L. Eric Smith

The photon haystack and emerging radiation detection technology

The resources devoted to interdicting special nuclear materials have increased considerably over the last several years in step with growing efforts to counter nuclear proliferation and nuclear terrorism. This changing landscape has led to a large amount of research and development that aims to improve the effectiveness of technology now deployed worldwide. Interdicting special nuclear materials is most commonly addressed by detecting and characterizing emitted gamma rays, but modest signature emissions can be obscured by attenuating material and must be differentiated from large and highly variable environmental background emissions. It is a daunting technical challenge to identify special nuclear materials via gamma-ray detection, but a host of new detection technologies is now emerging. This challenge motivates our review of special nuclear material signatures, the physics of detection approaches, emerging technologies, and performance metrics. The use of benchmark gamma-ray sources aids our discussion.

High-Energy Delayed Gamma Spectroscopy for Spent Nuclear Fuel Assay

High-accuracy, direct, nondestructive measurement of fissile and fissionable isotopes in spent fuel, particularly the Pu isotopes, is a well-documented, but still unmet challenge in international safeguards. As nuclear fuel cycles propagate around the globe, the need for improved materials accountancy techniques for irradiated light-water reactor fuel will increase. This modeling study investigates the use of delayed gamma rays from fission-product nuclei to directly measure the relative concentrations of 235U, 239Pu, and 241Pu in spent fuel assemblies. The method is based on the unique distribution of fission-product nuclei produced from fission in each of these fissile isotopes. Fission is stimulated in the assembly with a pulse-capable source of interrogating neutrons. The measured distributions of the short-lived fission products from the unknown sample are then fit with a linear combination of the known fission-product yield curves from pure 235U, 239Pu, and 241Pu to determine the original proportions of these fissile isotopes. Modeling approaches for the intense gamma-ray background promulgated by the long-lived fission-product inventory and for the high-energy gamma-ray signatures emitted by short-lived fission products from induced fission are described. Benchmarking measurements are presented and compare favorably with the results of these models. Results for the simulated assay of simplified individual fuel rods ranging from fresh to 60-GWd/MTU burnup demonstrate the utility of the modeling methods for viability studies, although additional work is needed to more realistically assess the potential of High-Energy Delayed Gamma Spectroscopy (HEDGS).

Signatures and Methods for the Automated Nondestructive Assay of

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 facilitys entire cylinder inventory. These measurements are time-consuming, expensive, 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. The 185-keV emission from U-235 is utilized in todays cylinder measurements, but augmenting this “traditional” signature with more-penetrating “non-traditional” signatures could help to achieve full-volume assay in an automated system. This paper describes the study of non-traditional signatures that include neutrons produced by F-19 (α, n) reactions (spawned primarily from U-234 alpha emission) and the high-energy gamma rays (extending up to 8 MeV) induced by those neutrons when they interact in the cylinder wall and nearby materials. The potential of these non-traditional signatures and assay methods for automated cylinder verification is explored using field measurements on a small population of cylinders ranging from 2.0% to 5% in U-235 enrichment. The standard deviation of the non-traditional high-energy gamma-ray assay approach was 4.7% relative to the declared cylinder enrichments; the standard deviation of the traditional enrichment meter approach using a well-collimated high-resolution spectrometer was 4.3%. The prospect of using the non-traditional high-energy gamma-ray signature in concert with the traditional 185-keV signature to reduce the uncertainty of automated cylinder assay is discussed.

{\rm UF}_{6}

Radiation transport modeling methods used in the radiation detection community fall into one of two broad categories: stochastic (Monte Carlo) and deterministic. Monte Carlo methods are typically the tool of choice for simulating gamma-ray spectrometers operating in homeland and national security settings (e.g. portal monitoring of vehicles or isotope identification using handheld devices), but deterministic codes that discretize the linear Boltzmann transport equation in space, angle, and energy offer potential advantages in computational efficiency for many complex radiation detection problems. This paper describes the development of deterministic algorithms for simulating gamma-ray spectroscopy scenarios. Key challenges include: formulating methods to automatically define an energy group structure that can support modeling of gamma-ray spectrometers ranging from low to high resolution; combining deterministic transport algorithms (e.g. ray-tracing and discrete ordinates) to mitigate ray effects for a wide range of problem types; and developing efficient and accurate methods to calculate gamma-ray spectrometer response functions from the deterministic angular flux solutions. In this paper, the software framework aimed at addressing these challenges is described and results from test problems that compare deterministic and Monte Carlo approaches are provided.

Cylinders at Uranium Enrichment Plants

Abstract Multicoincidence radionuclide analysis systems consisting of light-charged-particle detectors operating in coincidence with photon spectrometers are being developed to improve the sensitivity of radionuclide analysis in field applications. Requiring charged-particle/photon coincidence provides active shielding from environmental photon sources, and mapping photon–photon events into a coincidence plane can remove photon spectroscopy interferences. List-mode data acquisition and flexible hardware design ensures that the most sensitive coincidence schemes involving β, atomic electron, γ and X-ray emissions can be used for radionuclide quantification. System hardware design and preliminary measurement data are discussed. A centerpiece component of this project, the development of analysis tools and data libraries required to perform automated multicoincidence analysis, is also described.

Deterministic Transport Methods for the Simulation of Gamma-Ray Spectroscopy Scenarios

Nondestructive techniques for measuring the mass of fissile isotopes in spent nuclear fuel is a considerable challenge in the safeguarding of nuclear fuel cycles. A nondestructive assay technology that could provide direct measurement of fissile mass, particularly for the plutonium (Pu) isotopes, and improve upon the uncertainty of todays confirmatory methods is needed. Lead slowing-down spectroscopy (LSDS) has been studied for the spent fuel application previously, but the nonlinear effects of assembly self shielding (of the interrogating neutron population) have led to discouraging assay accuracy for realistic pressurized water reactor fuels. In this paper, we describe the development of time-spectral analysis algorithms for LSDS intended to overcome these self-shielding effects. The algorithm incorporates the tabulated energy-dependent cross sections from key fissile and absorbing isotopes, but leaves their mass as free variables. Multi-parameter regression analysis is then used to directly calculate not only the mass of fissile isotopes in the fuel assembly (e.g., Pu-239, U-235, and Pu-241), but also the mass of key absorbing isotopes such as Pu-240 and U-238. Modeling-based assay results using this self-shielding relationship indicate that LSDS has the potential to directly measure fissile isotopes with less than 5% average relative error for pressurized water reactor assemblies with burnup as high as 60 GWd/MTU. Shortcomings in the initial self-shielding model and potential improvements to the formulation are described.

Development of portable multicoincidence radionuclide analysis systems

Passive gamma-ray spectrometers composed of attenuation filters and integrating detection materials provide important advantages for measurements in high-radiation environments and for long-term monitoring. Each of these applications has requirements that constrain the design of the instrument, such as incident energy range of interest, sensor size and weight, readout method, and cost. The multitude of parameters in passive spectrometer design (e.g., attenuation filter material and thickness, integrating sensor type, number of pixels, reconstructed energy bin structure) results in a large design space to examine. The development of generalized design optimization tools to interrogate this space and to identify promising spectrometer designs is discussed, particularly the methods used to rapidly calculate system transfer functions and the use of genetic algorithms for design optimization. Preliminary measurements to validate the design tools are described, and example results from early design optimization efforts are provided.