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UPF and Y-12 Criticality Accident Alarm System (CAAS) Radiation Testing Report

This report documents the experimental conditions and results for the testing of the Mirion Technologies CAAS-3S Criticality Accident Alarm System (CAAS) for the Y-12 National Security Complex (Y-12) and Uranium Processing Facility (UPF). The testing was conducted at the Godiva IV Burst Reactor at the National Criticality Experiments Research Center (NCERC) at the Nevada National Security Site (NNSS) during the week of January 11, 2021. The testing was conducted in accordance with 25774-QL-POA-JR00-00002-VDE-27.0, CAAS-3S Radiation Testing of Cabinet Components Test Plan. The tests subjected the CAAS-3S system to intense and short duration mixed neutron and gamma radiation fields and to high integrated radiation doses. The purpose of the test was to environmentally qualify various CAAS-3S components in a radiation environment. Successful completion of the tests was predicated on the collaborative efforts of several organizations. Sandia National Laboratory (SNL) and Lawrence Livermore National Laboratory (LLNL) provided dosimetry to estimate photon and neutron dose. Los Alamos National Laboratory (LANL) manages the NCERC facility, operated the Godiva IV reactor, and provided field support for CAAS-3S placement and communications interface for data acquisition systems supplied by Mirion Technologies. Throughout the test campaign, Y-12 and UPF personnel provided technical support in determining changes to the test schedule, as needed, interpretation of the results, and comparison between the measured dosimetry data and predicted results. Throughout the test campaign, Mirion personnel provided technical support in the operation of the CAAS-3S system itself.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Effects of Chlorine Capture and a Proposed Density Law on the Reactivity of Plutonium Solution Systems

During fissionable material processing, all normal and credible abnormal conditions must remain safely subcritical. Nuclear Criticality Safety (NCS) uses a number of methods to determine subcriticality, one of which is the use of neutron transport codes such as MCNP6. In order to create models for use with MCNP6, both the geometry and materials in fissionable material processes must be known, or assumptions must be made and quantified for the impact to bias. One of the systems with a significant amount of bias due to material modeling assumptions is in the area of aqueous plutonium processing. These solutions are typically plutonium nitrate solutions or plutonium chloride solutions, which are modeled as fictitious plutonium metal-water mixtures because little is known about the actual density of the solution and there is no current predictive capability approved for use at Los Alamos National Laboratory (LANL) for modeling them. This research is currently underway to fill the gap and develop an algorithm for use with MCNP6 to model the density of plutonium chloride solutions. The method is to be validated with experimental data for density, and also validated with critical experiments using MCNP6. Note that the Chlorine Worth Study (CWS) was performed in December 2021 to help bridge the gap in chlorine data for critical experiments, and is currently awaiting International Criticality Safety Benchmark Evaluation Project (ICSBEP) review. This study was performed by LANL at the National Criticality Experiments Research Center (NCERC) at the Nevada National Security Site (NNSS). Additional information regarding this experiment may currently be found in LA-UR- 22-29180. Additionally, the Chemistry-Actinide Analytical Chemistry (C-AAC) at LANL has performed a number of solution density measurements for PuCl 3 -HC 1 -H 2 O, allowing for such data be used to create a semi-empirical density via the Pitzer method. The published dataset for the measurements is documented in LA-UR-22-25454. This method has already been tested successfully for aqueous plutonium nitrate solutions in SCALE. Current solution density measurements exist of plutonium concentrations of 0-~142g/L, all at 2M HC1, at temperatures 20-40°C. Additional data was taken for HC1-corrected density values, which essentially mimics the data for a pure PuCl x -water solution. The calculations in this report aim to support the current research by demonstrating the difference in system reactivity for the current modeling method when compared to the new proposed modeling with a density law implementation, which is being written as a Python tool to be used with MCNP6.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Empirical Bounding Analysis and User Recommendations for a Neutron Multiplicity Detector

Neutron multiplicity detectors are useful for a variety of applications including nuclear emergency response, nuclear nonproliferation, safeguards, and criticality safety. When measuring black-box problems (i.e., when the system being measured is completely unknown) with systems that have relatively low detection efficiency, expert analysis is frequently required to determine appropriate bounds for system parameters such as neutron multiplication and neutron leakage. This is because the detection efficiency can vary wildly, which also means that the resulting system parameters can have large variations. This work applies an empirical approach to provide bounds on system parameters (such as system multiplication, neutron leakage, and detector efficiency). The results of this bounding analysis are then used as inputs to provide recommendations to users regarding criticality safety. In addition to describing the method used, this work provides sample results from a measurement campaign performed at the National Criticality Experiments Research Center (NCERC).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Preliminary RAM-RODD results for the MUSiC subcritical configurations

The Measurement of Uranium Subcritical and Critical (MUSiC) was performed at the DOE’s National Criticality Experiments Research Center (NCERC) located in the Nevada National Security Site (NNSS). The measurement utilized the Rocky Flats shells to perform benchmark measurements of similar highly enriched uranium (HEU) systems that span a wide range of reactivities. The Rocky Flats (RF) shells are 93.16% U-235 enriched metal hemishells that can be stacked concentrically. Ten configurations were measured with effective multiplication factors spanning between deeply subcritical (~ 0.64) through delayed critical. Details of the measured configurations are listed in Table 1. This unique set of measurements with its large span of reactivies is being used to determine the range over which neutron noise techniques such as Feynman variance-to-mean, Rossi-alpha, and pulsed neutron source techniques can be accurately employed for a bare HEU system. The results of the measurements will be published as a benchmark in The International Criticality Safety Benchmark Evaluation Project (ICSBEP) Handbook. The results will support the growing amount of subcritical benchmark data, such as the SCRaP measurements, that is available to the community. The measurements were performed using several different detector systems for the purposes of cross-validation and obtaining detector independent results. Four detector systems were deployed, three by the NCERC team and one from the University of Michigan. The detector systems included a Neutron Multiplicity Array Detector (NoMAD) system (similar to the MC-15), four small volume 0.635 cm (Ø) × 7.59 cm 3 He detectors (ideal for measuring prompt neutron decay constants due to their fast recovery speed), the Rossi Alpha Measurements – Rapid Organic (n, γ) Discrimination Detector (RAM-RODD), and the Organic Scintillator Array (OSCAR). RAM-RODD is an array of eight 5.08 cm (Ø) × 5.08 cm EJ-309 organic scintillator detectors. OSCAR is a University of Michigan system and is an array of twelve 5.08 cm (Ø) × 5.08 cm stilbene detectors. Details of measurements performed with OSCAR will be discussed in a separate talk. The focus of this work is preliminary results obtained by RAM-RODD for the 8 subcritical configurations. Additional details on the measurements and on the setup and deployment of RAM-RODD will be discussed. Preliminary neutron noise analysis results including Rossi-alpha and Feynman-alpha will also be presented.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Design of a Critical Experiment to Validate Yttrium Hydride at Varying Temperatures

As microreactors become an emerging nuclear energy source for remote applications, designers are looking at the use of high temperature moderator material to reduce the fuel mass in the core by up to a factor of two. The microreactor community is in constant search of the best moderator material to retain hydrogen at high temperatures while optimizing neutronic performance. Recent simulation work has shown that materials which have a high and low Z component are optimal for this application. Material properties studies have further shown that yttrium hydride maintains hydrogen and stays as a solid until well over the needed temperatures, and thus retains hydrogen. A critical experiment is planned at the National Criticality Experiments Research Center (NCERC) to test the reactivity behavior of yttrium hydride at standard and elevated temperatures.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Design of a High-Assay Low-Enriched Uranium Tri-Structural Isotropic Critical Experiment for Advanced Reactor Validation

High-assay low-enriched uranium (HALEU) fuel is a key component of many small modular reactor designs. Critical experiments are an important way to understand the neutronic performance of systems by obtaining nuclear data validations through measurements. Data reduce uncertainty and risk by showing that systems respond as predicted to changes such as temperature, subsequently advancing the overall technology readiness level of the materials within. Numerous critical experiments have been performed at the National Criticality Experiments Research Center (NCERC) operated by Los Alamos National Laboratory at the Nevada National Security Site since it became operational in 2011. However, the first experiment with HALEU fuel did not occur until 2024. Through extensive engineering, the experiment described in this paper was successfully designed and executed for the Comet vertical lift assembly at NCERC to perform measurements with HALEU tri-structural isotropic fuel that will assist in validation of nuclear data and computational modeling of small modular reactors for years to come.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Design Optimization for EUROPA Critical Experiment

The Experiment for Unresolved Region Of Plutonium Actinides (EUROPA) is an integral critical experiment currently being designed to target the intermediate energy region of plutonium. Intermediate energies, those between 0.625 eV - 100 keV, contain the end of resolved and beginning of the unresolved resonance region, making experiments in this energy range prudent for validating the representation of cross sections in this transition region. Below is the preliminary design of the experiment to be performed at the National Criticality Experiments Research Center (NCERC). Experiment optimization required an exhaustive down selection of several moderating, absorbing, and reflecting materials using Particle Swarm Optimization (PSO) in order to achieve maximum sensitivity to the intermediate energy region.

07 ISOTOPE AND RADIATION SOURCES↗

Polymer Compositions in Critical Experiments: Possibly Not What You Think

The Chlorine Worth Study (CWS) Experiment was performed at the National Criticality Experiments Research Center (NCERC) in December 2021. Its goal was to provide a validation benchmark experiment with chlorine and plutonium in the thermal neutron spectrum. This purpose is necessary to reduce the margin of subcriticality in aqueous chloride operations at the Los Alamos National Laboratory Plutonium Facility (PF-4). Reducing the margin of subcriticality will enable higher throughput, required to meet NNSA mission needs. The experiment used layers of plutonium plates, polyethylene (HDPE), aluminum, and polyvinyl chloride (PVC) or chlorinated polyvinyl chloride (CPVC). They were optimized to match plutonium-chloride solutions of 30 g/L, 300 g/L, and 600 g/L. Upon completion of the experiment, a International Criticality Safety Benchmark Evaluation Program (ICSBEP) report was immediately started. The compositions of all materials were assumed pure unless additional information was known (such as for the plutonium plates). During the benchmark analysis, the assumed CPVC composition was questioned. The follow-on work led to lessons learned on compositions in benchmarks. Materials, and specifically polymers, are often much more complex than a basic chemical formula. The CWS experiment is used as an example in this paper to document the lessons learned.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

NCERC Capabilities

National Criticality Experiments Research Center (NCERC), located at the Nevada Nuclear Security Site (NNSS) operated by Los Alamos National Laboratory, is our nation’s only general-purpose critical experiments facility and is one of only a few that remain operational throughout the world. NCERC Directly Contributes to Important National and International Missions and is Making Investments in Pipeline and the Facility for enduring capability and expanding missions. More detailed capabilities are described.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

A New Era of Nuclear Criticality Experiments: The First 10 Years of Radiation Test Object Operations at NCERC

The work presented in this paper focuses on the first 10 years (2011–2020) of radiation test object (RTO) operations at the National Criticality Experiments Research Center. RTOs are subcritical configurations of special nuclear material that are built by hand. These configurations are utilized for benchmark experiments, detector testing/characterization, and training. An overview of the types of measurements used in RTO operations is given as well as a history of RTO operations at Los Alamos National Laboratory from 1944–2011.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The Deimos Experiment: Advanced Reactor Testbed

Advanced reactor initiatives are growing significantly through programs nationwide. This research area includes small modular reactors, microreactors, and space reactors. Many of the reactors being designed are untested concepts. They include unique moderators, varying fuel types, high temperatures, and compact configurations. The shift in fuel type, from highly enriched uranium (HEU) to high assay, low enriched uranium (HALEU), is particularly important as it has driven many of the other changes. For example, lower enrichment requires advanced moderators, which in turn require different reflectors to make the systems compact. The change in materials including the transition from HEU to HALEU affects the temperature feedback of the systems. Additionally, these advanced reactor concepts generally have a thermal neutron spectrum in contrast to earlier fast spectrum advanced reactor. With the extensive changes from previous reactor designs, validation experiments are needed. The National Criticality Experiments Research Center (NCERC) is uniquely equipped to perform such experiments. The Deimos experiment, designed for execution at NCERC, will serve as a testbed for advanced reactor concepts. It will use HALEU fuel in a graphite matrix, provide the ability to use advanced moderators, and allow measurements of temperature reactivity coefficients (TRCs).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

How to Safely Build 100-plus Kilograms of Weapons-Grade Plutonium

The goal of the EUCLID (Experiments Underpinned by Computational Learning for Improvements in Nuclear Data) project was to reduce compensating errors by utilizing machine learning to both help determine which reactions contain compensating errors as well as optimizing an experiment which can be used to maximally reduce these errors. Compensating errors can adversely impact the predictive power of application simulations, and therefore it’s useful to further constrain nuclear data and reduce these errors. The EUCLID project included building two configurations at the National Criticality Experiments Research Center (NCERC). These two configurations had very different geometries (one was cube-like and one was slab-like). Previous works focus on selection of the target experiment(s), radiation transport capabilities developed in the project, the experiment optimization, and the performance of the experiments. This work will focus only on the safety aspects of performing this experiment, which utilized over 100 kg of weapons-grade plutonium.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

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 ↗

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 ↗

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 ↗

Update on the Benchmark Analysis of the Jupiter Experiments: Plutonium Moderated by Lead

The Jupiter experiment was a series of measurements in the summer of 2017 to analyze the effects of voids in lead moderated plutonium assemblies. This experiment was part of a larger campaign that took place at the National Criticality Experiments Research Center (NCERC) in collaboration with the Japan Atomic Energy Agency (JAEA) that also investigated assemblies with differing uranium enrichments. The purpose for this campaign was to provide data useful for a potential lead-bismuth cooled accelerator driven system. This data is needed due to the low number of benchmarks involving lead. Given the wide use of lead for shielding in addition to new reactor designs, there is a need for further benchmarking that this experiment could help fulfill. In addition, adding more benchmarks to the International Criticality Safety Benchmark Evaluation Project (ICSBEP) is helpful for further validation of simulation methods used for criticality safety. This summary is an update on the current progress of this analysis, and all results shown are preliminary.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

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

Comet is a general-purpose, heavy-duty, vertical-lift assembly designed for flexibility in conducting a variety of critical experiments. It is currently located at the National Criticality Experiments Research Center (NCERC) in Nevada. In the past, Comet resided at Technical Area-18 in Los Alamos, New Mexico, as part of the Los Alamos Critical Experiments Facility (LACEF). The Comet assembly was relocated to NCERC in 2008 and became fully operational in June of 2011. The first critical experiment performed on Comet at NCERC was a verification of one of the previous configurations of the Zeus experiment series. Over the next 10 years, many additional experiments followed including other Zeus configurations as well as completely new designs. This paper discusses the Comet vertical-lift assembly, the transition from LACEF to NCERC, and a selection of experiments that have been performed on Comet during its first 10 years of operation at NCERC.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

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↗