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DOE OSTI2023

Gamma-ray Measurements from Neutron Pulsed Die-Away Experiments

Pulsed-neutron die-away experiments are a promising experimental method that complement criticality benchmarks for nuclear data validation. The experiments have several advantages that include compatibility with non-fissile material, low benchmark uncertainties, and high sensitivity to absorption and scattering cross sections. When validating thermal neutron scattering laws, small targets are desirable for their large sensitivity to the scattering cross section and angular distribution. Unfortunately, room return or scattering from a shielding box limits the use of the very small targets needed to maximize sensitivity to thermal scattering laws. To address this problem, we propose changing the observable of the experiment from leaked thermal neutrons to γ-rays produced by (n, γ) reactions in the target. If feasible, this change allows removal of the shielding box, achieving higher sensitivity to thermal neutron scattering laws. This study focuses on replicating benchmark pulsed-neutron die-away experiments with γ-rays. We compare the integral parameters with γ-rays to those obtained with neutrons. We also discuss experimental design choices such as detector placement, shielding, and the presence of Cd. The results show the integral parameter with γ-rays is sensitive to detector location with respect to the target when Cd shielding is present. In addition, while Pb shielding around the γ-ray detectors do not seem to affect the integral parameter, the presence of Cd shielding does and adds background γ-rays to the die-away curves making it difficult to calculate the integral parameter.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

Experimental Validation of Thermal Scattering Evaluations

In order to test the performance of new neutron thermal scattering law (TSL) evaluations it is desirable to have experimental data that is highly sensitive to the TSL and provides high fidelity information on the energy dependent performance of TSL evaluations. Three relevant experiments are discussed including: accurate thermal total cross section measurements, thermal neutron die-away experiments, and neutron leakage experiments. The experimental setups and results are reviewed, and examples provided for some moderators including polyethylene, Plexiglas, and YHx. For the experiments preformed thus far, there is generally good agreement between the measured total cross section and simulations using current TSL evaluations, however in certain energy ranges differences were observed. Similarly, neutron die-away and leakage measurements for samples at room temperature are in good agreement with data computed from TSLs, however leakage measurements for polyethylene at 29K show discrepancies with TSL evaluations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Neutron Pulsed Die-Away Experiments at LLNL [Slides]

This presentation discusses why PNDA is ideal for TSL validations as it does not require fissile material, it has very simple target shapes and compositions, it is only sensitive to absorption and scattering of target medium, and that well conducted experiments have uncertainties of 0.1% - 0.5%. The presentation concludes by examining PNDA’s advantages and its role in nuclear data validations as it offers a cost-effective experiment for an integral benchmark, it provides the ability to focus on specific cross section data validation including thermal neutron absorption and thermal scattering laws, and the low experimental uncertainty makes it an excellent benchmark candidate. Additionally, it is easily tunable and can facilitate temperature dependent cross section validation by cooling or heating up targets.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Preliminary Design of a New Pulsed-Neutron Die--Away Experiments with Absorbers (IER-552 CED-1)

This report presents the preliminary design (CED-1) of IER-552, pulsed-neutron die-away (PNDA) experiments with absorbers, to be conducted by Lawrence Livermore National Laboratory (LLNL). The goal of the PNDA experiments with absorbing materials is to produce high-quality, low-cost integral benchmarks that can be used to validate cross sections that are high priority nuclear data for the Department of Energy’s Nuclear Criticality Safety Program (NCSP). PNDA experiments can be used to generate nuclear data validation benchmarks quickly and cheaply, as they do not require fissile material or a nuclear facility to conduct them. The original PNDA experiments were set up at LLNL under IER-501. Extending the PNDA experiments to include absorbing materials leverages existing facilities and resources at LLNL to validate cross sections, with a basic experiment design that uses a neutron generator to impinge a short, mono-energetic neutron pulse on a poisoned, moderating target sample. The neutron pulse lasts 100 µs, after which the neutron population in the sample reaches thermal equilibrium and later spatial equilibrium. In this fully equilibrized state, the neutron population has a characteristic decay-time eigenvalue. The eigenvalue can be used as an integral parameter to validate nuclear data involved with neutron scattering and absorption. Two observables can be measured: the neutron population and the population of secondary γ-rays produced by inelastic and capture reactions. This report explores the feasibility of both approaches. For γ-ray measurements, this allows for direct measurement of reactions of interest for validation. During the neutron burst time, inelastic (prompt) γ-rays dominate, and these data can be isolated for validation of neutron inelastic scattering data. After the pulse ends, neutron capture (delayed) γ-rays dominate and are produced by many reaction channels as neutrons slow down to thermal energies. Two sets of γ-ray spectra (inelastic, capture) can be produced for validation. Additionally, the time-dependent decay of the capture γ-ray population when the neutron population is thermalized and in its fundamental mode can be used for validation. Two experiments can be imagined where pulsed neutrons are used to validate the nuclear data of absorbing materials. The first integrates well into the existing PNDA testbed at LLNL. The absorber material would be introduced into a moderating target and the same neutron generator, neutron detectors, electronics, and shielding box used for IER-501 would be employed. From the same experimental setup, many absorbing materials can be validated by simply changing the neutron poison in the moderator. The only significant modification would be the introduction of a γ-ray detector. Such an experiment would primarily serve to validate nuclear data in the thermal energy range. The second kind of experiment would validate the fast and epithermal energy range. It would involve pulsing neutron into a bare assembly of the absorber material and measuring the die-away of neutrons. The fast leakage of such an assembly requires nanosecond neutron-generator pulse widths and fast detectors/electronics that could measure ~200 ns die-away curves. This kind of experiment would ideally be performed at a cyclotron, like that available at Lawrence Berkeley National Laboratory.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Proposed Methodology for Evaluating and Validating TSLs [Slides]

This presentation begins by providing an overview of the research and discusses recent efforts in validating thermal neutron scattering cross sections, including differential cross section measurements at ORNL for evaluation and validation, total cross section measurements at RPI, pulsed-neutron die-away experiments at LLNL, and integral criticality experiments by LLNL. The presentation also proposes a methodology not only for validating thermal scattering files that utilizes all available experimental data, but also for evaluating new libraries as demonstrated on polystyrene. In conclusion, polystyrene evaluation was conducted using multiple experiments, including differential and integral. The proposed methodology has been shown to improve neutron transport and files have been submitted to NNDC for inclusion in ENDF/B-VIII.1 release. MCT-012 & PCM-002 has been relatively insensitive to changes in $\mathcal{S}(α,β)$. The research found that differences in differential results don’t always propagate to differences in integral results, hence why evaluation of differential data important. Future work on the project is also discussed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Experiments for validation of TSL evaluations [Slides]

There is a recent revival of thermal scattering evaluation capabilities and there are many new evaluations available in ENDF-8.0 and elsewhere. This creates a need for experimental validation other than criticality benchmarks. Thermal scattering libraries (TSL) provide information to describe the double differential thermal scattering at different moderator temperatures. For moderators, the biggest effect of TSL is the thermal scattering cross section.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Overview of Nuclear Data Measurement and Analysis at RPI [Slides]

This presentation discusses the experimental, simulation, and nuclear data methods that were validated for the RPI γ-Multiplicity Detector. When the neutron capture γ-cascade data is well-known, the γ-emission spectra can be accurately calculated using the modified simulation tools. The RPI γ-Multiplicity Detector system is now ready for analysis and recommendations for isotopes with deficiencies in γ-ray data. The presentation also discusses future work which includes developing a method for analyzing and adjusting nuclear data for 59 Co, 55 Mn and other measured isotopes including 181 Ta. Additionally, future work includes comparing experimental γ-emission spectra with MCNP-6.2/DICEBOX simulations for 238 U and 235 U. In summation, new capture and transmission measurements for 54 Fe will help improve resonance parameter evaluation. Neutron capture gamma cascade spectra and yields were measured in the resolved resonance region and compared to evaluations. In addition, the pulsed neutron die-away method was developed as a tool to provide data for validation of TSLs.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Overview of Nuclear Data Measurement and Analysis at RP [Slides]

This presentation details neutron capture in 54 Fe along with neutron capture yield and γ-ray cascade spectra measurements. The presentation then follows with thermal neutron die-away measurements and concludes with URR improvement to SAMMY.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2025

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↗
DOE OSTI2026

Performance evaluation of neutron noise analysis in detecting special nuclear materials

Reliable and rapid inspection techniques play a vital role in preventing illicit trafficking of special nuclear materials. Active interrogation systems using neutrons produced by portable, high-flux deuterium-deuterium or deuterium-tritium neutron generators are being actively developed as a secondary scanning tool for this purpose. In this study, a neutron noise analysis-based approach for detecting unshielded and shielded special nuclear materials by using a pulsed deuterium-tritium neutron generator was evaluated. Here, this approach analyzes the fluctuation of neutron counts. Its performance was quantified with regard to time-to-detection to achieve a minimum probability of detection of 99% and a probability of false alarm of less than 1% considering various amounts of special nuclear materials and different shielding configurations. It was demonstrated that this approach could detect 17 uranium slugs in 5 s given a neutron generator yield of 8.1 × 10 7 n/s. These slugs could be detected within a reasonable time frame (200 s) when they were shielded by 10.16 cm of high-density polyethylene. The results obtained using the neutron noise analysis approach were compared with those obtained using the commonly used differential die-away analysis technique, a sensitive technique for detecting the presence of fissile materials by utilizing the prompt fission neutrons produced when the source neutrons from a neutron generator are completely diminished. For example, the time to detect 2 unshielded uranium slugs was 2.1 s when using the differential die-away analysis technique; it increased to 93 s for the neutron noise analysis approach. Although the noise analysis-based approach exhibits an overall performance which is not as good as that of differential die-away, neutron noise provides an alternative method for effective detection of special nuclear materials.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2026

Conceptual design study of neutron detectors for safeguards measurement of an irradiated pebble

Nuclear material control and accounting (MC&A) of pebble-bed reactors (PBRs) is challenging because a PBR utilizes hundreds of thousands of identical, unmarked pebbles that are continuously recirculated through the core. To develop tools that enable the implementation of international safeguards, especially in the context of MC&A of spent pebbles, we designed and simulated three neutron detection concepts to determine fissile content in individual pebbles: a differential die-away (DDA) detector, a californium interrogation prompt neutron (CIPN) detector, and a passive neutron albedo reactivity (PNAR) detector using Monte Carlo calculations. Burnup calculations were performed on the spent pebbles from the PBMR-400 classic PBR. The varying neutron and gamma source terms, and isotopic compositions in the spent pebbles calculated at various burnup levels were used in the neutron detector models. DDA was found to be sensitive to the number of passes a pebble has had through the core and to the fissile content contained in a spent pebble. Optimization in the DDA design further increased the neutron count rates and thus reduced counting uncertainty. Meanwhile, passive neutron counting using the same detector body could distinguish pebbles with different numbers of passes, but its response was dominated by neutron-emitting actinides and was not sensitive to fissile content. On the other hand, the PNAR technique was not viable for a single pebble but performed reasonably for a 27-pebble array, which suggested potential use for verification measurements of containers filled with 27 or more spent pebbles.

CIPN↗
DOE OSTI2023

Passive and active neutron signatures of 233 U for nondestructive assay

The thorium fuel cycle is emerging as an attractive alternative to conventional nuclear fuel cycles, as it does not require the enrichment of uranium for long-term sustainability. The operating principle of this fuel cycle is the irradiation of 232 Th to produce 233 U, which is fissile and sustains the fission chain reaction. 233 U poses unique challenges for nuclear safeguards, as it is associated with a uniquely extreme γ-ray environment from 232 U contamination, which limits the feasibility of the γ-ray-based assay, as well as more conservative accountability requirements than for 235 U set by the International Atomic Energy Agency. Consequently, instrumentation used for safeguarding 235 U in traditional fuel cycles may be inapplicable. It is essential that the nondestructive signatures of 233 U be characterized so that nuclear safeguards can be applied to thorium fuel-cycle facilities as they come online. In this work, a set of 233 U 3 O 8 plates, containing 984 g 233 U, was measured at the National Criticality Experiments Research Center. A high-pressure 4 He gaseous scintillation detector, which is insensitive to γ-rays, was used to perform a passive fast neutron spectral signature measurement of 233 U 3 O 8 , and was used in conjunction with a pulsed deuterium-tritium neutron generator to demonstrate the differential die-away signature of this material. Furthermore, an array of 3 He detectors was used in conjunction with the same neutron generator to measure the delayed neutron time profile of 233 U, which is unique to this nuclide. These measurements provide a benchmark for future nondestructive assay instrumentation development, and demonstrate a set of key neutron signatures to be leveraged for nuclear safeguards in the thorium fuel cycle.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Burnup Monitoring for Pebble Bed Reactor Systems

A pebble burnup monitoring system is a required component for domestic reactor safety and safeguards applications associated with pebble bed reactors (PBRs). One of the main requirements of a PBR burnup monitoring system is that it needs to be capable of rapid measurements to assess the burnup of each individual pebble to determine whether to recirculate it in the reactor or discard it as spent fuel. This report considers three different approaches for a burnup monitoring system for pebbles discharged from the reactor core in a pebble bed modular reactor-400: • passive gamma spectrometry measurement, • passive neutron coincidence measurement, and • active neutron counter based on the differential die-away technique. Conceptual designs have been created for each of these detectors, and preliminary analysis has been performed using Monte Carlo N-Particle and Oak Ridge Isotope Generation code simulations. The advantages and practical limitations (e.g., high radiation background) of each system were identified. Simulations suggest that each of the three measurement techniques can be successfully employed to distinguish between pebbles based on their number of passes through the core and to quantify the burnup of pebbles.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2023

Boron coated straw-based neutron multiplicity counter for neutron interrogation of TRISO fueled pebbles

Pebble bed reactors (PBRs) can improve the safety and economics of the nuclear energy production. PBRs rely on TRIstructural-ISOtropic (TRISO) fuel pebbles for enhanced fission product retention. Accurate characterization of individual fuel pebbles would enable the validation of computational models, efficient use of TRISO fuel, and improve fuel accountability. Here, we have developed and tested a new neutron multiplicity counter (NMC) based on 192 boron coated straw (BCS) detectors optimized for 235 U assay in TRISO fuel. The new design yielded a singles and doubles neutron detection efficiency of 4.71% and 0.174%, respectively, and a die-away time of 16.7 μs. The NMC has a low intrinsic gamma-ray detection efficiency of 8.71 x 10 –8 at an exposure rate of 80.3 mR/h. In simulation, a high-efficiency version of the NMC encompassing 396 straws was able to estimate the 235 U in a pebble with a relative uncertainty and error both below 2% in 100 s.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗