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Energy-resolved neutron imaging and diffraction including grain orientation mapping using event camera technology

Time-of-flight neutron diffraction and energy-resolved imaging each provide unique perspectives into material properties. Neutron diffraction is useful for assessing microstructural parameters such as phase composition, texture, and dislocation densities, though it typically provides averaged data over the sampled volume. Energy-resolved imaging, on the other hand, offers both spatial and spectral information by detecting Bragg edges and neutron absorption resonances, which enables detailed mapping of microstructure and isotopic composition. When combined, these techniques have the potential to enrich our understanding of material behavior across different scales, enhancing our understanding of complex materials. Traditionally, these modalities are conducted on separate instruments, which is time-consuming and poses challenges for data integration. Here, we report the integration of the LumaCam, an event-mode energy-resolved neutron imaging camera with the HIPPO time-of-flight diffractometer at LANSCE. This integration enables simultaneous diffraction and imaging across the full spectrum, with analysis optimized for diffraction and Bragg-edge imaging in the thermal range (0.45–10 Å) and resonance imaging in the epithermal range (0.5–3000 eV), facilitating comprehensive multi-modal analysis. We demonstrate its capabilities through case studies, including spatial mapping of grain orientations in a steel sample and accurate thickness estimations for irregular samples including a depleted uranium cylinder and a natural silver-containing mineral specimen. The combined setup enhances real-time sample alignment and provides comprehensive data for crystal structure, texture, and isotopic composition analysis. This approach opens new possibilities for advanced applications in nuclear engineering, archaeology, and materials science.

36 MATERIALS SCIENCE

A simulation pipeline for fast neutron imaging and spectroscopy using quantified detector attributes

Radiation imaging capabilities, essential in the nuclear nonproliferation regime, facilitate source localization and, in certain cases, spectroscopy. Scatter-based neutron cameras, which can measure the neutron signatures from special nuclear material, hold particular interest. Systems incorporating organic scintillators can extract neutron energy spectra, potentially distinguishing fission neutron sources from others, such as alpha-neutron sources. The development and testing of a scatter-based neutron imager, however, can be challenging without having an accurate simulation model or first constructing a prototype. This work describes a simulation pipeline that takes output from MCNPX-PoliMi simulations and creates the expected back-projection neutron images and neutron energy spectra. This pipeline was developed to improve the modeling of fast neutron imagers and bridge the current gap in literature, which predominantly focuses on gamma-ray Compton imager models. This work also reports on the significance of various real-world system considerations and their effects on the simulated detector responses. The pipeline was verified and validated with experimental data collected using a 252 Cf spontaneous fission source using a fast neutron scattering imager developed at the University of Michigan.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND

Forward modeling approach to nuclear reaction cross sections: Applications in neutron inelastic scattering

The development of nuclear reaction models for the production of evaluated nuclear data has traditionally been performed by comparing measured cross sections with predictions from reaction model codes whose physical input parameters are adjusted to obtain the best agreement between measured and modeled results. To more directly probe reaction model inputs, this work introduces a forward modeling approach to experimental reaction cross-section determination, where the most important physical input parameters to reaction model calculations are obtained via 𝜒 2 minimization between measured and calculated observables. This was demonstrated using data collected by the Gamma Energy Neutron Energy Spectrometer for Inelastic Scattering (GENESIS) at the 88-inch cyclotron at Lawrence Berkeley National Laboratory, a detection array consisting of organic liquid scintillators and high-purity germanium (HPGe) detectors. Using a broad-spectrum neutron beam and a 99.98%-enriched 56 Fe target, GENESIS was used to perform a simultaneous measurement of 56 Fe 𝛾-ray production cross sections and secondary neutron energy and angle distributions. The results of the forward modeling approach to the determination of energy-differential 𝛾-ray production cross sections for the yrast 4 + → 2 + and 6 + → 4 + transitions, as well as eight other off-yrast transitions, were compared against those obtained using conventional techniques, and the results are in good agreement. In addition to discrete 𝛾-ray yield total scattered neutron energy-angular distributions as a function of incident neutron energy were also obtained using forward modeling and found to agree with evaluated data, with the exception of elastic scattering at small angles. The fitted reaction model parameters obtained through forward modeling were also used to calculate the cross section for the unobserved (𝑛, 2⁢𝑛) reaction; excellent agreement with the current evaluation was obtained, providing a validation of the predictive capabilities of the forward model approach. This work bridges the gap between nuclear data experiment and evaluation by providing a new means for extracting inelastic neutron-scattering cross sections and neutron-induced 𝛾-ray production data while directly probing reaction model physics.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS

Godiva IV Thermal Neutron Dosimetry Modeling and Variance Reduction

The transfer of the Godiva IV experiment from the Los Alamos Critical Experiments Facility (LACEF) to the National Critical Experiments Research Center (NCERC) introduced a vastly different experiment room return to the neutron flux. The contribution of the background to the burst neutron energy spectrum is significant in the thermal and epithermal neutron energies. Target materials may be placed in various locations in the Godiva room, or outside of the room, for thermal neutron activation. Modeling of this dosimetry problem in Monte Carlo N-Particle (MCNP) presented a novel challenge compared to previous Godiva IV glory hole irradiation simulations. An advanced dosimetry modeling framework for high efficiency calculations in locations far from the Godiva IV fission source was desired. The mesh-based weight windows and point detector advanced variance reduction techniques in MCNP were implemented and tested using adaptations of the critical experiment benchmark model of the Godiva IV problem. The models were validated against measured activations of Nickel, Indium, Scandium, and Cobalt foils at locations 2 meters from the Godiva IV core. Dosimetry measurements were performed in collaboration with Sandia National Laboratory. The weight windows and point detector variance reduction coupled method resulted in the highest problem efficiency.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS

Interpreting scattered neutron spectra on omega cryogenic implosions with measured backgrounds and higher-order scattering

Measurements of the areal density (⁠ρR⁠) of inertially confined implosions are critical to evaluate their performance. On OMEGA, ρR is inferred from measurements of the scattered neutron spectrum via neutron-time-of-flight (nTOF) and magnetic recoil spectrometer detectors. The nTOF measurements, in particular, have the ability to measure a wide range of neutron energies and thus scattering angles, with high precision. However, the neutrons that are backscattered into the detector must transit through the entire dense fuel assembly, and as a result are subject to rescattering effects, which have been heretofore neglected in the interpretation of OMEGA neutron spectra. At the backscatter edge, neglecting rescattering on OMEGA can lead to a ~10 to 20% reduction of the apparent areal density and therefore must be included in the analysis. The low ρR s on OMEGA also mean that backgrounds from non-target physics effects, such as scattering in the target chamber or slow scintillator decays, can significantly alter the measured signal. Here, we discuss how the Monte Carlo neutron spectrum postprocessor IRIS is used to include second-order scattering effects in the interpretation of the scattered neutron spectrum in OMEGA implosion experiments, and how dedicated implosion experiments are used to measure nTOF backgrounds in order to infer backscattered areal densities on OMEGA.

Deuterium

Characterizing the Experiment for Calibration with Uranium (Excalibur) neutron source for use in warhead verification

Neutron sources can play a variety of roles in warhead verification. For transmission radiography, a source of directed high energy neutrons is required, while for applications to detect fissile isotopes, sub-MeV neutrons are preferred. The Excalibur (Experiment for Calibration with Uranium) neutron source has been built and used in a variety of verification-related experiments. Excalibur is based on a commercial deuterium-tritium neutron generator specified and measured to be capable of producing 14 MeV neutrons at rates of up to 8.2 × 10 8 neutrons/s. Here, the generator is enclosed in a carbon-steel 32" diameter, 23.62" high carbon-steel cylinder that moderates the mean neutron energy to under 500 keV. This, in turn, is encased in 5%-borated polyethylene such that the entire assembly is a 48" x 48" box that is 30" tall. For radiographic applications, a narrow, tapered channel in the steel and polyethylene allows 14 MeV neutrons to stream directly from the generator to a test object. Its collimating capability is demonstrated by measuring the neutron flux profile. In the moderated mode of operation, the generator is fully enclosed in the steel, but a large section of the polyethylene is removed, providing a flux of sub-MeV neutrons from a wide range of angles. Neutron angular and spectral measurements using both a nested neutron spectrometer and a commercial liquid scintillator coupled with a 3 He detector show the expected softer neutron spectrum in moderated mode in good agreement with MCNP6 calculations. The gamma-ray spectrum from Excalibur is also in good agreement with MCNP modeling. Based on these findings, the future application of Excalibur in its two configurations is discussed.

Fissile material detection

Benchmarking fast-neutron response of 7 Li-enriched C 7 LYC scintillators: Simulations and experiment

New insights into the fast neutron response of 7 Li-enriched C 7 LYC scintillators have been obtained through detailed Geant4 simulations of 35 Cl(n,p) and 35 Cl(n, α) reactions that are primarily responsible for the fast neutron response of C 7 LYC. The light output of a 1” x1” C 7 LYC detector was simulated using the Birks equation for light quenching in scintillators. The simulations were benchmarked against neutron scattering data from a 12 C target obtained with a white neutron beam at the Los Alamos LANSCE facility and fourteen 1”x1” C 7 LYC detectors. Incident neutron energies extracted from time-of-flight measurements, and appropriate recoil corrections for the different detector angles were used to map the response of C 7 LYC to mono-energetic neutrons. Resonances in the 35 Cl(n,p) reaction cross-section below 3 MeV incident neutron energy were directly observed in C 7 LYC. The experimental data and simulations are compared with ENDF databases, as well as recent direct cross-section measurements of neutrons scattered from a 35 Cl target. In conclusion, the results suggest a scrutiny of the 35 Cl(n,p) and 35 Cl(n, α) cross sections at low energy in the ENDF library.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS

Introduction, Investigation, and Experimental Validation of a Novel Passive Neutron Spectrometer

Unfolding neutron energy spectra are instrumental for determining personal health effects and calculating dose received. This area of study is heavily researched, and Lawrence Livermore National Laboratory (LLNL) is investigating a passive neutron spectrometer for the purpose of acquiring the information needed to determine personnel dose in the event of a criticality accident. A part of this investigation is presented in this article through the examination of four experimental detector responses (DRs). These four DRs were acquired in the presence of 252 Cf, AmBe, GODIVA, and National Ignition Facility (NIF) neutron sources. An algorithm developed at LLNL was used to unfold the neutron fluence from each of the four DRs, and subsequently, fluence-to-dose conversion factors provided by the American National Standards Institute were used to calculate dose. Additionally, a multistep unfolding process was developed and employed to calculate the effects of both direct (from the source) and indirect (from room return) neutrons. The average error when unfolding the direct DR was less than 8%. The dose from 252 Cf was predicted with only 8% error. The multistep approach allowed for the identification of the low-energy neutrons in the 252 Cf, AmBe, and NIF DRs.

Nuclear Criticality Safety Program (NCSP)

Neutron moderation at IPF

We discuss here the possibility of using the Isotope Production Facility (IPF) at LANSCE to test the feasibility and performance of a graphite cube to create a neutron target. The idea of a neutron target enables the measurement of neutron induced reactions in inverse kinematics. This idea is part of the LANSCE strategy to stay a worldwide leader for neutron-induced research. The proof of-principle is the core of the LDRD project 20240004DR. The first steps are a series of activation experiments with different neutron energy distributions. Figs. 1 and 2 show a graphite cube built and simulated from pieces available at LANSCE. First activation experiments have already been performed at lower neutron energies utilizing (p,n) reactions on Li and Be.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS

Tantalum Experiments in Fully-Reflected Water-Moderated Triangular-Pitched U(6.90)O 2 Fuel Rod Lattices (1.02 cm Pitch)

The United States (US) Department of Energy (DOE) Nuclear Energy Research Initiative funded the design and construction of the Seven Percent Critical Experiment (7uPCX) at Sandia National Laboratories (SNL). The start-up of the experiment facility and the execution of the experiments described here were funded by the DOE Nuclear Criticality Safety Program. The 7uPCX is designed to investigate critical systems with fuel for light water reactors in the enrichment range above 5 % 235 U. The 7uPCX assembly is a water moderated and — reflected array of aluminum-clad U(6.90 %)O 2 fuel rods. Other critical experiments performed in the 7uPCX assembly are documented in LEU-COMP-THERM-078, LEU-COMP-THERM-080, LEU-COMP-THERM 096, LEU- COMP-THERM-097, LEU-COMP-THERM-101, LEU-COMP-THERM-102, and LEU-COMP-THERM-111. Applied interests in neutron-absorbing elements at epithermal and intermediate neutron energy ranges at DOE’s Hanford Site and Savannah River Site were identified through DOE Office of Environmental Management (EM) workshops and needs surveys performed in conjunction with the National Nuclear Security Administration/Nuclear Criticality Safety Program. In response, a team lead by Oak Ridge National Laboratory (ORNL) performed a study evaluating the use of 7uPCX for testing the epithermal cross sections of materials at SNL. This marked the inception of the set of experiments described here. The purpose of these experiments was to measure the effects of tantalum in nearly-critical systems. The tantalum was introduced into the fuel arrays as experiment rods within a central test region. The central test region was designed to target the epithermal neutron energy range by providing a dry cylindrical cavity constructed of aluminum and lined with 0.04 in (0.1016 cm) thick cadmium sheet. The central test region has an outer diameter of 3.75 in (9.525 cm) length of 31 in (78.74 cm) and can hold 85 tantalum rods nominally 0.25 in (0.635 cm) outside diameter and 31.25 in (79.375 cm) long. The critical experiments were done using a set of triangular-pitched grid plates fabricated for these experiments. The grid plate set accommodated a fuel array of a total of 2016 fuel rod positions on a pitch of 0.4 in (1.016 cm) in a series of 21 hexagonal rings positioned around the central test region. The fuel used in these experiments was fabricated using unirradiated 6.90 % enriched UO 2 fuel pellets from fuel elements designed to be used in the internal nuclear superheater section of the Pathfinder boiling water reactor operated in South Dakota by the Northern States Power Company in the 1960s. The fuel elements were obtained from The Pennsylvania State University where they had been stored for many years. The fuel pellets in those fuel elements were removed from the original Incoloy cladding and reclad in 3003 aluminum tubes and end caps for use in the experiments reported here. The eight cases in this experiment series were performed in 2024 in the Sandia Critical Experiments (SCX) at the Sandia Pulsed Reactor Facility by varying the number of fuel rods in the critical assembly. The personnel involved in conducting these experiments included David Ames, Elijah Lutz, Beth Hanson, Patrick Ward, Jason Soares, and Augie Chapa from SNL, as well as Mathieu Dupont and B.J. Marshall from ORNL. Case 1 had no tantalum experiment rods. Case 2 had seven tantalum rods in the center of the central test region. Case 3 had 18 tantalum rods in the third hexagonal ring of the central test region. Case 4 had 19 tantalum rods in the center of the central test region. Case 5 had 30 tantalum rods in the outer most positions of the central test region. Case 6 had 37 tantalum rods in the center of the central test region. Case 7 had 61 tantalum rods in the center of the central test region. Case 8 had 85 tantalum rods filling all positions in the central test region. All eight critical experiments are judged to be acceptable as benchmark experiments.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS

Feasibility of an Active Interrogation System to Classify Waste with He-4 Neutron Spectroscopy

This work investigates a 4 He-detector active interrogation system that leverages neutron spectroscopy to classify nuclear waste streams. MCNP models tested the concept through the simulation of a D-D neutron generator, an array of 4 He detectors, and various waste compositions. The fast-neutron Differential Die-Away signature was augmented with a neutron-energy discrimination signature. This signature isolates induced fission neutrons, the energy of which is greater than that of the D-D monoenergetic spectrum. With the incorporation of this spectroscopic technique, the measurement time decreased by 3–9% (depending on the degree of neutron moderation and absorption presented by the sample), demonstrating how neutron spectroscopy can enhance active interrogation methods. The reduced measurement times would have significant financial and logistical benefits for facilities with large footprints of low-level waste production.

4He detectors

Design of Quasi-Integral Experiments at the Flexible Neutron Source at the University of Tennessee

Nuclear reaction data libraries make use of experimental data that are differential in reaction and neutron energy for evaluation and data that are integral in reaction and energy for validation. In many cases, integral measurements can provide lower experimental uncertainties than differential measurements, but the impact of individual reactions and energies cannot generally be determined from the single experimental observable. “Quasi-integral” or “quasi-differential” measurements, which are integral in one characteristic (energy or reaction) and differential in the other, can often provide a middle ground of lower experimental uncertainties combined with some ability to unpack the impact of individual reactions or energies. Furthermore, the Flexible Neutron Source (FNS) at the University of Tennessee, Knoxville, is a new experimental facility that can perform integral and quasi-integral measurements by removing components of the integral configuration to determine the impact of specific reactions. Possible flux-averaged cross-section measurements, flux perturbation measurements, and neutron downscattering measurements are simulated here to show the value of the FNS to evaluation and validation of nuclear data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS

Analysis of SPND Material Candidates for Real-Time Neutron Spectrum Monitoring Poster

The future of the nuclear industry will be shaped by advanced reactor designs requiring innovative instrumentation for safe operation. A key area of innovation is the ability to accurately and reliably monitor the neutron energy spectrum during operations, which would also enhance the experimental capabilities of existing research reactors. To address this need, our research focuses on the potential use of Self-Powered Neutron Detectors (SPNDs) for real-time neutron spectrum monitoring. We investigated various candidate materials for SPNDs by evaluating their energy-dependent reaction rates. Promising materials were further modeled using MCNP to determine the free electron production per neutron across the neutron energy spectrum, approximating their energy-dependent signal sensitivity. Our findings identified Samarium (Sm) and Gadolinium (Gd) as top candidates for thermal neutrons, Hafnium (Hf) and Thulium (Tm) for epithermal neutrons, and Tantalum (Ta) for fast neutrons. These materials will undergo future experimental validation to confirm the modeled responses and assess their feasibility for real-time neutron spectrum measurements.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN

Commissioning a time-gated camera for fast neutron beamline spatial-energy characterization at LANSCE-WNR spallation source

An energy-resolved fast neutron beam imaging diagnostic has been successfully commissioned at the Weapons Neutron Research (WNR) spallation source within the Los Alamos Neutron Science Center (LANSCE) facility. This diagnostic replaces the existing analog phosphor image plates, which integrate across all neutron energies, as well as other particles, with a near-real-time energy-sensitive imaging capability. The system uses a fast plastic scintillator coupled with an intensified CCD camera. Specifically, the Teledyne Pi-MAX4 camera is coupled with either a 4 mm thick Eljen (EJ) 204 or 228 plastic scintillator. These scintillators are most sensitive to the fast neutrons (0.8-800 MeV) directly from the spallation source rather than low energy background radiation. Experimentally, these plastic scintillators were shown to have sufficiently fast decay to differentiate the bright gamma flash from the spallation neutrons. The spatial resolution is dominated by neutron beam divergence, with minimal additional contributions from scatter and light divergence. The system successfully resolved changes in neutron beam characteristics caused by intentional proton steering variations. Additionally, simulations of scintillator light yield as a function of thickness conducted using PHITS (with Scinful-QMD package) found that increasing scintillator thickness from 4 mm to 6 or 8 mm could potentially increase brightness ~ 3x. This may be explored if there is a need to reduce image acquisition time from several minutes to under one minute.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND

Energy-resolved fast-neutron radiography using an event-mode neutron imaging detector

Energy-resolved fast-neutron radiography is a powerful non-destructive technique that can be used to remotely measure the quantity and distribution of elements and isotopes in a sample. This is done by comparing the energy-dependent neutron transmission of a sample with the known cross-sections of individual isotopes. The reconstruction of the composition is possible due to the unique features (e.g. resonances) in the cross-sections of individual isotopes. At short-pulsed (≲ 1 ns) neutron sources, such information is accessible via time-of-flight neutron imaging in principle, but requires a detector with nanosecond temporal resolution. Conventional neutron detectors can meet this requirement only by heavily compromising spatial resolution or efficiency. Here, we present a unique approach on fast neutron resonance radiography using a scintillator-based event-mode imaging detector at a short-pulsed neutron source, including first results on spatially mapped resonance profiles using MeV neutrons. The event mode approach applied in the presented detector allows recording of individual neutron interactions with nanosecond precision in time and sub-mm resolution in space. As a result, the entire available neutron energy spectrum can be measured for each pulse. At the same time, the use of a thick scintillator screen and lenses to focus the produced light results in a highly flexible field of view and a high interaction probability in the sensitive volume of the detector.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND

AGC-4 As-Run Uncertainty Analysis

The concept of measuring neutron flux (or fluence rate) with activation foils has existed since the late 1940s and is a well-used methodology. Activation foils are selected for their unique isotopic cross sections that create reaction products with desirable properties: relatively simple radioactive decay scheme, measurable quantities of gamma-rays or betas, and half-lives appropriate for the irradiation and decay durations of the experiment. The activation materials, deemed flux wires, fluence wires, dosimeters, or flux foils, are fabricated to have a mass appropriate for the irradiation as well so the measurement using a radiation detector following the irradiation is sufficient but not overwhelming in terms of total activity. Activation measurement results are expressed in terms of reaction rate, which can then be used to “adjust” the neutron spectrum. The Advanced Graphite Creep (AGC)-4 experiment contained 26 flux wire packages, each containing an iron and a niobium wire inside a vanadium capsule. For all stackup positions, the value of fast to thermal neutrons is higher than expected, but the total neutron fluence is near the predicted value of ~2 x 1022 n/cm2. As compared to the predicted neutron spectrum, there are four takeaways in the results as compared to the predicted ATR irradiation: 1) Additional fast (fission) neutrons present, 2) Spectrum hardening due to temperature, 3) Spectrum hardening due to container attenuation, 4) Total neutron fluence is close to predicted values. Since the neutron energy spectrum is a key parameter when attributing neutron damage in materials, the adjusted energy-dependent spectrum and the total neutron fluence results from the dosimeters can be incorporated for future calculations.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS