C particles. By using the experimental 10 B areal density measurements, and the exact size and location of the B4C particles obtained by XCT, a plate model can theoretically be built that reproduces the plate with extremely high fidelity. The results of this modeling study could increase the confidence of the criticality safety community in its modeling methods when using this type of neutron absorber material, and the industry could use these validations to change the boron loading credit limits from the U.S. Nuclear Regulatory Commission standard review plan for dry cask storage of spent nuclear fuel. The modeling calculations are performed with SCALE 6.3.0 using the KENO V.a sequence for criticality calculations with the ENDF/B-VIII.0 continuous-energy cross section library.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fission neutron activations of stainless steel and its corresponding elemental components

Characterizing neutron activation of stainless steel is a critical task for many applications, and yet little activation data is available for this alloy. To address the need, a series of neutron activation experiments have been performed using the Flattop critical assembly at the National Criticality Experiments Research Center. Several experimental conditions were probed for complete understanding of the neutron environment, including foil composition and position within the assembly. The experimental results reported here will aid in the production of stainless steel benchmarks for a range of nuclear data applications including those used in nuclear forensics analysis.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Formatting and V&V of Consistent 238,240−24 2Pu $\overline{v}_p$ Evaluated Mean Values and Covariances

This report is in answer to the Nuclear Criticality Safety Program FY24 quarter 4 milestone that requires: “Format and V&V nu-bar means and covariances” for 238,240-242 Pu average prompt fission neutron multiplicities, $\overline{ν}$ p , that were obtained by a consistent evaluation leveraging the fission-event generator CGMF and a detailed uncertainty quantification of experimental data. It is described how nuclear data mean values and covariances were formatted using ENDFtk. Implementing the new 238,240-242 Pu $\overline{ν}$ p into the ENDF/B-VIII.1β 4 library leads to only small overall changes in criticality values of the Jezebel, Dirty Jezebel, Jupiter-001, Jupiter-002, EUCLID 3x2 and EUCLID 8x1 critical assemblies. Simulated k eff uncertainties due to $\overline{ν}$ p covariances change only little if cross-isotope covariances are considered or not for those assemblies with low percentage content of minor Pu isotopes. However, for the Dirty Jezebel critical assembly, that has a sizeable 240 Pu and non-negligible 241 Pu content, the simulated k eff uncertainties due to considering or neglecting cross-isotope $\overline{ν}$ p covariances is 443 versus 374 pcm.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Comparison of Approach-to-Critical Results in Current and Pulse Mode for Systems with High Starter Neutron Rates

Reactors and critical assemblies use a variety of detection systems to monitor the neutron population. The count rate is proportional to the neutron flux present at the location of the detector. When such systems are placed external to an assembly, it is often assumed that the relative leakage multiplication will be proportional to the detector count rate (assuming that the source term, system geometry, and detector placement have not changed). Such systems are often used in an approach-to-critical during reactor startup to ensure that the critical configuration is well predicted. Various types of detectors have been used during an approach-to-critical. These include 3 He, BF 3 , ion chambers, fission chambers, and fission foils. Any of these types of systems (or others) should work well when adequate counting statistics are available. These detector systems can be operated in either pulse or current mode. The National Criticality Experiments Research Center (NCERC) has two detection systems that are commonly used in critical assembly operations. The start-up (referred to as "SU" in this work) system is made up of 3 He proportional counters in pulse mode and the linear counter system (referred to as "LC" in this work) consists of compensated ion-chambers in current mode. Typically the SU system is used for approach-to-critical operations and the LC system is only used at/above delayed critical ( k eff = 1). This work investigates the use of the LC system for an approach-to-critical. It has been long hypothesized that such an approach would be feasible for systems with high starter neutron rates.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

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 ↗

Experimental detailed power distribution in a fast spectrum thermionic reactor fuel element at the core/BeO reflector interface region

A zero-power critical assembly was designed, constructed, and operated for the prupose of conducting a series of benchmark experiments dealing with the physics characteristics of a UN-fueled, Li-7-cooled, Mo-reflected, drum-controlled compact fast reactor for use with a space-power conversion system. The critical assembly was modified to simulate a fast spectrum advanced thermionics reactor by: (1) using BeO as a reflector in place of some of the existing molybdenum, (2) substituting Nb-1Zr tubing for some of the existing Ta tubing, and (3) inserting four full-scale mockups of thermionic type fuel elements near the core and BeO reflector boundary. These mockups were surrounded with a buffer zone having the equivalent thermionic core composition. In addition to measuring the critical mass of this thermionic configuration, a detailed power distribution in one of the thermionic element stages in the mixed spectrum region was measured. A power peak to average ratio of two was observed for this fuel stage at the midplane of the core and adjacent to the reflector. Also, the power on the outer surface adjacent to the BeO was slightly more than a factor of two larger than the power on the inside surface of a 5.08 cm (2.0 in.) high annular fuel segment with a 2.52 cm (0.993 in. ) o.d. and a 1.86 cm (0.731 in.) i.d.

Klann, P. G.↗

CERBERUS: A ZEUS Configuration With HEU and Copper Reflected by Copper

The Critical Experiment Reflected By copper to bEtteR Understand Scattering (CERBERUS) experiment is a a series of measurements performed at the National Criticality Experiments Research Center (NCERC) on the Comet critical assembly machine with a thick copper (Cu) reflector around alternating layers of Cu plates and highly enriched uranium (HEU) pancake plates. The measurements were performed by personnel from Los Alamos National Laboratory (LANL): T. Cutler, K. Amundson, N. Thompson, T. Grove, K. Stolte, and Z. Lemke, along with the multiple people who supported additional measurements and material handling. The purpose of this experiment was to investigate the impact of Cu scattering cross-sections in an integral experiment using the Comet critical assembly machine. Three configurations, which differed in the amount of Cu between each HEU layer, were evaluated as benchmarks. The three configurations are 3/16 inch, 5/16 inch, and 7/16 inch, which represent the amount of Cu above and below each HEU layer. Throughout the rest of the document the units associated with the configuration will be removed from the configuration name.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Multidimensional analysis of fast-spectrum material replacement measurements for systematic estimation of cross section uncertainties

A series of central core and core-reflector interface sample replacement experiments for 16 materials performed in the NASA heavy-metal-reflected, fast spectrum critical assembly (NCA) were analyzed in four and 13 groups using the GAM 2 cross-section set. The individual worths obtained by TDSN and DOT multidimensional transport theory calculations showed significant differences from the experimental results. These were attributed to cross-section uncertainties in the GAM 2 cross sections. Simultaneous analysis of the measured and calculated sample worths permitted separation of the worths into capture and scattering components which systematically provided fast spectrum averaged correction factors to the magnitudes of the GAM 2 absorption and scattering cross sections. Several Los Alamos clean critical assemblies containing Oy, Ta, and Mo as well as one of the NCA compositions were reanalyzed using the corrected cross sections. In all cases the eigenvalues were significantly improved and were recomputed to within 1 percent of the experimental eigenvalue. A comparable procedure may be used for ENDF cross sections when these are available.

Klann, P. G.↗

Understanding the impact of nuclear-data covariances on various integral responses using adjustment

The EUCLID (Experiments Underpinned by Computational Learning for Improvements in Nuclear Data) project created a library of sensitivities for nine different integral responses with respect to nuclear data. These integral responses were obtained from measurements at LLNL (Lawrence Livermore National Laboratory) pulsed spheres, critical and sub-critical assemblies. At the same time, covariances for ENDF/B-VIII.0 were processed at LANL (Los Alamos National Laboratory). The combination of these data allow us to study the impact of nuclear-data covariances on various integral responses, either by forward-propagating covariances via sensitivities, or by using nuclear data, integral responses, and sensitivities for adjustment. Here, we will present: the impact of 1 H, 9 Be, 12 C, 27 Al, 56 Fe, 235,238 U, and 239,240 Pu ENDF/B-VIII.0 covariances on simulated bounds of the following integral responses: LLNL pulsed-spheres neutron-leakage spectra, the effective neutron multiplication factor, reaction rates, and reactivity coefficients of ICSBEP critical assemblies. Also, adjustment results with the same nuclear-data covariances and responses will be discussed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Quick Look Report of Godiva U233 shot March 2022 Data Collection Activities

This report discussing the March 2022 irradiation of U233 on the Godiva critical assembly using burst mode and subsequent analysis of the fission products starting at 65 minutes post irradiation, and ending 12 days later. The Short-Lived Fission Product Yield (SLFPY) project is one of many efforts under the Nuclear Physics Multi-Lab and related Venture Project. The objective of the SLFPY project is to provide improved measurements of fission product yields for select nuclides. The SLFPY project consists of measurement and analysis campaigns. To produce fission data, samples of actinide material are irradiated in a high-flux neutron environment. These samples are quickly placed in front of a detection system where both gamma singles and coincidence spectra are collected as a function of time. Gamma spectroscopy is performed on the irradiated material on site near the irradiation facility, starting as soon as feasible after the irradiation and continuing for 7 days or longer. Following the data collection, time-dependent fission yield analyses are performed using gamma-ray spectroscopy. This document summarizes the measurement campaign performed March 21 - April 4, 2022 where sub-gram quantities of 233 U nitrate (UO 2 (NO 3 ) 2 ) were irradiated in the Godiva reactor. The Godiva burst #2076 conducted under experiment IER 504 had a temperature change of +156 degrees Celsius, lasted 13.32 microseconds, and had a reactivity of $\$$1.089. The targets consisted of uranium oxide solution deposited in a quartz tube and packed with quartz wool. The flame-sealed quartz ampoules were used to contain the uranium samples for the irradiation and count activities. On March 22, 2022, at 10:27:00 a.m. the three uranium ampoules, along with a witness foil pack, were irradiated in the Godiva critical assembly using burst mode operations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Determining the 9 $\mathrm{Be}$($n, γ$) 10 $\mathrm{Be}$ integral cross section at fission neutron energies

The 9 B neutron capture cross section has significant implications for Be materials in the nuclear industry as well as the α process in stellar nucleosynthesis. While the cross section is well constrained at thermal neutron energies, there is a lack of experimental data at higher neutron energies, and the evaluated nuclear data libraries can differ by up to two orders of magnitude. We calculate the 9 Be(n, γ) 10 Be integral cross section at fission neutron energies in an effort to resolve disagreements amongst the nuclear data libraries. Foil irradiation experiments were performed using the Flattop critical assembly at the National Criticality Experiments Research Center with either the highly enriched U or Pu cores, with target foil stacks placed at multiple locations to exploit different neutron energy profiles. Accelerator mass spectrometry was used to measure the 10 Be/ 9 Be ratio in irradiated Be foils, while all other activation products were quantified through gamma spectrometry. The experiments were simulated using the Monte Carlo N-Particle radiation transport code and combined with experimental results to determine the total neutron fluence, while the staysl-pnnl suite and fispact-ii code were used to validate the model and assess the systematic uncertainty. The new 9 Be(n, γ) 10 Be integral cross sections calculated in this work are 26.5 ± 2.2µb at 0.59 ± 0.07 MeV, 24 ± 3 µb at 0.98 ± 0.14 MeV, 21.7 ± 1.3 µb at 1.26 ± 0.11 MeV, 21.8 ± 1.4 µb at 1.32 ± 0.11 MeV, and 18.6 ± 1.1 µb at 1.46 ± 0.13 MeV. These results do not agree with integral cross sections from any of the nuclear data library evaluations. Discrepancies between the new integral cross sections reported here and the nuclear data libraries suggest a more complex cross-section structure in the MeV range which allows for more resonance contributions, and more work is needed to further constrain the evaluated cross sections.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗