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Novel Perovskite Semiconductors for the Detection of Special Nuclear Material

Special nuclear material (SNM) detection using portable, highly efficient detectors is of paramount importance to national security for treaty verification and nonproliferation monitoring. The most mature technology for neutron detection is the 3He proportional counter; however, despite its high efficiency and ubiquitous use, 3He detectors have significant drawbacks, including long absorption lengths, high voltage requirements, and dependence on the availability of 3 He. The goal of this project is to synthesize a novel, boron-based perovskite semiconductor crystals to create a more efficient and more portable neutron detector. This innovative material will lead to a significant decrease in power and size requirements with higher operating temperatures than other traditional solid-state detectors. Directly incorporating 10 B eliminates the need for a conversion layer and leads to high neutron absorption coefficients. In this seedling project, we successfully synthesized millimeter sized crystals using inverse temperature crystallization with sizes of 1.73 mm in length and 480 μm in thickness.

36 MATERIALS SCIENCE↗

Novel Perovskite Semiconductors for the Detection of Special Nuclear Material

Special nuclear material detection using portable, highly efficient detectors is of paramount importance to national security and environmental monitoring. Current neutron detectors, including gas proportional counters and scintillators, are not suitable for discrete or portable monitoring due to size, weight, and power limitations. For example, 3 He gas proportional detectors have significant drawbacks, including long absorption lengths, high voltage requirements, and dependence on the availability of 3 He. The goal of this project is to synthesize a novel, boron-based perovskite semiconductor crystals to create a more efficient and more portable neutron detector. This innovative material will lead to a significant decrease in power and size requirements with higher operating temperatures than other traditional solid-state detectors. Directly incorporating 10 B eliminates the need for a conversion layer and leads to high neutron absorption coefficients. In this seedling project, we used inverse temperature crystallization with boron precursors to create CH 3 NH 3 PbI 3-x (BF 4 ) x . The crystals were analyzed with X-ray diffraction, but the results were inconclusive. Future work will focus on tailoring the solution growth and selecting appropriate solvents and precursors.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Special Nuclear Material Characterization Using Digital 3-D Position Sensitive CdZnTe Detectors and High Purity Germanium Spectrometers

Special nuclear material (SNM) monitoring often requires high resolution gamma-ray spectroscopy for material characterization. Portable systems and rapid deployment are also highly valued for some applications. Deployable gamma-ray imaging spectrometers using pixelated CdZnTe semiconductor detectors have become commercially available within the past three years to meet these requirements. CdZnTe systems have demonstrated room-temperature energy resolutions below 0.5% FWHM at 662 keV using single pixel events and below 0.7% FWHM at 662 keV using all events. The systems are able to go from storage to measurement in less than two minutes. Special nuclear materials were measured at the Y-12 National Security Complex and at the Device Assembly Facility at the Nevada National Security Site. The use of a CdZnTe system to measure uranium enrichment was demonstrated and uranium spectral features were compared to a commercially available high purity germanium (HPGe) spectrometer. The use of passive gamma ray spectroscopy techniques to estimate plutonium grade using CdZnTe detectors was demonstrated for the first time.

CdZnTe detectors, gamma-ray imaging, gamma-ray spe↗

Neutron and gamma-ray energy reconstruction for characterization of special nuclear material

Characterization of special nuclear material may be performed using energy spectroscopy of either the neutron or gamma-ray emissions from the sample. Gamma-ray spectroscopy can be performed relatively easily using high-resolution semiconductors such as high-purity germanium. Neutron spectroscopy, by contrast, is a complex inverse problem. Here, results are presented for 252 Cf and PuBe energy spectra unfolded using a single EJ309 organic scintillator; excellent agreement is observed with the reference spectra. Neutron energy spectroscopy is also possible using a two-plane detector array, whereby time-offlight kinematics can be used. With this system, energy spectra can also be obtained as a function of position. Finally, spatial-dependent energy spectra are presented for neutron and gamma-ray sources that are in excellent agreement with expectations.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Detection of special nuclear material from delayed neutron emission induced by a dual-particle monoenergetic source

Detection of unique signatures of special nuclear materials is critical for their interdiction in a variety of nuclear security and nonproliferation scenarios. We report on the observation of delayed neutrons from fission of uranium induced in dual-particle active interrogation based on the {sup 11}B(d,n γ){sup 12}C nuclear reaction. Majority of the fissions are attributed to fast fission induced by the incident quasi-monoenergetic neutrons. A Li-doped glass–polymer composite scintillation neutron detector, which displays excellent neutron/γ discrimination at low energies, was used in the measurements, along with a recoil-based liquid scintillation detector. Time-dependent buildup and decay of delayed neutron emission from {sup 238}U were measured between the interrogating beam pulses and after the interrogating beam was turned off, respectively. Characteristic buildup and decay time profiles were compared to the common parametrization into six delayed neutron groups, finding a good agreement between the measurement and nuclear data. This method is promising for detecting fissile and fissionable materials in cargo scanning applications and can be readily integrated with transmission radiography using low-energy nuclear reaction sources.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Uncovering Special Nuclear Materials by Low-energy Nuclear Reaction Imaging

Weapons-grade uranium and plutonium could be used as nuclear explosives with extreme destructive potential. The problem of their detection, especially in standard cargo containers during transit, has been described as “searching for a needle in a haystack” because of the inherently low rate of spontaneous emission of characteristic penetrating radiation and the ease of its shielding. Currently, the only practical approach for uncovering well-shielded special nuclear materials is by use of active interrogation using an external radiation source. However, the similarity of these materials to shielding and the required radiation doses that may exceed regulatory limits prevent this method from being widely used in practice. We introduce a low-dose active detection technique, referred to as low-energy nuclear reaction imaging, which exploits the physics of interactions of multi-MeV monoenergetic photons and neutrons to simultaneously measure the material’s areal density and effective atomic number, while confirming the presence of fissionable materials by observing the beta-delayed neutron emission. For the first time, we demonstrate identification and imaging of uranium with this novel technique using a simple yet robust source, setting the stage for its wide adoption in security applications.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

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↗

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 ↗

Special Nuclear Material Hold-up Measurement

Facilities that process special nuclear material (SNM) generally have a variety of equipment, shielding, and nearby radiation sources, which can pose challenges when performing nondestructive analysis (NDA) within the facility, as shown in Figure 1. In this figure, the left image features two individuals performing a holdup measurement of a large duct at a posting, utilizing a detector probe attached to a yardstick to reduce some aspect of the measurement uncertainty. Note that the distance to the holdup within the pipe from the posting cannot be accounted for. The right image similarly features several individuals guiding a holdup measurement of a ducting pipe several meters overhead, by attaching a detector probe to a long handle and lining that up with a posting on the outside of the pipe. SNM processing begets SNM holdup, and this difficulty with accurate NDA can result in unaccounted accumulation of SNM holdup within a process or area. Normal SNM processing operations can accumulate holdup within filters, pumps, pipes, ducts, other equipment, and facility support systems, as demonstrated by Figure 2. It is important for deactivation and decommissioning (D&D) gloveboxes and their ancillary equipment, material accountability, criticality safety, facility operations, waste management, radiation safety, and security to accurately characterize the location, composition, and quantity of this holdup to minimize these associated risks and potential diversion pathways. Current NDA techniques for assay of holdup are expensive, time consuming, and have high uncertainty.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Uncertainty quantification in application of the enrichment meter principle for nondestructive assay of special nuclear material

The various methods of nondestructive assay (NDA) of special nuclear material (SNM) have applications in nuclear nonproliferation, including detection and identification of illicit SNM at border crossings, and quantifying SNM at nuclear facilities for safeguards. No assay method is complete without “error bars,” which provide one way of expressing confidence in the assay result. Consequently, NDA specialists typically quantify total uncertainty in terms of “random” and “systematic” components, and then specify error bars for the total mass estimate in multiple items. Uncertainty quantification (UQ) for NDA has always been important, but it is recognized that greater rigor is needed and achievable using modern statistical methods. To this end, we describe the extent to which the guideline for expressing uncertainty in measurements (GUM) can be used for NDA. Also, we propose improvements over GUM for NDA by illustrating UQ challenges that it does not address, including calibration with errors in predictors, model error, and item-specific biases. A case study is presented using low-resolution NaI spectra and applying the enrichment meter principle to estimate the U-235 mass in an item. The case study illustrates how to update the current American Society for Testing and Materials guide for application of the enrichment meter principle using gamma spectra from a NaI detector.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Special Nuclear Material Gamma-Ray Signatures for Reachback Analysts

These are slides on special nuclear material gamma-ray signatures for reachback analysts for an LSS Spectroscopy course. The closing thoughts for this presentation are the following: SNM materials have definite spectral signatures that should be readily recognizable to analysts in both bare and shielded configurations. One can estimate burnup of plutonium using certain pairs of peaks that are a few keV apart. In most cases, one cannot reliably estimate uranium enrichment in an analogous way to the estimation of plutonium burnup. The origin of the most intense peaks from some SNM items may be indirect and from ‘associated nuclides.' Indirect SNM signatures sometimes have commonalities with the natural gamma-ray background.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Active and Passive Diagnostic Signatures of Special Nuclear Materials

An overview will be given discussing signatures associated with special nuclear materials acquired using both active and passive diagnostic techniques. Examples of how technology advancements have helped improve diagnostic capabilities to meet the challenges of today’s applications will be discussed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Ion Mobility – Mass Spectrometry Rapid Imaging of Special Nuclear Materials

Robot Nose will use new fast data throughput methods and experience with laser microfocus to dramatically improve the speed and spatial resolution of an established instrument, making it a useful tool for imaging special nuclear materials (SNM). Mass spectrometry imaging instruments have traditionally been too slow and mass alone is generally an insufficient measurement for organic analyses. This situation was markedly improved by Ionwerks Inc., who pioneered the combination of ion mobility with mass spectrometry imaging. In 2D mobility-mass plots, clearly identifiable trend lines can be selected and reduced to 1D mass spectra without isobaric interferences. This is a major advantage over other imaging mass spectrometers that generally cannot distinguish isobars without custom-built lasers or high voltage accelerators. Special nuclear material (SNM) contains substantial fissile isotopes, particularly 233U, 235U, and 239Pu. A complete forensic analysis of SNM therefore requires quantitative isotopic measurement – often through some form of mass spectrometry. SNM contaminated with inclusions such as pollen grains can help identify its prior locations. The project team is presently working on an approach to allow rapid screening of 1-3 cm diameter thin samples of such material.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

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↗

Active interrogation of Special Nuclear Material containers using AmBe quasi-forward biased directional source and PGNAA

Special Nuclear Material (SNM) including 95% 235 U and 239 Pu is capable of being identified by utilizing a quasi-forward directional AmBe source from Patent No: US20190013109A1 using Prompt Gamma Neutron Activation Analysis (PGNAA) simulated with Monte-Carlo N-Particle transport 6.2 (MCNP). HPGe and LaBr 3 detector arrays were used to identify and quantify the peak-to-background and peak-to-total ratios of the associated photon spectra from the SNM encased in a polyethylene shield. The conducted simulations varied the volume of the SNM and neutron source strength in the MCNP data card to conduct an uncertainty analysis. Photopeaks identified include K-shell X-rays from 235 U and 239 Pu, 61 keV from fission, 2.223 MeV prompt gamma from hydrogen, 511 keV annihilation, and a single and double escape peak from the prompt gamma interaction from hydrogen. Relationships between peak-to-total and peak-to-background as a function of SNM and particle history were investigated to aid in the analysis. The capabilities of both detector systems to acquire well resolved photopeak with a 5% relative error or less, with a 1 Ci source activity, and a peak-to-background ratio of 1.15. Finally, this was determined to take 326 s for LaBr 3 and 163 s for HPGe which is comparable to current methods for material detection which take between 100 and 900 s to acquire.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

New Developments and Applications of Superheated Emulsions: Warhead Verification and Special Nuclear Material Interdiction

In recent years, neutron detection with superheated emulsions has received renewed attention thanks to improved detector manufacturing and read-out techniques, and thanks to successful applications in warhead verification and special nuclear material (SNM) interdiction. Detectors are currently manufactured with methods allowing high uniformity of the drop sizes, which in turn allows the use of optical read-out techniques based on dynamic light scattering. Furthermore, small detector cartridges arranged in 2D matrices are developed for the verification of a declared warhead without revealing its design. For this application, the enabling features of the emulsions are that bubbles formed at different times cannot be distinguished from each other, while the passive nature of the detectors avoids the susceptibility to electronic snooping and tampering. Large modules of emulsions are developed to detect the presence of shielded special nuclear materials hidden in cargo containers ‘interrogated’ with high energy X-rays. In this case, the enabling features of the emulsions are photon discrimination, a neutron detection threshold close to 3 MeV and a rate-insensitive read-out.

d’Errico, Francesco↗

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↗