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Pulsed, Photonuclear-induced, Neutron Measurements of Nuclear Materials with Composite Shielding

Active measurements were performed using a 10-MeV electron accelerator with inspection objects containing various nuclear and nonnuclear materials available at the Idaho National Laboratory’s Zero Power Physics Reactor (ZPPR) facility. The inspection objects were assembled from ZPPR reactor plate materials to evaluate the measurement technologies for the characterization of plutonium, depleted uranium or highly enriched uranium shielded by both nuclear and non-nuclear materials. A series of pulsed photonuclear, time-correlated measurements were performed with unshielded calibration materials and then compared with the more complex composite shield configurations. The measurements used multiple 3He detectors that are designed to detect fission neutrons between pulses of an electron linear accelerator. The accelerator produced 10-MeV bremsstrahlung X-rays at a repetition rate of 125 Hz (8 ms between pulses) with a 4-us pulse width. All inspected objects were positioned on beam centerline and 100 cm from the X-ray source. The time-correlated data was collected in parallel using both a Los Alamos National Laboratory-designed list-mode acquisition system and a commercial multichannel scaler analyzer. A combination of different measurement configurations and data analysis methods enabled the identification of each object. This paper describes the experimental configuration, the ZPPR inspection objects used, and the various measurement and analysis results for each inspected object.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Active Well Counting Using New PSD Plastic Detectors

This report presents results and analysis from a series of proof-of-concept measurements to assess the suitability of segmented detectors constructed from Eljen EJ-299-34 PSD-plastic scintillator with pulse-shape discrimination capability for the purposes of quantifying uranium via active neutron coincidence counting. Present quantification of bulk uranium materials for international safeguards and domestic materials control and accounting relies on active neutron coincidence counting systems, such as the Active Well Coincidence Counter (AWCC) and the Uranium Neutron Coincidence Collar (UNCL), that use moderated He-3 proportional counters along with necessarily low-intensity 241Am(Li) neutron sources. Scintillation-based fast-neutron detectors are a potentially superior technology to the existing AWCC and UNCL designs due to their spectroscopic capability and their inherently short neutron coincidence times that largely eliminate random coincidences and enable interrogation by stronger sources. One of the past impediments to the investigation and adoption of scintillation counters for the purpose of quantifying bulk uranium was the commercial availability of scintillators having the necessary neutron-gamma pulse-shape discrimination properties only as flammable liquids. Recently, Eljen EJ-299-34 PSD-plastic scintillator became commercially available. The present work is the first assessment of an array of PSD-plastic detectors for the purposes of quantifying bulk uranium. The detector panel used in the present work was originally built as the focal plane for a fast-neutron imager, but it was repurposed for the present investigation by construction of a stand to support the inner well of an AWCC immediately in front of the detector panel. The detector panel and data acquisition of this system are particularly well suited for performing active-well fast-neutron counting of LEU and HEU samples because the active detector volume is solid, the 241Am(Li) interrogating neutrons are largely below the detector threshold, and the segmented construction of the detector modules allow for separation of true neutron-neutron coincidences from inter-detector scattering using the kinematics of neutron scattering. The results from a series of measurements of a suite of uranium standards are presented, and compared to measurements of the same standards and source configurations using the AWCC. Using these results, the performance of the segmented detectors reconfigured as a well counter is predicted and outperforms the AWCC.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

The scientific case for concurrent neutron and X-ray scattering and spectroscopy

The interrogation of materials with X-rays or neutrons to determine structure, energetics, and dynamics is fundamental to advancing physical and chemical materials science and enabling innovative material technologies. A persistent challenge in materials development is that progress depends on understanding structure and dynamics across multiple length and time scales in increasingly complex, multicomponent systems featuring interfaces, heterogeneity, and hierarchical organization. Despite rapidly growing demands on materials characterization, current experimental approaches are almost exclusively based on isolated X-ray or neutron scattering and spectroscopy, reflecting a paradigm largely unchanged for decades. To assess the scientific need for a new experimental paradigm, a 3-day workshop sponsored by the U.S. National Science Foundation (NSF) was held at the SpringHill Suites, San Jose, California, from June 2 to 4, 2022. The workshop brought together 70 national and international experts who critically evaluated opportunities enabled by concurrent neutron and X-ray (NeX) scattering, spectroscopy, and imaging experiments. The participants reached a clear consensus that establishing NeX capabilities is crucial for advancing the science of complex materials in the United States. This report illustrates the scientific drivers for NeX experiments through representative examples spanning biomaterials, energy materials, soft matter, nanomaterials, quantum materials, geoscience, and applied materials research. The complementarity of neutrons and X-rays is essential for robust model development and refinement, particularly in multiphase and multicomponent systems. While joint refinement of data from separate experiments is valuable, concurrent measurements uniquely eliminate uncertainties arising from sample evolution, environmental drift, and irreproducibility associated with experiments performed at different locations and times. Realizing NeX capabilities will require the development of new instrumentation, data analysis frameworks, and robust sample environments compatible with both neutron and X-ray probes. Addressing these challenges will enable unambiguous interpretation of complex materials behavior and open new frontiers in materials research.

X-ray↗

Elemental analysis using temporal gating of a pulsed neutron generator

Technologies related to determining elemental composition of a sample that comprises fissile material are described herein. In a general embodiment, a pulsed neutron generator periodically emits bursts of neutrons, and is synchronized with an analyzer circuit. The bursts of neutrons are used to interrogate the sample, and the sample outputs gamma rays based upon the neutrons impacting the sample. A detector outputs pulses based upon the gamma rays impinging upon the material of the detector, and the analyzer circuit assigns the pulses to temporally-based bins based upon the analyzer circuit being synchronized with the pulsed neutron generator. A computing device outputs data that is indicative of elemental composition of the sample based upon the binned pulses.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Optimization of Binning Parameters in the Feynman Variance-to-Mean Method for Delayed Neutron Reinterrogation

The focus of this work is to determine the optimal input parameters for analyzing active interrogation data that utilizes the physics of the delayed neutron re-interrogation technique. This work compares the signature from an active neutron measurement of a highly enriched uranium (HEU) system to an active background measurement (i.e., without the HEU item in place). The item being measured represents a 21.8 kg metal sphere of HEU (93 weight percent) assembled from a subset of the Rocky Flats (RF) uranium hemishells. The detection system consisted of two NoMAD neutron multiplicity detectors, a SNAP III neutron detector, and a Thermo Fisher P211 pulsed 14 MeV neutron source. In addition, varying analyses of the NoMAD list-mode detector data are performed to determine whether it is preferential to use a particular analysis bin size for producing Feynman histograms, selection of pulses to prevent discrepancies from buildup, or window of time during the pulsed neutron interrogation. This work is still currently ongoing.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

The Scientific Case for Concurrent Neutron and X-ray Scattering and Spectroscopy

The interrogation of materials with X-rays or neutrons to determine the structure, energetics, and dynamics of materials is fundamental to advancing materials' physical and chemical science and developing innovative material technologies. A transcending challenge in developing novel materials is that progress hinges on understanding the structure and dynamics across multiple time and length scales in complex materials that feature multiple components, interfaces, and compositions. Despite the ever-growing demands on materials’ characterization, existing approaches are almost exclusively based on isolated X-ray or neutron scattering, i.e., an approach commensurate with the more narrowly defined needs of fifty years ago. A three-day workshop sponsored by the U.S. National Science Foundation (NSF) analyzed the demand for concurrent neutron and X-ray (NeX) experiments. It was held at the Spring Hill Suites, San Jose, California, from June 2 to 4, 2022. In this workshop, 70 national and international experts ascertained the crucial need to establish NeX capabilities to advance the science of complex materials and systems in the US. Here, we illustrate the need for NeX scattering and spectroscopy experiments by showcasing examples that span areas as diverse as biomaterials, energy science, soft matter, and nanomaterials. To provide NeX capability will require new instrumentation that enables concurrent experiments. Affected areas include chemistry, soft matter, quantum materials, pure and applied chemistry, bioscience, geoscience, and applied materials. NeX benefits research outcomes due to the complementarity of the two techniques, which is essential for better model refinement. While joint refinement of data from separate neutron and X-ray experiments is critical to avoid ambiguities, especially in multiphase-multicomponent materials, concurrent experiments overcome scientific and technical barriers associated with single measurements, separated by location and, thus, time. Among all the examples, these factors introduce uncertainties in the results that complicate data analysis. [1,2] [3] While models are strongly sample-dependent, the principles of joint refinement are generally applicable to these disciplines, including the development of advanced parameterization, modeling, and analysis techniques that also consider the temporal and spatial resolutions of the two methods, leading to unambiguous data interpretation. Solutions for technical barriers must be found to realize NeX experiments, including developing robust sample environments that meet the optical requirements of neutrons and X-rays.

36 MATERIALS SCIENCE↗

High-fidelity photoneutron detection via neutron activation analysis

To interdict illicit radioactive sources and prevent nuclear terror, governments have deployed portal monitor systems at ports of entry. Such portal monitors rely upon the detection of spontaneously-emitted radiation signatures, however, detection scenarios become more challenging for highly enriched uranium, which emits relatively few spontaneous radiation signatures. Photon active interrogation techniques can augment current cargo inspection scenarios and improve detection capabilities for illicit nuclear material. A high-energy photon interrogation source can induce photofission in nuclear material, producing strong radiation signatures for detection. Prompt fission signals are of specific interest because prompt neutrons are greater than 99% of the fission signal. When using detectors capable of spectroscopy, e.g., pulse shape discrimination-capable organic scintillators, the intense interrogating source often will cause pulse pile-up, degrading particle classification. In this work, we demonstrate photoneutron detection via neutron activation of aluminum and iron. The experiments rely upon nuclear reactions that can only be induced by neutrons, and are robust against pile-up, thereby providing high-confidence neutron rates. In this work, we apply neutron activation analysis for the detection of high-energy neutrons produced by high-energy photon irradiation; the depleted uranium sample was irradiated with a 9-MeV bremsstrahlung beam. We find that the irradiated depleted uranium produced an aluminum activation flux of 1.77 × 10 5 n cm –2 s –1 and an iron-56 activation flux of 1.05 × 10 5 n cm –2 s –1 . Furthermore, the ability to detect radioactivity induced by neutrons created in (, n) and photofission reactions demonstrates a new approach for photon active interrogation to identify nuclear materials.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Low-cost, multi-mode detector solutions

Low-cost radiation detectors capable of providing efficient gamma-ray and neutron detection are essential in passive nuclear monitoring systems such as radiation portal monitors (RPMs) and detection of Special Nuclear Materials (SNM) through Active Interrogation (AI). Here, three low-cost detector solutions are discussed—(1) Large-area polystyrene-based plastic scintillators for AI (2) Pulse Shape Discrimination (PSD) capable plastic scintillators doped with heavy-metals for imparting gamma-ray spectroscopy (3) Composite detector technology based on inorganic scintillator submerged into the plastic scintillator, for detection of thermal and fast neutrons in addition to gamma-ray spectroscopy. Composite detectors using inorganic component such as Cs 2 LiYCl 6 (CLYC), Cs 2 LiLaBr x Cl 6-x (CLLBC), or CsI:Tl have been developed up to 4” sizes. Neutron and gamma efficiencies are compared for samples with different inorganic loading.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Fission signal detection using helium-4 gas fast neutron scintillation detectors

We demonstrate the unambiguous detection of the fission neutron signal produced in natural uranium during active neutron interrogation using a deuterium-deuterium fusion neutron generator and a high pressure {sup 4}He gas fast neutron scintillation detector. The energy deposition by individual neutrons is quantified, and energy discrimination is used to differentiate the induced fission neutrons from the mono-energetic interrogation neutrons. The detector can discriminate between different incident neutron energies using pulse height discrimination of the slow scintillation component of the elastic scattering interaction between a neutron and the {sup 4}He atom. Energy histograms resulting from this data show the buildup of a detected fission neutron signal at higher energies. The detector is shown here to detect a unique fission neutron signal from a natural uranium sample during active interrogation with a (d, d) neutron generator. This signal path has a direct application to the detection of shielded nuclear material in cargo and air containers. It allows for continuous interrogation and detection while greatly minimizing the potential for false alarms.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

A Permanent-Magnet Microwave Ion Source for a Compact High-Yield Neutron Generator

We present recent work on the development of a microwave ion source that will be used in a high-yield compact neutron generator for active interrogation applications. The sealed tube generator will be capable of producing high neutron yields, 5x1011 n/s for D-T and ~;;1x1010 n/s for D-D reactions, while remaining transportable. We constructed a microwave ion source (2.45 GHz) with permanent magnets to provide the magnetic field strength of 87.5 mT necessary for satisfying the electron cyclotron resonance (ECR) condition. Microwave ion sources can produce high extracted beam currents at the low gas pressures required for sealed tube operation and at lower power levels than previously used RF-driven ion sources. A 100 mA deuterium/tritium beam will be extracted through a large slit (60x6 mm2) to spread the beam power over a larger target area. This paper describes the design of the permanent-magnet microwave ion source and discusses the impact of the magnetic field design on the source performance. The required equivalent proton beam current density of 40 mA/cm2 was extracted at a moderate microwave power of 400 W with an optimized magnetic field.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

New NDA Methods for Thorium Fuel Cycle Safeguards (Final Report)

This project developed portable Neutron Resonance Transmission Analysis (pNRTA) as a new non-destructive assay (NDA) method for thorium fuel cycles safeguards and other applications where multiple isotopes must be measured when present together. pNRTA leverages epithermal neutron resonances to assay multiple safeguards-relevant isotopes (e.g., 233 U and 235 U) when they are present together in a sample. Existing techniques are challenged by this task, driving the need for new active interrogation methods. With selected detectors, pNRTA works in high gamma-ray backgrounds from fission and activation products and 232 U progeny expected in thorium fuel cycle samples. This project leveraged a pNRTA system developed at Pacific Northwest National Laboratory (PNNL) and collaboration with the Massachusetts Institute of Technology (MIT). The system uses a commercially available deuterium-tritium (DT) neutron generator at short standoff (2 m). Key achievements in this project included: first-of-a-kind pNRTA quantitative measurements of 233 U oxide samples, an assessment of neutron detector technologies suitable for pNRTA in high gamma-ray background environments, experimentally demonstrating quantitative assay of samples containing 233 U and 235 U, and modeling studies showing the applicability of pNRTA to a wide range of material forms. Further, a custom algorithm was developed at MIT, which provided mean bias of 9% and relative standard deviation of 36% in assaying 233 U, 235 U, 238 U, and 232 Th content in eight measured samples. These outcomes form a solid technical basis for pNRTA as a new promising capability for international safeguards verification that is portable, non-destructive, quantitative, and isotopic specific.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Directed Neutron Beams From Inverse Kinematic Reactions

Kinematic focusing of an emitted fairly mono-energetic neutron beam by the use of inverse-kinematic reactions, i.e. where the projectile mass is greater than the target atom's mass, can provide for the utilization of a significant fraction of the fast neutron yield and also provide for a safer radiation environment. We examine the merit of various neutron production reactions and consider the practicalities of producing the primary beam using the suitable accelerator technologies. Preliminary progress at the NSWC-Carderock Positive Ion Accelerator Facility is described. Possible important applications for this type of neutron-based system can be both advanced medical imaging techniques and active ''stand-off'' interrogation of contraband items.

43 PARTICLE ACCELERATORS↗

Development and characterization of a high yield transportable pulsed neutron source with efficient and compact pulsed power system

The results of characterization experiments carried out on a newly developed dense plasma focus device based intense pulsed neutron source with efficient and compact pulsed power system are reported. Its high current sealed pseudospark switch based low inductance capacitor bank with maximum stored energy of ∼10 kJ is segregated into four modules of ∼2.5 kJ each and it cumulatively delivers peak current in the range of 400 kA–600 kA (corresponding to charging voltage range of 14 kV–18 kV) in a quarter time period of ∼2 μs. The neutron yield performance of this device has been optimized by discretely varying deuterium filling gas pressure in the range of 6 mbar–11 mbar at ∼17 kV/550 kA discharge. At ∼7 kJ/8.5 mbar operation, the average neutron yield has been measured to be in the order of ∼4 × 10{sup 9} neutrons/pulse which is the highest ever reported neutron yield from a plasma focus device with the same stored energy. The average forward to radial anisotropy in neutron yield is found to be ∼2. The entire system is contained on a moveable trolley having dimensions 1.5 m × 1 m × 0.7 m and its operation and control (up to the distance of 25 m) are facilitated through optically isolated handheld remote console. The overall compactness of this system provides minimum proximity to small as well as large samples for irradiation. The major intended application objective of this high neutron yield dense plasma focus device development is to explore the feasibility of active neutron interrogation experiments by utilization of intense pulsed neutron sources.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Pulsed-Neutron Experiments at the Inherently Safe Subcritical Assembly

The pulsed neutron technique is a powerful, dynamic method to assay the reactivity of a multiplying system. This work presents the novel application of the pulsed neutron technique to the Inherently Safe Subcritical Assembly, an experimental configuration accepted by the International Criticality Safety Benchmark Evaluation Project Handbook. The experiments were replicated with COG11.3, a continuous-energy Monte Carlo code. The pulsed neutron data were analyzed using the Sjöstrand and Gozani area-ratio methods and by extracting the prompt neutron decay constant. Subsequent static k-eigenvalue and 𝛼-eigenvalue simulations were also performed for the same configurations. Neutron detector dead-time effects from the experiments were corrected using the Backwards Extrapolation Method and shown to have a negligible impact on the estimated reactivities. The results highlight that capturing time-dependent effects like delayed neutron precursor buildup are essential to accurately reproduce experimental results. They also highlight the importance of shielding the detectors from generator source neutrons in deeply subcritical configurations.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗