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Summary In Brief The Associated Particle Tagging (APT) project, a collaboration of Pacific Northwest National Laboratory (PNNL), Idaho National Laboratory (INL) and the Idaho State University (ISU)/Idaho Accelerator Center (IAC), has completed an exploratory study to assess the role of magnetic spectrometers as the linchpin technology in next-generation tagged-neutron and tagged-photon active interrogation (AI).
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.
Interrogation of special nuclear materials can benefit from mobile sources providing significant fluxes of neutrons (10 8 /s at 2.5 MeV, 10 10 /s at 14.1 MeV) and of photons (>10 12 /s at 1-3 MeV). We propose a source that satisfies these requirements simultaneously plus also provides, via the reaction 11 B(d,n) 12 C(γ 15.1 ), a significant flux of 15-MeV photons, which are highly penetrating and optimal for inducing photo-fission in actinides. The source is based on a compact (< 5 m) deuteron RF accelerator that delivers an average current of a few mA of deuterons at 3-4 MeV to a boron target. The accelerator consists of a short RFQ followed by efficient inter-digital H-mode structures with permanent-magnet-quadrupole beam focusing [Kurennoy et al. (2012)], which suit perfectly for deuteron acceleration at low energies. Our estimates, based on recent measurements, indicate that the required fluxes of both neutrons and photons can be achieved at ~1 mA of 4-MeV deuterons. The goal of the proposed study is to confirm feasibility of the approach and develop requirements for future full system implementation.
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The Associated Particle technique has recently been utilized with a germanium-based high-resolution $\gamma$-ray spectrometer and assessed for its capability to improve field identification of recovered chemical warfare (CW) materiel through prompt gamma-ray neutron activation analysis (PGNAA) measurements. An accurate chemical identification is necessary for the safe handling, destruction, and disposal of such hazardous items. A particularly challenging pair of CW agents commonly found in recovered munitions are phosgene (CG) and cyanogen chloride (CK), which have two of three elements in common, i.e. chlorine and carbon, but differ in the third being either oxygen or nitrogen. The detection of both latter elements is complicated by high oxygen concentration in the field environment which interferes with the small signal produced from the chemical agents. The matter is further complicated by the precautionary field practice of overpacking recovered munitions with vermiculite in larger steel multiple round containers (MRCs), which places additional oxygen-rich material around the munition while further attenuating an already weak signal emitted from the munition center. Here, this work reports quantitative results from realistic field measurements of CG and CK simulants in mock 4.2-inch mortar rounds overpacked with vermiculite in a large MRC. Results obtained with the AP technique are compared to those obtained with the traditional PGNAA approach for both overpacked- and bare-munition measurements. The AP technique is shown to provide a much more confident discrimination between the two chemicals, particularly for the more challenging field-relevant overpacked measurements, where a significant gain in sensitivity to all the key elements chlorine, carbon, nitrogen and oxygen is achieved.
We describe an associated particle neutron generator that employs a negative ion source to produce high neutron flux from a small source size. Furthermore, negative ions produced in an rf-driven plasma source are extracted through a small aperture to form a beam which bombards a positively biased, high voltage target electrode. Electrons co-extracted with the negative ions are removed by a permanent magnet electron filter. The use of negative ions enables high neutron output (100% atomic ion beam), high quality imaging (small neutron source size), and reliable operation (no high voltage breakdowns). Finally, the neutron generator can operate in either pulsed or continuous-wave (cw) mode and has been demonstrated to produce 10 6 D-D n/s (equivalent to similar to 10 8 D-T n/s) from a 1 mm-diameter neutron source size to facilitate high fidelity associated particle imaging.
In this work, high-resolution prompt γ-ray neutron activation analysis (PGNAA) is performed using the associated particle (AP) technique with a deuterium-tritium neutron generator and high-purity germanium detector. Although the time resolution is inferior compared to similar systems employing fast scintillation γ-ray detectors, the strong background suppression combined with the high γ-ray energy resolution provides an important boost in sensitivity to certain key elements, especially relevant to field measurements of complex chemicals encased within thick layers of metal, such as in the case of recovered chemical warfare (CW) munitions. Results for various CW and explosive simulants contained within mock munitions are presented and compared with results obtained from traditional PGNAA measurements without the aid of the AP technique. Significant improvements in identification and discrimination between certain chemicals are achieved with the high energy resolution AP technique.
Presentation described project to develop man-portable device for detection of nuclear material using dense plasma focus technology.
An experiment was performed to determine the neutron energy of near-monoergetic deuterium–deu-terium (D–D) neutrons that elastically scatter in a hydrogenous target. The experiment used two liquid scintillators to perform time of flight (TOF) measurements to determine neutron energy, with the start detector also serving as the scatter target. The stop detector was placed 1.0 m away and at scatter angles of π/6, π/4, and π/3 rad, and 1.5 m at a scatter angle of π/4 rad. When discrete 1 ns increments were implemented, the TOF peaks had estimated errors between 21.2 and 3.6% relative to their expected locations. Full widths at half-maximum (FWHM) ranged between 9.6 and 20.9 ns, or approximately 0.56–0.66 MeV. Monte Carlo simulations were also conducted that approximated the experimental setup and had both D–D and deuterium–tritium (DT) neutrons. The simulated results had errors between -17.2 and 0.0% relative to their expected TOF peaks when 1 ns increments were applied. The largest D–D and D–T FWHMs were 26.7 and 13.7 ns, or approximately 0.85 and 4.98 MeV, respectively. These values, however, can be reduced through manipulation of the dimensions of the system components. Lastly, the results encourage further study of the neutron elastic scatter TOF system with particular interest in application to active neutron interrogation to search for conventional explosives.
The ability to perform nondestructive assay (NDA) of fresh fuel assemblies with high precision in reasonable measurement times is significant for nuclear nonproliferation and safeguards. The current methodology used by the International Atomic Energy Agency (IAEA) for NDA of fresh fuel assemblies involves a He-3 based Uranium Neutron Collar (UNCL) system, which is an active coincidence counting system designed to measure time-correlated neutron doubles from induced fissions within the assembly. The UNCL system provides an easily implementable process of quantifying the 235 U linear density of the fresh fuel assemblies; however, operational limitations of the UNCL include long assay times and adverse sensitivity to poisoned assemblies. This has engendered investigation in alternative detector materials for fast-neutron counting to rectify some of these current limitations in the UNCL. The potential improvements of using fast-neutron organic scintillators (e.g. liquid scintillators, stilbene, PSDcapable plastics, etc.) was compared directly to the original Uranium Neutron Collar (UNCL) in-detail during the initial Advanced Neutron Detection Technology Rodeo. The simulation results showed that these alternative detector materials can provide an improvement in the assay time required to reach a suitable precision due to both their lower sensitivity to the interrogation source neutrons (i.e. AmLi neutrons) and their inherently shorter coincidence gate widths. The IAEA has developed a liquid scintillator-based Fast-Neutron Collar (FNCL) as a potential replacement system for the UNCL.
The Probing In situ with Neutrons and Gamma rays (PING) instrument is a promising planetary science application of the active neutron-gamma ray technology so successfully used in oil field well logging and mineral exploration on Earth. The objective of our technology development program at NASA Goddard Space Flight Center's (NASA/GSFC) Astrochemistry Laboratory is to extend the application of neutron interrogation techniques to landed in situ planetary composition measurements by using a 14 MeV Pulsed Neutron Generator (PNG) combined with neutron and gamma ray detectors, to probe the surface and subsurface of planetary bodies without the need to drill. We are thus working to bring the PING instrument to the point where it can be flown on a variety of surface lander or rover missions to the Moon, Mars, Venus, asteroids, comets and the satellites of the outer planets.
Sensitive fast-neutron detectors are required for use in lead slowing down spectrometry (LSDS), an active interrogation technique for used nuclear fuel assay for Materials Protection, Accounting, and Controls Technologies (MPACT). During the past several years UNLV sponsored a research project at RPI to investigate LSDS; began development of fission chamber detectors for use in LSDS experiments in collaboration with INL, LANL, and Oregon State U.; and participated in a LSDS experiment at LANL. In the LSDS technique, research has demonstrated that these fission chamber detectors must be sensitive to fission energy neutrons but insensitive to thermal-energy neutrons. Because most systems are highly sensitive to large thermal neutron populations due to the well-known large thermal cross section of 235U, even a miniscule amount of this isotope in a fission chamber will overwhelm the small population of higher-energy neutrons. Thus, fast-fission chamber detectors must be fabricated with highly depleted uranium (DU) or ultra-pure thorium (Th), which is about half as efficient as DU. Previous research conducted at RPI demonstrated that the required purity of DU for assay of used nuclear fuel using LSDS is less than 4 ppm 235U, material that until recently was not available in the U.S. In 2009 the PI purchased 3 grams of ultra-depleted uranium (uDU, 99.99998% 238U with just 0.2 ± 0.1 ppm 235U) from VNIIEF in Sarov, Russia. We received the material in the form of U3O8 powder in August of 2009, and verified its purity and depletion in a FY10 MPACT collaboration project. In addition, chemical processing for use in FC R&D was initiated, fission chamber detectors and a scanning alpha-particle spectrometer were developed, and foils were used in a preliminary LSDS experiment at a LANL/LANSCE in Sept. of 2010. The as-received U3O8 powder must be chemically processed to convert it to another chemical form while maintaining its purity, which then must be used to electro-deposit U or UO2 in extremely thin layers (1 to 2 mg/cm2) on various media such as films, foils, or discs. After many months of investigation and trials in FY10 and 11, UNLV researchers developed a new method to produce pure UO2 deposits on foils using a unique approach, which has never been demonstrated, that involves dissolution of U3O8 directly into room temperature ionic liquid (RTIL) followed by electrodeposition from the RTIL-uDU solution (Th deposition from RTIL had been previously demonstrated). The high-purity dissolution of the U3O8 permits the use of RTIL solutions for deposition of U on metal foils in layers without introducing contamination. In FY10 and early FY11 a natural U surrogate for the uDU was used to investigate this and other techniques. In this research project UNLV will deposit directly from RTIL to produce uDU and Th foils devoid of possible contaminants. After these layers have been deposited, they will be examined for purity and uniformity. UNLV will complete the development and demonstration of the RTIL technology/ methodology to prepare uDU and Th samples for use in constructing fast-neutron detectors. Although this material was purchased for use in research using fast-fission chamber detectors for active inspection techniques for MPACT, it could also contribute to R&D for other applications, such as cross section measurements or neutron spectroscopy for national security
Here, we compare the pulse-shape-discrimination performance of a large Stilbene detector, manufactured at the Lawrence Livermore National Laboratory, to a similarly sized liquid scintillator, made by Eljen Technologies, Inc. (type EJ309), under various high-count-rate scenarios, such as can be expected during Active Interrogation of objects using an electric neutron generator for detecting the presence of Special Nuclear Materials and contraband. Pulse Shape Discrimination (PSD) is performed with an extension of previously described wavelet and event fitting algorithms, which are also used to reject pileup events and to correct the energy calibration for event signals clipped during digitization. We find that strong PSD and pileup rejection cuts are required to function in this high-count-rate environment. Whereas the Stilbene detector has intrinsically better pulse-shape discrimination performance, the pulses of events from the liquid scintillator are somewhat narrower, reducing pileup. We use an event fitting cut that provides simultaneous PSD identification and pileup rejection. When applying the same cut to data taken with both detectors, we find that Stilbene has higher event use efficiency by about a factor of two and retains a better gamma rejection ratio compared to EJ309.
The entry of fusion as a viable, competitive source of power has been stymied by the challenge of finding an economical way to provide for the confinement and heating of the plasma fuel. The main impediment for current nuclear fusion concepts is the complexity and large mass associated with the confinement systems. To take advantage of the smaller scale, higher density regime of magnetic fusion, an efficient method for achieving the compressional heating required to reach fusion gain conditions must be found. The very compact, high energy density plasmoid commonly referred to as a Field Reversed Configuration (FRC) provides for an ideal target for this purpose. To make fusion with the FRC practical, an efficient method for repetitively compressing the FRC to fusion gain conditions is required. A novel approach to be explored in this endeavor is to remotely launch a converging array of small macro-particles (macrons) that merge and form a more massive liner inside the reactor which then radially compresses and heats the FRC plasmoid to fusion conditions. The closed magnetic field in the target FRC plasmoid suppresses the thermal transport to the confining liner significantly lowering the imploding power needed to compress the target. With the momentum flux being delivered by an assemblage of low mass, but high velocity macrons, many of the difficulties encountered with the liner implosion power technology are eliminated. The undertaking to be described in this proposal is to evaluate the feasibility achieving fusion conditions from this simple and low cost approach to fusion. During phase I the design and testing of the key components for the creation of the macron formed liner have been successfully carried out. Detailed numerical calculations of the merging, formation and radial implosion of the Macron Formed Liner (MFL) were also performed. The phase II effort will focus on an experimental demonstration of the macron launcher at full power, and the demonstration of megagauss magnetic field compression by a small array of full scale macrons. In addition the physics of the compression of an FRC to fusion conditions will be undertaken with a smaller scale MFL. The timescale for testing will be rapidly accelerated by taking advantage of other facilities at MSNW where the target FRC will be created and translated inside the MFL just prior to implosion of the MFL. Experimental success would establish the concept at the proof of principle level and the following phase III effort would focus on the full development of the concept into a fusion gain device. Successful operation would lead to several benefits in various fields. It would have application to high energy density physics, as well as nuclear waste transmutation and alternate fission fuel cycles. The smaller scale device could find immediate application as an intense source of neutrons for diagnostic imaging and non-invasive object interrogation.
The use of ion beams in interrogating materials performance for nuclear energy applications is advancing at a rapid rate. Ion irradiations have been proven to produce radiation effects data that are of direct relevance for understanding neutron-induced displacement damage. This development reflects significant and continued investment in infrastructure by the U.S. Department of Energy (DOE) as well as support of science and engineering research at universities and national laboratories. Application of ion beam irradiation methods to enhance the deployment of materials in reactors is in the spirit of the Gateway for Accelerated Innovation in Nuclear (GAIN) initiative sponsored by DOE to accelerate the deployment of innovation in the U.S. nuclear industry. Ion beam irradiation shows considerable promise for assisting in down selecting candidate materials for use in both current and advanced nuclear energy systems. Ion beams allow rapid achievement of materials damage levels not accessible by neutron irradiation in test reactors due to cost and time constraints. Ion beam studies provide data on the effects of irradiation under very specific conditions of temperature, radiation dose, and radiation dose rate that are difficult or impossible to achieve via reactor irradiation experiments. This data can be used to develop and validate detailed predictive radiation effects models for use in reactor materials research and development. Despite the current high state of the art and the maturity of quality assurance, there are still challenges to the deployment of ion beam data in support of reactor materials qualification. For the most part, these challenges arise from the lack of a detailed mechanistic understanding of potential difference between ion induced and neutron induced materials damage, which is exacerbated by difficulties in obtaining bulk physical and mechanical properties data from the micron-scale heavy ion irradiation depths. In particular, improved understanding of dose rate effects, as a function of temperature, are needed. This document offers a roadmap for the development and enhancement of current U.S. ion beam irradiation technologies within university and national laboratory settings, and especially for the deployment of new highly controlled in situ interrogation of materials during irradiation to provide dynamic and mechanistic data for model development. The status and capabilities of relevant U.S. ion beam facilities are summarized and recommended “best practices” for performing ion irradiations are described. The potential role of ion beam irradiations to assist the development and deployment of reactor materials is outlined. Key principles include developing methods for rapid and cost-effective materials selection and development, characterizing fundamental material response under irradiation, and developing a robust mechanistic understanding of microstructure evolution under irradiation (including development and validation of reliable predictive models for microstructure evolution).
Abstract Not Provided
No abstract prepared.
Electrified interfaces are critical to the performance of energy systems and often demonstrate substantial complexity under operating conditions. A nanoscale understanding of the interfacial microenvironment, i.e., the solid-electrolyte interphase (SEI), in lithium-mediated nitrogen reduction (Li–N 2 R) is key for realizing efficient ammonia (NH 3 ) production. Herein, we used time-resolved neutron reflectometry (NR) to observe SEI formation under Li–N 2 R conditions. We found that the LiBF 4 -based electrolyte provided a substantially more well-defined SEI layer than previous SEI NR interrogations that used LiClO 4 , highlighting the underlying chemistry that dictates electrolyte design and enabling new NR-based studies. Using in situ NR, we found that the LiBF 4 -derived SEI under Li–N 2 R conditions comprises a thick, diffuse outer layer and a thin, compact inner layer at low current cycling (<2 mA/cm 2 ), revealing a structure which ex situ studies have not been able to probe. Increased current cycling and sustained current cycling led to the merging of the layers into a single-layer SEI. Here, we used isotope contrast methods with d 6 -EtOH and d 8 -THF to drive time-resolved tracking of SEI growth at low current cycling, revealing that the proton donor modifies the inner layer, and the solvent modifies the outer layer. Li dendritic growth was observed in the absence of a proton donor. Neutron absorption also indicated the presence of boron in the SEI, underscoring the value of neutron-based interrogation. Our results inform Li-based systems and reaction microenvironments, and these methods can be applied broadly to interfacial energy technologies.