Proposed thorium-based nuclear fuel cycles are likely to require quantification and verification of 233U within nuclear material. Because of their similar fission cross sections, active neutron nondestructive assay (NDA) systems may respond similarly to 233U and 235 U. Traditional safeguards equipment has been optimized for 235U and 238U quantification associated with conventional uranium/plutonium fuel cycles and may not be directly applicable to 233U quantification when mixed with other actinides. This work used models of the large volume active well coincidence counter (LV-AWCC) at Oak Ridge National Laboratory to evaluate the performance of this neutron NDA system to differentiate fissile uranium isotopes. The models were developed to simulate NDA system performance in response to a number of triangular radiation signature training device sources within the central cavity or well. This work predicted that the LV-AWCC can effectively differentiate 233U from 235U in certain modes of operation. Inactive mode, the LV-AWCC with the cadmium liner results indifferent doubles count rates between the fissile isotopes fora given fissile uranium mass. Without the cadmium liner, the uranium isotopes provide a statistically indistinguishable doubles count rate response for the fissile masses considered in this work (up to approximately 150 g). The cadmium liner serves to harden the neutron interrogation spectrum, which better exploits the notable difference in the 233U and 235U fission cross sections at approximately 1 eV. In passive mode, the two fissile isotopes exhibit different doubles and singles count rates regardless of liner presence because the passive source strength of 233U is approximately 2 orders of magnitude stronger than that of 235U due to the shorter half-life and correspondingly higher (alpha, n) yield. We conclude that using neutron interrogation in the LV-AWCC, two measurements are needed to quantify 233U content in mixed uranium items. The first measurement is used to determine the total fissile uranium mass using a mode that cannot distinguish fissile isotopes (i.e., where a similar response is observed for both fissile uranium isotopes such as active doubles without cadmium or using a thermal neutron interrogation source). The second measurement is used to determine the 233U content by using a differentiating technique (e.g., passive doubles, passive doubles to singles ratio, active doubles with cadmium).

Most of the Pu separated from irradiated commercial nuclear fuel is stored as PuO 2. The primary quantitative nondestructive measurement technique used to verify the amount of Pu in storage containers is passive neutron correlation counting. An important physical property of the oxide material is the ratio, α, of the rate of (α, n) neutrons produced inside the item to the rate of neutrons produced by spontaneous fission. This ratio influences the precision of the correlated counting method and affects the interpretation of the data because of how it changes both the primary total neutron production rate and the rate of induced fission events taking place inside the item. In addition to the main O(α, n) contribution, additional contributions come from α-particle interactions with light element impurities that are inevitably present. In this work, we calculate specific (α, n) yield coefficients, expressed in units of neutrons per second per gram of α-emitting nuclide per part per million by mass of the specified impurity element distributed in a pure PuO 2 matrix, for some key α-emitting actinides commonly present in reprocessed Pu (238–242Pu+241Am). These coefficients are directly applicable to nuclear safeguards verification work in which the α ratio is often calculated from the Pu-isotopic composition and chemical information obtained by other means. They also provide a convenient up-to-date reference set against which values generated by other methods can be compared. Results are presented for impurities with atomic number from 3 to 17 inclusive, plus K and Fe. In most cases, these coefficients are not expected to change by more than 5%–10% at any time in the future. However, as new data become available, changes as large as 20% may be needed for some targets (e.g., F). The present yield calculations are limited by the general shortage of quality experimental total (α, n) reaction cross section data, which, together with unexplained variation between determinations, means that an objective and coherent evaluation is not possible. The situation is even less satisfactory for the partial differential cross section needed to calculate neutron spectra.

Passive neutron multiplicity counting can be used to determine the absolute emission rate of Cf-252 spontaneous fission sources. Such sources can then be used to characterize and calibrate instruments used to assay Pu for materials control and accountancy, nuclear safeguards, and nuclear security applications. An important contribution determining the ultimate accuracy of this technique is how well the neutron multiplicity distribution of Cf-252 is known (actually the low order factorial moments are typically used). This knowledge governs how well the emission rate of the Cf-252 sources can be determined. Additionally, because Cf-252 is used as a reference standard against which other spontaneously fissile systems are compared, it also governs the scaling of the Cf-252 characterization and calibration data to the corresponding performance estimates for the spontaneously fissile Pu-nuclides. The main scale setting parameter is nu-bar, the average number of neutrons released following fission, of Cf-252. This is a fundamental nuclear constant. In this work we briefly review the 14 high quality absolute determinations of nu-bar and subject them to a full covariance evaluation. This is compared to several variants of weighted mean, including an extension where an allowance is made for the uncertainty in the estimated variance on each point. The prompt nu-bar value was found to be robust to the different statistical assessment methods applied, and moreover, the overall uncertainty estimates were of similar magnitude. Based on the full covariance treatment a prompt nu-bar value of (3.7573 +/- 0.0056) prompt neutrons per fission was obtained, where the uncertainty is at the 1-sigma level (68% confidence interval). This compares favorably with the value of Zucker and Holden, (3.757 +/- 0.010) prompt neutrons per fission, long used in the nuclear safeguards community. The relative standard deviation of 0.15% obtained from the analysis reported here is sufficiently small that we advocate for a new high accuracy determination of the delayed neutron contribution, since this is needed to correct the Mn-bath class of nu-bar measurements. Collectively the measurements span the period 1963 to 1985. Of the 14 measurements six carry very little weight (individually 2% or less), five carry intermediate weight (individually 3%-7%), while three values are highly weighted (individually 15%-32%). These have reported relative standard deviations of between 0.2% and 0.3%. Given the small number of measurements with small reported uncertainties, and the fact that the youngest such determination is over 30 years old, we also strongly suggest that new measurements of the highest currently achievable quality are needed. In this regard a high efficiency He-3 based counter would remove the residual concern over gamma-sensitivity of doped liquid scintillator tank data.

Natural, depleted, and low enriched uranium hexafluoride is manufactured and transported on an industrial scale to support commercial nuclear power plant operation. One-way material production and flow is verified by nuclear safeguards inspectorates is by neutron counting. The dominant neutron source term is (α,n) production due to 234U which gets enriched/depleted along with 235U. In this paper we describe recent efforts to accurately determine the (α,n)/s/g of 234U in UF6. This piece of nuclear data is of direct value to the nuclear safeguards community in the science-based verification and assay of bulk uranium hexafluoride. It also provides a benchmark on codes that calculate yield curves for various compounds from cross section data, and hence, provides a scale or normalization constraint on evaluated basic cross section data. In turn, evaluated basic data allows the yield from other materials to be calculated; for instance, moist uranyl fluoride, which is of interest in holdup measurements.

Bulk uranium items are often measured using active neutron interrogation systems to take advantage of the relatively high penetrability of neutrons, providing the ability to measure uranium mass in large, dense configurations. Because the emitted neutrons from 235U and 238U in such configurations are, for all practical purposes, indistinguishable, established active measurement techniques require many representative calibration standards and/or well-known isotopic information to interpret the assay results (i.e., extract an isotopic mass from the effective mass). The primary objective of this work is to investigate the ability of a dual-energy neutron interrogation technique to estimate uranium enrichment for bulk materials, which has the potential to eliminate the need for a (traditionally separate) gamma isotopic measurement. Dual neutron interrogation energies were achieved by adding a deuterium–tritium (D–T) neutron generator into the measurement chamber of the Oak Ridge National Laboratory 252Cf Shuffler. This new technique exploits the change in fission rates as a function of interrogating neutron energy to independently determine the 235U and 238U content in the measurement item. Results from traditional 252Cf measurements and the new D–T measurements were then used to develop a relationship between uranium enrichment and the ratio of the two delayed neutron count rates. Technical feasibility is successfully demonstrated using the modified 252Cf Shuffler as a test bed, although several areas where refinements are both possible and needed before DEANI can be deployed as an analytical tool to meet specific measurement goals are identified.

He-3 gas has been used in various scientific and security applications for decades, but it is now in short supply. Alternatives to He-3 detectors are currently being integrated and tested in neutron coincidence counter designs, of a type which are widely used in nuclear safeguards for nuclear materials assay. A boron-coated-straw-based design, similar to the High-Level Neutron Coincidence Counter-II, was built by Proportional Technologies Inc., and has been tested by the Oak Ridge National Laboratory (ORNL) at both the JRC in Ispra and ORNL. Characterization measurements, along with nondestructive assays of various plutonium samples, have been conducted to determine the performance of this coincidence counter replacement in comparison with other similar counters. This paper presents results of these measurements.

Neutron time correlation analysis is one of the main technical nuclear safeguards techniques used to verify declarations of, or to independently assay, special nuclear materials. Quantitative information is generally extracted from the neutron-event pulse train, collected from moderated assemblies of He-3 proportional counters, in the form of correlated count rates that are derived from event-triggered coincidence gates. These count rates, most commonly referred to as singles, doubles and triples rates etc., when extracted using shift-register autocorrelation logic, are related to the reduced factorial moments of the time correlated clusters of neutrons emerging from the measurement items. Correcting these various rates for dead time losses has received considerable attention recently. The dead time losses for the higher moments in particular, and especially for large mass (high rate and highly multiplying) items, can be significant. Consequently, even in thoughtfully designed systems, accurate dead time treatments are needed if biased mass determinations are to be avoided. In support of this effort, in this paper we discuss a new approach to experimentally estimate the effective system dead time of neutron coincidence counting systems. It involves counting a random neutron source (e.g. AmLi is a good approximation to a source without correlated emission) and relating the second and higher moments of the neutron number distribution recorded in random triggered interrogation coincidence gates to the effective value of dead time parameter. We develop the theoretical basis of the method and apply it to the Oak Ridge Large Volume Active Well Coincidence Counter using sealed AmLi radionuclide neutron sources and standard multiplicity shift register electronics. The method is simple to apply compared to the predominant present approach which involves using a set of Cf-252 sources of wide emission rate, it gives excellent precision in a conveniently short time, and it yields consistent results as a function of the order of the moment used to extract the dead time parameter. This latter observation is reassuring in that it suggests the assumptions underpinning the theoretical analysis are fit for practical application purposes. However, we found that the effective dead time parameter obtained is not constant, as might be expected for a parameter that in the dead time model is characteristic of the detector system, but rather, varies systematically with gate width. Published by Elsevier B.V.

The objective of this project was to design and optimize, in simulation space, an active neutron coincidence counter (or collar) using boron-coated straws (BCSs) as a non-3He replacement to the Uranium Neutron Coincidence Collar (UNCL). UNCL has been used by the International Atomic Energy Agency (IAEA) and European Atomic Energy Community (Euratom) since the 1980s to verify the 235U content in fresh light water reactor fuel assemblies for safeguards purposes. This report documents the design and optimization of the BCS collar.

The 235U mass assay of bulk uranium items, such as oxide canisters, fuel pellets, and fuel assemblies, is not achievable by traditional gamma-ray assay techniques due to the limited penetration of the item by the characteristic 235U gamma rays. Instead, fast neutron interrogation methods such as active neutron coincidence counting must be used. For international safeguards applications, the most commonly used active neutron systems, the Active Well Coincidence Counter (AWCC), Uranium Neutron Collar (UNCL) and 252Cf Shuffler, rely on fast neutron interrogation using an isotopic neutron source [i.e., 252Cf or Am(Li)] to achieve better measurement accuracies than are possible using gamma-ray techniques for high-mass, high-density items. However, the Am(Li) sources required for the AWCC and UNCL systems are no longer manufactured, and newly produced systems rely on limited supplies of sources salvaged from disused instruments. The 252Cf shuffler systems rely on the use of high-output 252Cf sources, which while still available have become extremely costly for use in routine operations and require replacement every five to seven years. Lack of a suitable alternative neutron interrogation source would leave a potentially significant gap in the safeguarding of uranium processing facilities. In this work, we made use of Oak Ridge National Laboratory’s (ORNL’s) Large Volume Active Well Coincidence Counter (LV-AWCC) and a commercially available deuterium-deuterium (D-D) neutron generator to examine the potential of the D-D neutron generator as an alternative to the isotopic sources. We present the performance of the LV-AWCC with D-D generator for the assay of 235U based on the results of Monte Carlo N-Particle (MCNP) simulations and measurements of depleted uranium (DU), low enriched uranium (LEU), and highly enriched uranium (HEU) items.

The potential performance of a notional active coincidence collar for assaying uranium fuel based on segmented detectors constructed from the new PSD plastic fast organic scintillator with pulse shape discrimination capability was investigated in simulation. Like the International Atomic Energy Agency's present Uranium Neutron Collar for LEU (UNCL), the PSD plastic collar would also function by stimulating fission in the 235U content of the fuel with a moderated 241Am/Li neutron source and detecting instances of induced fission via neutron coincidence counting. In contrast to the moderated detectors of the UNCL, the fast time scale of detection in the scintillator eliminates statistical errors due to accidental coincidences that limit the performance of the UNCL. However, the potential to detect a single neutron multiple times historically has been one of the properties of organic scintillator detectors that has prevented their adoption for international safeguards applications. Consequently, as part of the analysis of simulated data, a method was developed by which true neutron-neutron coincidences can be distinguished from inter-detector scatter that takes advantage of the position and timing resolution of segmented detectors. Then, the performance of the notional simulated coincidence collar was evaluated for assaying a variety of fresh fuels, including some containing burnable poisons and partial defects. In these simulations, particular attention was paid to the analysis of fast mode measurements. In fast mode, a Cd liner is placed inside the collar to shield the fuel from the interrogating source and detector moderators, thereby eliminating the thermal neutron flux that is most sensitive to the presence of burnable poisons that are ubiquitous in modern nuclear fuels. The simulations indicate that the predicted precision of fast mode measurements is similar to what can be achieved by the present UNCL in thermal mode. For example, the statistical accuracy of a ten-minute measurement of fission coincidences collected in fast mode will be approximately 1% for most fuels of interest, yielding a ~1.4% error after subtraction of a five minute measurement of the spontaneous fissions from 238U in the fuel, a ~2% error in analyzed linear density after accounting for the slope of the calibration curve, and a ~2.9% total error after addition of an assumed systematic error of 2%.

The hold-up measurement of low-enriched uranium materials may require use of alternate detector types relative to the measurement of highly enriched uranium. This is in part due to the difference in process scale (i.e., the components are generally larger for low-enriched uranium systems), but also because the characteristic gamma-ray lines from 235U used for assay of highly enriched uranium will be present at a much reduced intensity (on a per gram of uranium basis) at lower enrichments. Researchers at Oak Ridge National Laboratory examined the performance of several standard detector types, e.g., NaI(Tl), LaBr3(Ce), and HPGe, to select a suitable candidate for measuring and quantifying low-enriched uranium hold-up in process pipes and equipment at the Portsmouth gaseous diffusion plant. Detector characteristics, such as energy resolution (full width at half maximum) and net peak count rates at gamma ray energies spanning a range of 60–1332 keV, were measured for the above-mentioned detector types using the same sources and in the same geometry. Uranium enrichment standards (Certified Reference Material no. 969 and Certified Reference Material no. 146) were measured using each of the detector candidates in the same geometry. The net count rates recorded by each detector at 186 keV and 1,001 keV were plotted as a function of enrichment (atom percentage). Background measurements were made in unshielded and shielded configurations under both ambient and elevated conditions of 238U activity. The highly enriched uranium hold-up measurement campaign at the Portsmouth plant was performed on process equipment that had been cleaned out. Therefore, in most cases, the thickness of the uranium deposits was less than the “infinite thickness” for the 186 keV gamma rays to be completely self-attenuated. Because of this, in addition to measuring the 186 keV gamma, the 1,001 keV gamma ray from 234mPa—a daughter of 238U in secular equilibrium with its parent—will also need to be measured. Based on the performance criteria of detection efficiency, energy resolution, peak-to-continuum ratios, minimum detectable limits, and the weight of the shielded probe, a shielded (0.5 in. thick lead shield) 2 × 2 in. NaI(Tl) detector is recommended for use. The recommended approach is to carry out analysis using data from both 186 keV and 1,001 keV gamma rays, and select a best result based on propagated uncertainty estimates. It is also highly recommended that a two-point gain stabilization scheme based on an 241Am seed embedded in the probe be implemented. Shielding configurations to reduce the impact of background interference on the measurement of 1,001 keV gamma-ray are discussed.

By around 2025, thorium-based fuel cycles are likely to be deployed internationally. States such as China and India are pursuing research, development, and deployment pathways toward a number of commercial-scale thorium fuel cycles, and they are already building test reactors and the associated fuel cycle infrastructure. In the future, the potential exists for these emerging programs to sell, export, and deploy thorium fuel cycle technology in other states. Without technically adequate international safeguards protocols and measures in place, any future potential clandestine misuse of these fuel cycles could go undetected, compromising the deterrent value of these protocols and measures. The development of safeguards approaches for thorium-based fuel cycles is therefore a matter of some urgency. Yet, the focus of the international safeguards community remains mainly on safeguarding conventional U-235- and (PU)-P-239-based fuel cycles while the safeguards challenges of thorium-uranium fuel cycles remain largely uninvestigated. This raises the following question: Is the International Atomic Energy Agency and international safeguards system ready for thorium fuel cycles? Furthermore, is the safeguards technology of today sufficiently mature to meet the verification challenges posed by thorium-based fuel cycles? In defining these and other related research questions, the objectives of this paper are to identify key safeguards considerations for thorium-based fuel cycles and to call for an early dialogue between the international safeguards and the nuclear fuel cycle communities to prepare for the potential safeguards challenges associated with these fuel cycles. In this paper, it is concluded that directed research and development programs are required to meet the identified safeguards challenges and to take timely action in preparation for the international deployment of thorium fuel cycles.

Hybrid K-edge densitometry (HKED) is a non-destructive analytical assay technique used to provide rapid determination of actinide concentration in tank solutions. Of special interest for HKED is the estimation, along with associated uncertainties, of the ratio of the flouresence yeilds, ω K, of uranium and plutonium. Limited experimental data for ω K(Z) as a function of atomic number, Z, exist and the data are subject to experimental uncertainty. Previous studies have provided values for ω K(Z) with uncertainty estimates but have not included covariance information. We use a phenomenological model with a bootstrapping method to generate the ratio ω K(94)/ω K(92) and associated uncertainty.

Correlated neutron counting using multiplicity shift register logic extracts the first three factorial moments from the detected neutron pulse train. The descriptive properties of the measurement item (mass, the ratio of (alpha,n) to spontaneous fission neutron production, and leakage self-multiplication) are related to the observed singles (S), doubles (D) and triples (T) rates, and this is the basis of the widely used multiplicity counting assay method. The factorial moments required to interpret and invert the measurement data in the framework of the point kinetics model may be calculated from the spontaneous fission prompt neutron multiplicity distribution P(v). In the case of U-238 very few measurements of P(v) are available and the derived values, especially for the higher factorial moments, are not known with high accuracy.In this work, we report the measurement of the triples rate per gram of U-238 based on the analysis of a set of measurements in which a collection of 10 cylinders of UO2F2, each containing about 230 g of compound, were measured individually and in groups. Special care was taken to understand and compensate the recorded multiplicity histograms for the effect of random cosmic-ray induced background neutrons, which, because they also come in bursts and mimic fissions but with a different and harder multiplicity distribution. We compare our fully corrected (deadtime, background, efficiency, multiplication) experimental results with first principles expectations based on evaluated nuclear data. Based on our results we suspect that the current evaluated nuclear data is biased, which points to a need to undertake new basic measurements of the U-238 prompt neutron multiplicity distribution. Published by Elsevier B.V.

This report presents results and analysis from a series of proof-of-concept measurements to assess the suitability of segmented detectors constructed from Eljen EJ-299-34 PSD-plastic scintillator with pulse-shape discrimination capability for the purposes of quantifying uranium via active neutron coincidence counting. Present quantification of bulk uranium materials for international safeguards and domestic materials control and accounting relies on active neutron coincidence counting systems, such as the Active Well Coincidence Counter (AWCC) and the Uranium Neutron Coincidence Collar (UNCL), that use moderated He-3 proportional counters along with necessarily low-intensity 241Am(Li) neutron sources. Scintillation-based fast-neutron detectors are a potentially superior technology to the existing AWCC and UNCL designs due to their spectroscopic capability and their inherently short neutron coincidence times that largely eliminate random coincidences and enable interrogation by stronger sources. One of the past impediments to the investigation and adoption of scintillation counters for the purpose of quantifying bulk uranium was the commercial availability of scintillators having the necessary neutron-gamma pulse-shape discrimination properties only as flammable liquids. Recently, Eljen EJ-299-34 PSD-plastic scintillator became commercially available. The present work is the first assessment of an array of PSD-plastic detectors for the purposes of quantifying bulk uranium. The detector panel used in the present work was originally built as the focal plane for a fast-neutron imager, but it was repurposed for the present investigation by construction of a stand to support the inner well of an AWCC immediately in front of the detector panel. The detector panel and data acquisition of this system are particularly well suited for performing active-well fast-neutron counting of LEU and HEU samples because the active detector volume is solid, the 241Am(Li) interrogating neutrons are largely below the detector threshold, and the segmented construction of the detector modules allow for separation of true neutron-neutron coincidences from inter-detector scattering using the kinematics of neutron scattering. The results from a series of measurements of a suite of uranium standards are presented, and compared to measurements of the same standards and source configurations using the AWCC. Using these results, the performance of the segmented detectors reconfigured as a well counter is predicted and outperforms the AWCC.