In recent years, the International Atomic Energy Agency (IAEA) has pursued innovative techniques and an integrated suite of safeguards measures to address the verification challenges posed by the front end of the nuclear fuel cycle. Among the unattended instruments currently being explored by the IAEA is an Unattended Cylinder Verification Station (UCVS), which could provide automated, independent verification of the declared relative enrichment, 235 U mass, total uranium mass, and identification for all declared uranium hexafluoride cylinders in a facility (e.g., uranium enrichment plants and fuel fabrication plants). Under the auspices of the United States and European Commission Support Programs to the IAEA, a project was undertaken to assess the technical and practical viability of the UCVS concept. The first phase of the UCVS viability study was centered on a long-term field trial of a prototype UCVS system at a fuel fabrication facility. A key outcome of the study was a quantitative performance evaluation of two nondestructive assay (NDA) methods being considered for inclusion in a UCVS: Hybrid Enrichment Verification Array (HEVA), and Passive Neutron Enrichment Meter (PNEM). This paper provides a description of the UCVS prototype design and an overview of the long-term field trial. Analysis results and interpretation are presented with a focus on the performance of PNEM and HEVA for the assay of over 200 “typical” Type 30B cylinders, and the viability of an “NDA Fingerprint” concept as a high-fidelity means to periodically verify that material diversion has not occurred.

The International Atomic Energy Agency (IAEA) currently uses handheld gamma-ray spectrometers combined with ultrasonic wall-thickness gauges to verify the declared enrichment of uranium hexafluoride (UF6) cylinders. The current method provides relatively low accuracy for the assay of 235U enrichment, especially for natural and depleted UF6. Furthermore, the current method provides no capability to assay the absolute mass of 235U in the cylinder due to the localized instrument geometry and limited penetration of the 186-keV gamma-ray signature from 235U. Also, the current verification process is a time-consuming component of on-site inspections at uranium enrichment plants. Toward the goal of a more-capable cylinder assay method, the Pacific Northwest National Laboratory has developed the hybrid enrichment verification array (HEVA). HEVA measures both the traditional 186-keV direct signature and a non-traditional, high-energy neutron-induced signature (HEVANT). HEVANT enables full-volume assay of UF6 cylinders by exploiting the relatively larger mean free paths of the neutrons emitted from the UF6. In this work, Monte Carlo modeling is used as the basis for characterizing HEVANT in terms of the individual contributions to HEVANT from nuclides and hardware components. Monte Carlo modeling is also used to quantify the intrinsic efficiency of HEVA for neutron detection in a cylinder-assay geometry. Modeling predictions are validated against neutron-induced gamma-ray spectra from laboratory measurements and a relatively large population of Type 30B cylinders spanning a range of enrichments. Implications of the analysis and findings on the viability of HEVA for cylinder verification are discussed, such as the resistance of the HEVANT signature to manipulation by the nearby placement of neutron-conversion materials.

Current International Atomic Energy Agency (IAEA) methodologies for the verification of fresh low-enriched uranium (LEU) and mixed oxide (MOX) fuel assemblies are volume-averaging methods that lack sensitivity to individual pins. Further, as fresh fuel assemblies become more and more complex (e.g., heavy gadolinium loading, high degrees of axial and radial variation in fissile concentration), the accuracy of current IAEA instruments degrades and measurement time increases. Particularly in light of the fact that no special tooling is required to remove individual pins from modern fuel assemblies, the IAEA needs new capabilities for the verification of unirradiated (i.e., fresh LEU and MOX) assemblies to ensure that fissile material has not been diverted. Passive gamma emission tomography has demonstrated potential to provide pin-level verification of spent fuel, but gamma-ray emission rates from unirradiated fuel emissions are significantly lower, precluding purely passive tomography methods. The work presented here introduces the concept of Hybrid Gamma Emission Tomography (HGET) for verification of unirradiated fuels, in which a neutron source is used to actively interrogate the fuel assembly and the resulting gamma-ray emissions are imaged using tomographic methods to provide pin-level verification of fissile material concentration.

The work presented in this report is focused on the characterization and refinement of the Hybrid Enrichment Verification Array (HEVA) approach, which combines the traditional 186-keV 235U signature with high-energy prompt gamma rays from neutron capture in the detector and surrounding collimator material, to determine the relative enrichment and 235U mass of the cylinder. The design of the HEVA modules (hardware and software) deployed in the current field trial builds on over seven years of study and evolution by PNNL, and consists of a ø3''×3'' NaI(Tl) scintillator coupled to an Osprey digital multi-channel analyzer tube base from Canberra. The core of the HEVA methodology, the high-energy prompt gamma-ray signature, serves as an indirect method for the measurement of total neutron emission from the cylinder. A method for measuring the intrinsic efficiency of this “non-traditional” neutron signature and the results from a benchmark experiment are presented. Also discussed are potential perturbing effects on the non-traditional signature, including short-lived activation of materials in the HEVA module. Modeling and empirical results are presented to demonstrate that such effects are expected to be negligible for the envisioned implementation scenario. In comparison to previous versions, the new design boosts the high-energy prompt gamma-ray signature, provides more flexible and effective collimation, and improves count-rate management via commercially available pulse-processing electronics with a special modification prompted by PNNL.

The International Atomic Energy Agency (IAEA) continues to expand its use of unattended measurement systems. An increasing number of systems and an expanding family of instruments create challenges in terms of deployment efficiency and the implementation of data authentication measures. Traditional data security measures, for example tamper-indicating (TI) conduit, are impractical for the long separation distances (often 100 meters or more) between unattended monitoring system (UMS) components. Pacific Northwest National Laboratory (PNNL) is studying the viability of active time-domain reflectometry (TDR) for the detection of cable tampering in unattended radiation detection systems. The instrument concept under investigation would allow for unmanned cable integrity measurements, remote surveillance reporting and locating of cable faults and/or tampers. This report describes PNNL’s FY16 progress and includes: an overview of the TDR methods under investigation; description of the TDR evaluation testbed developed by PNNL; development and testing of advanced signal processing algorithms to extract weak signals from relatively high noise levels; and initial testing of a laboratory prototype intended for IAEA UMS applications and based on a commercially available TDR module. Preliminary viability findings and recommendations for the next stage of development and testing are provided.

In recent years, the International Atomic Energy Agency (IAEA) has pursued innovative techniques and an integrated suite of safeguards measures to address the verification challenges posed by the front end of the nuclear fuel cycle. Among the unattended instruments currently being explored by the IAEA is an Unattended Cylinder Verification Station (UCVS) that could provide automated, independent verification of the declared relative enrichment, 235U mass, total uranium mass and identification for all declared UF6 cylinders in a facility (e.g., uranium enrichment plants and fuel fabrication plants). Under the auspices of the United States and European Commission Support Programs to the IAEA, a project was undertaken to assess the technical and practical viability of the UCVS concept. The US Support Program team consisted of Pacific Northwest National Laboratory (PNNL, lead), Los Alamos National Laboratory (LANL), Oak Ridge National Laboratory (ORNL) and Savanah River National Laboratory (SRNL). At the core of the viability study is a long-term field trial of a prototype UCVS system at a Westinghouse fuel fabrication facility. A key outcome of the study is a quantitative performance evaluation of two nondestructive assay (NDA) methods being considered for inclusion in a UCVS: Hybrid Enrichment Verification Array (HEVA), and Passive Neutron Enrichment Meter (PNEM). This report provides context for the UCVS concept and the field trial: potential UCVS implementation concepts at an enrichment facility; an overview of UCVS prototype design; field trial objectives and activities. Field trial results and interpretation are presented, with a focus on the performance of PNEM and HEVA for the assay of over 200 “typical” Type 30B cylinders, and the viability of an “NDA Fingerprint” concept as a high-fidelity means to periodically verify that the contents of a given cylinder are consistent with previous scans. A modeling study, combined with field-measured instrument uncertainties, provides an assessment of the partial-defect sensitivity of HEVA and PNEM for both one-time assay and (repeated) NDA Fingerprint verification scenarios. The findings presented in this report represent a significant step forward in the community’s understanding of the strengths and limitations of the PNEM and HEVA NDA methods, and the viability of the UCVS concept in front-end fuel cycle facilities. This experience will inform Phase II of the UCVS viability study, should the IAEA pursue it.

The International Atomic Energy Agency (IAEA) continues to expand its use of unattended measurement systems. An increasing number of systems and an expanding family of instruments create challenges in terms of deployment efficiency and the implementation of data authentication measures. In collaboration with the IAEA, tamper-indicating measures to address data-transmission authentication challenges with unattended safeguards systems are under investigation. Pacific Northwest National Laboratory (PNNL) is studying the viability of active time-domain reflectometry (TDR) along two parallel but interconnected paths: (1) swept-frequency TDR as the highly flexible, laboratory gold standard to which field-deployable options can be compared, and (2) a low-cost commercially available spread-spectrum TDR technology as one option for field implementation. This report describes PNNL’s FY15 progress in the viability study including: an overview of the TDR methods under investigation; description of the testing configurations and mock tampering scenarios; results from a preliminary sensitivity comparison of the two TDR methods; demonstration of a quantitative metric for estimating field performance that acknowledges the need for high detection probability while minimizing false alarms. FY15 progress reported here sets the stage for a rigorous comparison of the candidate TDR methods, over a range of deployment scenarios and perturbing effects typical of IAEA unattended monitoring systems.

The International Atomic Energy Agency (IAEA) deploys unattended monitoring systems to provide continuous monitoring of nuclear material within safeguarded facilities around the world. As the number of unattended monitoring instruments increases, the IAEA is challenged to become more efficient in the implementation of those systems. In 2010, the IAEA initiated the Front-End Electronics for Unattended Measurement (FEUM) project with the goals of greater flexibility in the interfaces to various sensors and data acquisition systems, and improved capabilities for remotely located sensors (e.g., where sensor and front-end electronics might be separated by tens of meters). In consultation with the IAEA, a technical evaluation of a candidate FEUM device produced by a commercial vendor has been performed. This evaluation assessed the device against the IAEA’s original technical specifications and a broad range of important parameters that include sensor types, cable lengths and types, industrial electromagnetic noise that can degrade signals from remotely located detectors, and high radiation fields. Testing data, interpretation, findings and recommendations are provided.

iii Acknowledgments v Acronyms and Abbreviations vii 1.0 Introduction 1 2.0 Swept-Frequency Time-Domain Reflectometry 3 2.1 Swept Frequency TDR: Testing Arrangement 4 2.2 Cable Tamper: Preliminary Findings 5 2.3 Cable Splice: Preliminary Findings 6 3.0 Spread-Spectrum TDR with LiveWire 11 3.1 LiveWire: Testing Arrangement 12 3.2 LiveWire: Preliminary Findings 14 4.0 Conclusions and Next Steps 15 5.0 References 16 Appendix A Preliminary RG71 Cable Testing A.1

Ever since there has been spent fuel (SF), researchers have made nondestructive assay (NDA) measurements of that fuel to learn about its content. In general these measurements have focused on the simplest signatures (passive photon and total neutron emission) and the analysis has often focused on diversion detection and on determining properties such as burnup (BU) and cooling time (CT). Because of shortcomings in current analysis methods, inspectorates and policy makers are interested in improving the state-of-the-art in SF NDA. For this reason the U.S. Department of Energy, through the Next Generation Safeguards Initiative (NGSI), targeted the determination of elemental Pu mass in SF as a technical goal. As part of this research effort, 14 nondestructive assay techniques were studied . This wide range of techniques was selected to allow flexibility for the various needs of the safeguards inspectorates and to prepare for the likely integration of one or more techniques having complementary features. In the course of researching this broad range of NDA techniques, several cross-cutting issues were. This paper will describe some common issues and insights. In particular we will describe the following: (1) the role of neutron absorbers with emphasis on how these absorbers vary in SFmore » as a function of initial enrichment, BU and CT; (2) the need to partition the measured signal among different isotopic sources; and (3) the importance of the “first generation” concept which indicates the spatial location from which the signal originates as well as the isotopic origins.« less

Pacific Northwest National Laboratory (PNNL) intends to automate the UF6 cylinder nondestructive assay (NDA) verification currently performed by the International Atomic Energy Agency (IAEA) at enrichment plants. PNNL is proposing the installation of a portal monitor at a key measurement point to positively identify each cylinder, measure its mass and enrichment, store the data along with operator inputs in a secure database, and maintain continuity of knowledge on measured cylinders until inspector arrival. This report summarizes the status of the research and development of an enrichment assay methodology supporting the cylinder verification concept. The enrichment assay approach exploits a hybrid of two passively-detected ionizing-radiation signatures: the traditional enrichment meter signature (186-keV photon peak area) and a non-traditional signature, manifested in the high-energy (3 to 8 MeV) gamma-ray continuum, generated by neutron emission from UF6. PNNL has designed, fabricated, and field-tested several prototype assay sensor packages in an effort to demonstrate proof-of-principle for the hybrid assay approach, quantify the expected assay precision for various categories of cylinder contents, and assess the potential for unsupervised deployment of the technology in a portal-monitor form factor. We refer to recent sensor-package prototypes as the Hybrid Enrichment Verification Array (HEVA). The report provides an overview of the assay signatures and summarizes the results of several HEVA field measurement campaigns on populations of Type 30B UF6 cylinders containing low-enriched uranium (LEU), natural uranium (NU), and depleted uranium (DU). Approaches to performance optimization of the assay technique via radiation transport modeling are briefly described, as are spectroscopic and data-analysis algorithms.

There is considerable interest in developing direct measurement methods to determine the plutonium content of spent nuclear fuel within a fuel assembly. One technique that may prove successful is lead slowing-down spectroscopy. Lead Slowing Down Spectroscopy (LSDS) has been used for decades to make cross-section measurements on relatively small isotopic samples of well know masses. For spent fuel assembly measurements, LSDS will be applied in reverse; unknown masses will be determined using well-know cross-sections. In the LSDS, a pulse of neutrons (on the order of 10-100 MeV) is injected into a large lead stack (~ 1m3). The neutrons quickly down-scatter but exhibit little spread in energy about the average, continually-decreasing neutron energy making for a strong correlation between the elapsed time from the initial pulse and the average energy of the neutron. By measuring this elapsed time, it is possible to measure interactions of the neutrons with the fuel in the 0.1 to 1,000 eV range. Many of the actinides have strong resonances in this region, making it possible, through careful measurements and analysis, to extract isotopic masses from LSDS measurements. Pacific Northwest National Laboratory is actively conducting research on both LSDS measurement and data analysis techniques. This paper willmore » present results of the effort to construct and characterize a new lead slowing down spectrometer. The spectrometer was designed to begin testing both experimental measurement and data analysis techniques for determining the plutonium content of spent fuel. To characterize the spectrometer, a series of (n,γ) experiments were conducted to measure the correlation between the time after the neutrons enter the lead and the energy of the interaction. Results from these measurements as well as plans for future development of the spectrometer will be discussed.« less

Safeguards inspectors currently visit uranium enrichment plants to verify UF6 cylinder enrichment declarations. Measurements are performed with handheld high-resolution detectors on a limited number of cylinders taken to be representative of the plant’s cylinder inventory. These enrichment assay methods interrogate only a small fraction of the total cylinder volume, and are time-consuming and expensive to execute. Pacific Northwest National Laboratory (PNNL) is developing an automated UF6 cylinder verification station concept based on the combined collection of traditional enrichment-meter data (186 keV photons from 235U) and non-traditional, neutron-induced, high-energy gamma-ray signatures (3-8 MeV) with an array of collimated, medium-resolution scintillators. Previous work at PNNL (2010) demonstrated proof-of-principle that this hybrid method yields accurate, full-volume assay of the cylinder enrichment, reduces systematic errors when compared to several other enrichment assay methods, and provides simplified instrumentation and algorithms suitable for long-term, unattended operations. This system aims to increase the number of inspected cylinders at higher accuracy and with lower cost than when compared to inspectors with hand-held instruments. Several measurement campaigns of 30B cylinder populations and a refined MCNP model will be reported. The MCNP model consists of per-gram basis vectors for the different uranium isotopes and several fill geometries, enabling fast generationmore » of any UF6 enrichment level and multiple configurations. The refined model was used to optimize collimator design and detector configuration for the hybrid method. In addition, a new field prototype based on model results was utilized in a set of field measurements.« less

Fast neutron detection has applications in a number of topic areas, including national security and nuclear fuel cycle safeguards. Ideally, these sensors would have high sensitivity to fission (fast) neutrons but be insensitive to thermal neutrons and gamma rays. This paper describes a study of actinide-loaded glass for fast neutron detection, wherein a threshold fission reaction in the actinide produces fission products depositing approximately 200 MeV of energy. The prominent advantage of this approach to fast neutron detection, when compared to fission chambers, is the potential for several orders of magnitude increase in the mass of fissionable atoms per unit volume-thereby improving the absolute detection efficiency and offsetting the small (approximately 1 barn) threshold cross-sections.The detectors tested to date are glass-matrix based, loaded with thorium and a rare-earth activator. The threshold cross-section for fission of (232)Th (100% natural abundance) provides insensitivity to thermal neutrons, but the primary research question is whether the 200 MeV of energy released per fission is sufficiently distinct, in terms of total scintillation light and/or scintillation decay time, to be clearly distinguished from gamma rays and the inherent alpha emissions in the actinide. The high density of ionization and resulting propensity for recombination is expected to reduce the scintillation production well below that corresponding to 200 MeV electron equivalent.Technical challenges to be overcome in the fabricating actinide-loaded glasses and the testing of these early samples are significant. These include making a glass containing thorium and the proper activator that will scintillate, discriminating fast neutron events from the natural radioactivity of 232Th and its daughters and minimizing the severity of the non-linearity of energy to light conversion for the fission fragments. The first obstacle has been overcome; scintillating glass samples containing thorium have been produced and spectra on these samples have been acquired. These spectra as well as initial tests of fast neutron detection are presented here, along with a discussion of the research paths to be explored in the future. (C) 2010 Elsevier B.V. All rights reserved.

International Atomic Energy Agency (IAEA) inspectors currently perform periodic inspections at uranium enrichment plants to verify UF6 cylinder enrichment declarations. Measurements are typically performed with handheld high-resolution sensors on a sampling of cylinders taken to be representative of the facility's entire cylinder inventory. These measurements are time-consuming and assay only a small fraction of the total cylinder volume. An automated nondestructive assay system capable of providing enrichment measurements over the full volume of the cylinder could improve upon current verification practices in terms of manpower and assay accuracy. Pacific Northwest National Laboratory is developing an Integrated Cylinder Verification System (ICVS) intended for this purpose and has developed a field prototype of the nondestructive assay (NDA) components of an ICVS. The nondestructive assay methods would combine the “traditional” enrichment-meter signature (i.e. 186-keV emission from U-235) as well as “nontraditional” high-energy photon signatures derived from neutrons produced primarily by F-19(α,n) reactions. This paper describes the design, calibration and characterization of the NaI(Tl) and LaBr3(Ce) spectrometers utilized in the field prototype. An overview of a recent field measurement campaign is then provided, supported by example gamma-ray pulse-height spectra collected on cylinders of known enrichment.

Pacific Northwest National Laboratory (PNNL) is developing the concept of an automated UF6 cylinder verification station that would be located at key measurement points to positively identify each cylinder, measure its mass and enrichment, store the collected data in a secure database, and maintain continuity of knowledge on measured cylinders until the arrival of International Atomic Energy Agency (IAEA) inspectors. At the center of this unattended system is a hybrid enrichment assay technique that combines the traditional enrichment-meter method (based on the 186 keV peak from 235U) with non-traditional neutron-induced high-energy gamma-ray signatures (spawned primarily by 234U alpha emissions and 19F(alpha, neutron) reactions). Previous work by PNNL provided proof-of-principle for the non-traditional signatures to support accurate, full-volume interrogation of the cylinder enrichment, thereby reducing the systematic uncertainties in enrichment assay due to UF6 heterogeneity and providing greater sensitivity to material substitution scenarios. The work described here builds on that preliminary evaluation of the non-traditional signatures, but focuses on a prototype field system utilizing NaI(Tl) and LaBr3(Ce) spectrometers, and enrichment analysis algorithms that integrate the traditional and non-traditional signatures. Results for the assay of Type-30B cylinders ranging from 0.2 to 4.95 wt% 235U, at an AREVA fuel fabrication plant in Richland, WA, are described for the following enrichment analysis methods: 1) traditional enrichment meter signature (186 keV peak) as calculated using a square-wave convolute (SWC) algorithm; 2) non-traditional high-energy gamma-ray signature that provides neutron detection without neutron detectors and 3) hybrid algorithm that merges the traditional and non-traditional signatures. Uncertainties for each method, relative to the declared enrichment for each cylinder, are calculated and compared to the uncertainties from an attended HPGe verification station at AREVA, and the IAEA’s uncertainty target values for feed, tail and product cylinders. A summary of the major findings from the field measurements and subsequent analysis follows: • Traditional enrichment-meter assay using specially collimated NaI spectrometers and a Square-Wave-Convolute algorithm can achieve uncertainties comparable to HPGe and LaBr for product, natural and depleted cylinders. • Non-traditional signatures measured using NaI spectrometers enable interrogation of the entire cylinder volume and accurate measurement of absolute 235U mass in product, natural and depleted cylinders. • A hybrid enrichment assay method can achieve lower uncertainties than either the traditional or non-traditional methods acting independently because there is a low degree of correlation in the systematic errors of the two individual methods (wall thickness variation and 234U/235U variation, respectively). This work has indicated that the hybrid NDA method has the potential to serve as the foundation for an unattended cylinder verification station. When compared to today’s handheld cylinder-verification approach, such a station would have the following advantages: 1) improved enrichment assay accuracy for product, tail and feed cylinders; 2) full-volume assay of absolute 235U mass; 3) assay of minor isotopes (234U and 232U) important to verification of feedstock origin; single instrumentation design for both Type 30B and Type 48 cylinders; and 4) substantial reduction in the inspector manpower associated with cylinder verification.

Direct measurement of Pu in spent nuclear fuel remains a key challenge for safeguarding nuclear fuel cycles of today and tomorrow. Lead slowing-down spectroscopy (LSDS) is an active nondestructive assay method that has the potential to provide independent, direct measurement of Pu and U isotopic mass with an uncertainty lower than the approximately 10 percent typical of today’s confirmatory assay methods. Pacific Northwest National Laboratory’s (PNNL) previous work to assess the viability of LSDS for the assay of pressurized water reactor (PWR) assemblies indicated that the method could provide direct assay of Pu-239 and U-235 (and possibly Pu-240 and Pu-241) with uncertainties less than a few percent, assuming suitably efficient instrumentation, an intense pulsed neutron source, and improvements in the time-spectra analysis methods used to extract isotopic information from a complex LSDS signal. This previous simulation-based evaluation used relatively simple PWR fuel assembly definitions (e.g. constant burnup across the assembly) and a constant initial enrichment and cooling time. The time-spectra analysis method was founded on a preliminary analytical model of self-shielding intended to correct for assay-signal nonlinearities introduced by attenuation of the interrogating neutron flux within the assembly.

International Atomic Energy Agency (IAEA) inspectors currently perform periodic inspections at uranium enrichment plants to verify UF6 cylinder enrichment declarations. Measurements are typically performed with handheld high-resolution sensors on a sampling of cylinders taken to be representative of the facility's entire product-cylinder inventory. Pacific Northwest National Laboratory (PNNL) is developing a concept to automate the verification of enrichment plant cylinders to enable 100 percent product-cylinder verification and potentially, mass-balance calculations on the facility as a whole (by also measuring feed and tails cylinders). The Integrated Cylinder Verification System (ICVS) could be located at key measurement points to positively identify each cylinder, measure its mass and enrichment, store the collected data in a secure database, and maintain continuity of knowledge on measured cylinders until IAEA inspector arrival. The three main objectives of this FY09 project are summarized here and described in more detail in the report: (1) Develop a preliminary design for a prototype NDA system, (2) Refine PNNL's MCNP models of the NDA system, and (3) Procure and test key pulse-processing components. Progress against these tasks to date, and next steps, are discussed.