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An Artificial Neural Network System for Photon-Based Active Interrogation Applications

Active interrogation (AI) is a promising technique to detect shielded special nuclear materials (SNMs). At the University of Michigan, we are developing a photon-based AI system that uses bremsstrahlung radiation from an electron linear accelerator (linac) as an ionizing source and stilbene organic scintillating detectors for neutron detection. Stilbene scintillators are sensitive to fast neutrons and photons and have excellent pulse shape discrimination (PSD) capabilities. The traditional charge integration (CI) method commonly used for PSD analysis eliminates piled-up pulses and relies on a particle discrimination line to separate neutrons and photons. The presence of the intense photon flux during AI creates a significant number of piled-up events in the stilbene scintillator, thereby posing a great challenge to the traditional CI method. Identifying true single neutron pulses becomes challenging due to the presence of a pile-up cloud and overlapping neutron, photon and pile-up clouds in the PSD analysis. To mitigate the effect of pulse pile up and identify true single neutron pulses from stilbene scintillators, an artificial neural network (ANN) system is developed. The developed ANN system identifies single neutron pulses and neutron-photon combinations from piled-up events. The results obtained from a 252Cf measurement in the presence of the intense photon flux show that the developed ANN system outperforms the traditional CI method. Since many piled-up events lie above the particle discrimination line, they get misclassified as neutrons by the traditional CI method resulting in 25% overestimation of the net neutron count rate during the linac pulse. The overall net neutron count rate (single and restored neutrons) during the linac pulse, estimated by the ANN system is 60% of the ground truth. Energy spectroscopy of the ANN attributed single neutron pulses further provides evidence on the detection of prompt fission neutrons from the 252Cf fission source.

42 ENGINEERING↗

Measurements of Short-Lived Isomers from Photofission as a Method of Active Interrogation for Special Nuclear Materials

Isomeric fission products, such as 134m Te (T 1/2 = 164 ns) and 136m Xe (T 1/2 = 2.95 μs), are proposed as a signature of special nuclear materials in active interrogation applications. To test this conjecture, monoenergetic 9, 11, and 13 MeV photons from the HIγS facility are used to induce fission of 235 U, 238 U, and 239 Pu targets. The de-excitation γ rays of the isomers are measured using time-gated spectroscopy with high-purity germanium detectors. The 134m Te and 136m Xe isomers are detected and identified by the energy and decay half-life of their characteristic γ-ray transitions. The ratio of yields for these two signature γ rays, corresponding to 134m Te/( 136m Xe + 136 I), is found to be strongly correlated with the identity of the fissioning nuclei. These results show that fission-product isomers may be used in active interrogation to detect and identify special nuclear materials, even providing information on the isotopic enrichment. In conclusion, the feasibility of an active interrogation scenario using a bremsstrahlung beam is discussed.

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↗

12 C(p,p') 12 C Reaction ( E p =19.5–30 MeV) for Active Interrogation of Special Nuclear Material

Passive detection of special nuclear material (SNM) is challenging due to its inherently low rate of spontaneous emission of penetrating radiation, the relative ease of shielding, and the fluctuating and frequently overwhelming background. Active interrogation, the use of external radiation to increase the emission rate of characteristic radiation from SNM, has long been considered to be a promising method to overcome those challenges. Current active-interrogation systems that incorporate radiography tend to use bremsstrahlung beams, which can deliver high radiation doses. Low-energy ion-driven nuclear reactions that produce multiple monoenergetic photons may be used as an alternative. The 12 C ( p , p ' ) 12 C reaction is one such reaction that could produce large yields of highly penetrating 4.4- and 15.1-MeV gamma rays. This reaction does not directly produce neutrons below the approximately 19.7 MeV threshold, and the 15.1-MeV gamma-ray line is well matched to the photofission cross section of 235 U and 238 U . In this article, we report the measurements of thick-target gamma-ray yields at 4.4 and 15.1 MeV from the 12 C ( p , p ' ) 12 C reaction at proton energies of 19.5, 25, and 30 MeV. Measurements are made with two 3 -in. EJ-309 cylindrical liquid scintillation detectors and thermoluminescent dosimeters placed at 0 ° and 90 ° , with an additional 1.5 -in. Na I ( Tl ) cylindrical scintillation detector at 0 ° . We estimate the highest yields of the 4.4- and 15.1-MeV gamma rays of 1.65 × 10 10 and 4.47 × 10 8 sr - 1 μ C - 1 at a proton energy of 30 MeV, respectively. The yields in all experimental configurations are greater than in a comparable deuteron-driven reaction that produces the same gamma-ray energies— 11 B ( d , n γ ) 12 C . However, a significant increase of the neutron radiation dose accompanies the proton energy increase from 19.5 to 30 MeV.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Active Interrogation of the Snyder Shells using a SEA-7 Betatron

The shielded highly enriched uranium (HEU) problem is one that still needs to be addressed. As a first step towards a solution, the Snyder shells (depleted uranium) were actively interrogated with a SEA-7 betatron in various configurations using an MC15 as a detector. These configurations include masses from 0.55 to 5.1 kg, as well as 5.1 kg in a steel container. A strong electromagnetic field (EMF) background was identified in previous work, but the results in this work show all configurations produce a signal well above the background. An initial simulation capability was developed that produces the expected flux profile from the SEA-7 betatron, but further work needs to be done to determine the magnitude of the flux via a combination of experiment and simulation validation. Depleted uranium generally produces more neutrons than HEU, so additional future work will need to include similar measurements of HEU to confirm similar performance of the technique. Additionally the EMF background needs to be better characterized as a function of distance and angle from the SEA-7 source and mitigation techniques explored.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Comparison of active interrogation methods for source location in a scattering and absorbing medium, consisting of PGNAA, and an AmBe quasi-forward biased directional source

Source location of Special Nuclear Material (SNM) encompassing 95% 235 U and 239 Pu is identified by utilizing a directional source from Patent No: US20190013109A1 using Prompt Gamma Neutron Activation Analysis (PGNAA) and neutron spectroscopy simulated with Monte-Carlo N-Particle transport 6.2 (MCNP). BC-408, HPGe, LaBr 3 detector arrays were used to identify the location of the SNM using total counts incident on each detector, and PGNAA photopeaks from HPGe and LaBr 3 detector arrays in a polyethylene shield. The conducted simulations varied the volume and location of the SNM in the MCNP input files to observe how the source location method behaved. PGNAA photopeaks used for source identification include 61 keV from fission, 2.223 MeV prompt gamma from hydrogen, 511 keV annihilation, and a single and double escape peaks from the prompt gamma interaction from hydrogen. The capabilities of each detector systems to acquire well resolved photopeaks with a 1% relative error or less, and total relative error for F4 and F8 tallies were less than 0.015% relative error. Source predictions of the SNM with uneven amounts of polyethylene shielding between the source and detectors was observed to overpredict and give invalid source location predictions. Source locations of the SNM with even amounts of polyethylene material between the source and each detector were found to be valid. With a 1 Ci 241 Am source activity, it was determined that 1630 s were needed to obtain the results for each detector system with the quasi-forward directional AmBe source. Coupling source and material identification together would increase acquisition time but would only require one system to determine.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Gamma-Ray and Cosmic Ray Muon Modalities for Cargo Inspection

Screening and inspection of cargo containers are two essential methods to nondestructively examine the contents of shipment. These methods enable the detection of illicit transportation of unauthorized materials such as nuclear and radioactive materials, explosives, drugs, and so on, typically at borders or secure facilities. Although high-energy X-ray transmission is a standard system and is widely used for cargo inspection, the inherent challenges of high false-positive rates and high attenuation factors necessitate the development of complementary techniques that can increase the detection efficiency and accuracy in large and dense materials. Gamma-rays, which possess higher penetration characteristics because of their high energy, offer an alternative nonintrusive modality for cargo scanning. They represent a promising inspection method when compared to X-rays for three reasons: (1) improved ability to detect nuclear and radioactive materials, (2) higher inspection throughput rates, and (3) lower false-positive rates. Currently, there are two main gamma-ray inspection techniques, active and passive interrogation. Active interrogation can be further grouped into (1) gamma-ray transmission imaging and (2) neutron-induced gamma-ray emission detection. Gamma-ray transmission imaging utilizes differences in material densities for mapping the shipment contents and detecting anomalies. It is analogous to the X-ray transmission method; however, the high-energy photons make it more difficult to shield against, which enables more efficient performance in large and dense material inspection. Neutron-induced gamma-ray emission inspection is designed for the detection of nuclear and radioactive material because those materials emit characteristic gamma-rays when they are activated by neutron absorption. On the other hand, passive interrogation techniques rely on high-efficiency detectors to detect radiation emitted from hidden special nuclear or other radioactive materials. Similar to passive interrogation, cosmic ray muon monitoring and imaging are relatively new techniques that do not require external radioactive sources. These techniques have received attention as a potential next-generation radiographic probe to identify illicit transportation of nuclear and radioactive materials in cargo containers. Cosmic ray muons have unique features, (1) much higher energies than X-rays or gamma-rays (on the order of 10−1—104 GeV), (2) enhanced penetration capability, and (3) natural occurrence, thereby eliminating the need for induced radiation sources. These features enable cosmic ray muons to be utilized for detection of special nuclear materials in high-background-noise environments. By analyzing incoming and outgoing muon trajectories, scattering angles, and energies, it has been shown that it would be possible to locate hidden and well-shielded materials in cargo containers via three-dimensional muon tomography images or signal analysis. Gamma-rays, cosmic ray muons, and other nonintrusive cargo inspection modalities are complementary to each other, allowing them to address various cargo inspection conditions (i.e., scanning time, cost, radiation exposure level, and types of target materials). This chapter presents a detailed review of the theoretical fundamentals and technical principles behind the current gamma-ray and cosmic ray muon modalities for cargo inspection. Additionally, critical assessments and suggestions for the future directions to advance the use of gamma and muon modalities are discussed.

Bae, Junghyun↗

Detection of uranium-photofission neutrons with a 4 He scintillation detector

The use of photon active interrogation to detect special nuclear material has held significant theoretical promise, as the interrogating source particles, photons, are fundamentally different from one of the main signatures of special nuclear material: neutrons produced in nuclear fission. However, neutrons produced by photonuclear reactions in the accelerator target, collimator, and environment can obscure the fission neutron signal. These (γ, n) neutrons could be discriminated from fission neutrons by their energy spectrum, but common detectors sensitive to the neutron spectrum, like organic scintillators, are typically hampered by the intense photon background characteristic of photon-based active interrogation. In contrast, high-pressure 4 ⁢He-based scintillation detectors are well-suited to photon active interrogation, as they are similarly sensitive to fast neutrons and can measure their spectrum, but show little response to gamma rays. Here, in this work, a photon active interrogation system utilizing a 4 ⁢He scintillation detector and a 9 MeV linac-bremsstrahlung x-ray source was experimentally evaluated. The detector was shown to be capable of operating in intense gamma-ray environments and detecting photofission neutrons from 238 ⁢U when interrogated by this x-ray source. The photofission neutrons show clear spectral separation from (γ, n) neutrons produced in lead, a common shielding material.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Assessment of Modeling and Nuclear Data Needs for Active Neutron Interrogation

This document is the primary deliverable for a scoping study proposed to DOE National Laboratory Announcement Number LAB 19-2114 in the NNSA research area. The study supports user applications employing active neutron interrogation by providing a science plan to improve the modeling capability and the nuclear data that radiation transport codes use. Users rely on the accuracy of the elastic scattering and non-elastic cross-sections spanning thermal energies to 14 MeV (and higher in some cases) for modeling the neutron transport through complex geometries of materials potentially composed of many elements. While the elastic scattering cross-section data are accepted for all commonly occurring elements, the non-elastic cross-section data and the associated emission data include reaction channels that require attention. The study focused on the non-elastic reactions that emit secondary, also known as prompt, gammas with the premise that many users would benefit from improved modeling of these reactions. Many users develop material assay technologies based upon gamma signatures from radiative capture, inelastic scattering, and reactions on low-Z isotopes emitting multiple particles, so the nuclear data gaps, modeling deficiencies, and recommendations for addressing the shortfalls were assessed for these reactions. Fission gammas were excluded from this study because there are other efforts underway to address known shortfalls. Follow-on efforts that successfully execute the recommendations will tangibly improve to the ability to model gamma signatures and backgrounds for user applications, such as controlled substance detection, oil-well logging, and space exploration.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Active Neutron Interrogation as a Method for Verification of the Absence of Special Nuclear Material in Arms Control Dismantlement

The next step in arms control reductions will deal with both strategic and non-strategic weapons, presenting new and hard challenges for verification. One verification approach that might be used in support of these reductions is the concept of deferred verification, which forgoes inspections at sensitive nuclear sites and relies on an inspection regime having access to the open segment of a State's nuclear sector, in "monitored transfer zones." A component of this approach is the anticipated need for an instrument suite capable of detecting well-shielded highly-enriched uranium or plutonium where it isn't supposed to be. This specific need was recently identified by the United Nations Institute for Disarmament Research in an enabling operating concept they call "contain and dispose." At the foundation of this approach is the idea that items declared as "not nuclear" are, by definition, not treaty limited and are thus "fair-game" for inspection and questioning. Active Neutron Interrogation (ANI), using beta-delayed neutron emissions as the signature for special nuclear material (SNM) detection, is a promising method to address this challenge. The method is quick, has high sensitivity and high specificity for detecting shielded SNM, is robust against changing background radiation environments, is robust against the presence of unknown shielding, and avoids the use of gamma-ray spectrometry which may introduce complications due to the potential release of sensitive information. This paper will present recent research activities exploring technical aspects of using ANI as a FAIRGAME verification method and discuss future prospects and research needs

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗

Improved evaluation of safeguards parameters from spent fuel measurements with the Differential Die-Away (DDA) instrument

The Differential Die-Away (DDA) technique is a highly sensitive non-destructive assay method for characterizing and detecting the presence of fissile material within an item of interest. DDA utilizes a series of pulses from a neutron generator (NG) to actively interrogate an item of interest. The die-away time of the neutron population induced by this active interrogation and the integral of the total differential die-away signal can be used to characterize items such as nuclear waste drums and spent nuclear fuel assemblies. In this work, Los Alamos National Laboratory (LANL) conceptualized, designed, and fabricated a DDA instrument that was deployed for field test measurements at the Central Interim Storage Facility for Spent Nuclear Fuel (Clab) in Oskarshamn, Sweden. The instrument performed multiple static measurements at fixed locations and dynamic axial scans of 15 pressurized water reactor (PWR) and 10 boiling water reactor (BWR) spent fuel assemblies, collecting both passive and active measurement data. The static assays of the assemblies measured the differential die-away signal, die-away time, and total passive neutron emission rate to create calibration curves for the evaluation of assembly multiplication, burnup, initial enrichment, effective fissile mass, and total elemental plutonium mass. Each calibration curve was optimized by minimizing the relative root mean square error (RRMSE) of assembly assay results compared to declared assembly parameters. The same quantities were also measured with the axial scans, and the resulting data were applied in two ways: (1) in the creation of calibration curves to improve evaluation of the same safeguards parameters as static assays, and (2) for comparison to simulation. In most cases, across both PWR and BWR assemblies, axial scan data improved the estimation of the above parameters, quantified by decreasing the calibration curve RRMSE. These axial scan results demonstrate the ability of the DDA instrument and analysis method to characterize spent PWR and BWR fuel as well as, or better than, a static assay of the same assembly. Furthermore, the DDA instrument’s unique ability to obtain both active and passive data in a single, axial scan of an entire spent fuel assembly represents a more efficient and accurate way of assaying spent fuel for verification purposes. These results represent a significant advancement for characterizing spent nuclear fuel compared to current technologies.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

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 ↗

Development and evaluation of a list mode neutron coincidence collar for spatial response measurements of fresh fuel assemblies

A traditional safeguards neutron coincidence counting system, the Neutron Coincidence Collar, has been modified to incorporate individual preamplifiers on each of its 18 3He tubes in active interrogation mode. When used with list mode data acquisition (LMDA) and analysis, a signal from each 3He tube can be recorded and analyzed to allow a spatial response measurement to be performed on an item based on count rate and 3He tube location within the system. The ultimate goal of this project is to demonstrate the capabilities of a list mode response matrix for the nondestructive assay of fresh nuclear fuel assemblies. To enable partial defect detection of fuel pin locations and absences within an assembly, the project aims to extend well-established correlated neutron analysis techniques on a preexisting Neutron Coincidence Collar by extracting a greater number of useful signatures from the system than are currently generated. LMDA, combined with the addition of multiple preamplifiers, facilitates this capability by increasing the number of simultaneous signals that can be measured; this allows an in-depth analysis of neutron coincidence events to determine a fissioning item’s location based on the measured doubles count rate in various channel logic coincidence combinations. All of this can be done from a single measurement pulse train in offline analysis, which is the major benefit provided by LMDA. Through various stages of development and testing, a Mirion Technologies model JCC-71 Neutron Coincidence Collar has been successfully retrofit with modern electronics designed in-house at Oak Ridge National Laboratory, matching preexisting JAB-01 electronics performance, while maintaining the original system footprint. This paper presents these various stages of development and experimental evaluation of the proof of concept system.

Moore, Angela S.↗

Identification and Description of a Silicic Volcaniclastic Layer in Gale Crater, Mars, Using Active Neutron Interrogation

The Dynamic Albedo of Neutrons instrument aboard the Mars Science Laboratory rover, Curiosity, has been used to map a stratigraphically-conformable layer of high-SiO 2 material in Gale crater. Previous work has shown this material contains tridymite, a high-temperature/low-pressure felsic mineral, interpreted to have a volcanic source rock. We describe several characteristics including orientation, extent, hydration, and geochemistry, consistent with a volcaniclastic material conformably deposited within a lacustrine mudstone succession. Relationships with widely dispersed alteration features and orbital detections of hydrated SiO 2 suggest that this high-SiO 2 layer extends at least 17 km laterally. Mineralogical abundances previously reported for this high-SiO 2 material indicated that hydrous species were restricted to the amorphous (non-crystalline) fraction, which is dominated by SiO2. The low mean bulk hydration of this high-SiO 2 layer (1.85 ± 0.13 wt.% water-equivalent hydrogen) is consistent with silicic glass in addition to opal-A and opal- CT. Persistent volcanic glass and tridymite in addition to opal in an ancient sedimentary unit indicates that the conversion to more ordered forms of crystalline SiO 2 has not proceeded to completion and that this material has had only limited exposure to water since it originally erupted, despite having been transported in a uviolacustrine system. Our results, including the conformable nature, large areal extent, and presence of vol- canic glass, indicate that this high-SiO 2 material is derived from the product of evolved magma on Mars. This is the rst identi cation of a silicic volcaniclastic layer on another planet, and has important implications for magma evolution mechanisms on single-plate planets.

58 GEOSCIENCES↗

Demonstration of active neutron interrogation of special nuclear materials using a high-intensity short-pulse-laser-driven neutron source

Detecting shielded special nuclear material, such as nuclear explosives, is a difficult challenge pursued by non-proliferation, anti-terrorism, and nuclear security programs worldwide. Interrogation with intense fast-neutron pulses is a promising method to characterize concealed nuclear material rapidly but is limited by suitable source availability and proven instrumentation. In this study we have pioneered a demonstration of such an interrogation method using a high-intensity, short-pulse, laser-driven neutron source that offers potential benefits compared to conventional neutron sources. The measurement results reported here represent the first experimental demonstration of this interrogation approach on enriched uranium items and demonstrate the feasibility of a precise measurement using realistic nuclear materials, representative of field scenarios, even with just a single laser-driven neutron pulse. Bright pulsed sources can overcome the nuisance background of items with strong internal neutron sources, improving analytical power, while single-shot assay is attractive in high-throughput situations where time is at a premium. The science and technology of this type of neutron production is developing rapidly, and we anticipate that practical mobile interrogation systems will become available based on the detection concepts demonstrated here to meet the growing measurement needs.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗