Design and testing of a unique active Compton-suppressed LaBr3(Ce) detector system for improved sensitivity assays of TRU in remote-handled TRU wastes

The US Department of Energy’s transuranic (TRU) waste inventory includes about 4,500 m3 of remote-handled TRU (RH-TRU) wastes composed of a variety of containerized waste forms having a contact surface dose rate that exceeds 2 mSv/hr (200 mrem/hr) containing waste materials with a total TRU concentration greater than 3700 Bq/g (100 nCi/g). As part of a research project to investigate the use of active Compton-suppressed room-temperature gamma-ray detectors for direct non-destructive quantification of the TRU content of these RH-TRU wastes, we have designed and purchased a unique detector system using a LaBr3(Ce) primary detector and a NaI(Tl) suppression mantle. The LaBr3(Ce) primary detector is a cylindrical unit ~25 mm in diameter by 76 mm long viewed by a 38 mm diameter photomultiplier. The NaI(Tl) suppression mantle (secondary detector) is 175 mm by 175 mm with a center well that accommodates the primary detector. An important feature of this arrangement is the lack of any “can” between the primary and secondary detectors. These primary and secondary detectors are optically isolated by a thin layer (.003") of aluminized kapton, but the hermetic seal and thus the aluminum can surrounds the outer boundary of the detector system envelope. The hermetic seal at the primary detector PMT is at the PMT wall. This arrangement virtually eliminates the “dead” material between the primary and secondary detectors, a feature that preliminary modeling indicated would substantially improve the Compton suppression capability of this device. This paper presents both the expected performance of this unit determined from modeling with MCNPX, and the performance measured in our laboratory with radioactive sources

Lead Slowing-Down Spectrometry Time Spectral Analysis for Spent Fuel Assay: FY11 Status Report

Developing a method for the accurate, direct, and independent assay of the fissile isotopes in bulk materials (such as used fuel) from next-generation domestic nuclear fuel cycles is a goal of the Office of Nuclear Energy, Fuel Cycle R&D, Material Protection and Control Technology (MPACT) Campaign. To meet this goal, MPACT supports a multi-institutional collaboration, of which PNNL is a part, to study the feasibility of Lead Slowing Down Spectroscopy (LSDS). This technique is an active nondestructive assay method that has the potential to provide independent, direct measurement of Pu and U isotopic masses in used fuel with an uncertainty considerably lower than the approximately 10% typical of today's confirmatory assay methods. This document is a progress report for FY2011 PNNL analysis and algorithm development. Progress made by PNNL in FY2011 continues to indicate the promise of LSDS analysis and algorithms applied to used fuel. PNNL developed an empirical model based on calibration of the LSDS to responses generated from well-characterized used fuel. The empirical model, which accounts for self-shielding effects using empirical basis vectors calculated from the singular value decomposition (SVD) of a matrix containing the true self-shielding functions of the used fuel assembly models. The potential for the direct and independent assay of the sum of the masses of 239Pu and 241Pu to within approximately 3% over a wide used fuel parameter space was demonstrated. Also, in FY2011, PNNL continued to develop an analytical model. Such efforts included the addition of six more non-fissile absorbers in the analytical shielding function and the non-uniformity of the neutron flux across the LSDS assay chamber. A hybrid analytical-empirical approach was developed to determine the mass of total Pu (sum of the masses of 239Pu, 240Pu, and 241Pu), which is an important quantity in safeguards. Results using this hybrid method were of approximately the same accuracy as the pure empirical approach. In addition, total Pu with much better accuracy with the hybrid approach than the pure analytical approach. In FY2012, PNNL will continue efforts to optimize its empirical model and minimize its reliance on calibration data. In addition, PNNL will continue to develop an analytical model, considering effects such as neutron-scattering in the fuel and cladding, as well as neutrons streaming through gaps between fuel pins in the fuel assembly

Lead Slowing Down Spectrometer Status Report

This report documents the progress that has been completed in the first half of FY2012 in the MPACT-funded Lead Slowing Down Spectrometer project. Significant progress has been made on the algorithm development. We have an improve understanding of the experimental responses in LSDS for fuel-related material. The calibration of the ultra-depleted uranium foils was completed, but the results are inconsistent from measurement to measurement. Future work includes developing a conceptual model of an LSDS system to assay plutonium in used fuel, improving agreement between simulations and measurement, design of a thorium fission chamber, and evaluation of additional detector techniques

Lead Slowing-Down Spectrometry for Spent Fuel Assay: FY11 Status Report

Executive Summary Developing a method for the accurate, direct, and independent assay of the fissile isotopes in bulk materials (such as used fuel) from next-generation domestic nuclear fuel cycles is a goal of the Office of Nuclear Energy, Fuel Cycle R&D, Material Protection and Control Technology (MPACT) Campaign. To meet this goal, MPACT supports a multi-institutional collaboration to study the feasibility of Lead Slowing Down Spectroscopy (LSDS). This technique is an active nondestructive assay method that has the potential to provide independent, direct measurement of Pu and U isotopic masses in used fuel with an uncertainty considerably lower than the approximately 10% typical of today’s confirmatory assay methods. This document is a progress report for FY2011 collaboration activities. Progress made by the collaboration in FY2011 continues to indicate the promise of LSDS techniques applied to used fuel. PNNL developed an empirical model based on calibration of the LSDS to responses generated from well-characterized used fuel. The empirical model demonstrated the potential for the direct and independent assay of the sum of the masses of 239Pu and 241Pu to within approximately 3% over a wide used fuel parameter space. Similar results were obtained using a perturbation approach developed by LANL. Benchmark measurements have been successfully conducted at LANL and at RPI using their respective LSDS instruments. The ISU and UNLV collaborative effort is focused on the fabrication and testing of prototype fission chambers lined with ultra-depleted 238U and 232Th, and uranium deposition on a stainless steel disc using spiked U3O8 from room temperature ionic liquid was successful, with improving thickness obtained. In FY2012, the collaboration plans a broad array of activities. PNNL will focus on optimizing its empirical model and minimizing its reliance on calibration data, as well continuing efforts on developing an analytical model. Additional measurements are planned at LANL and RPI. LANL measurements will include a Pu sample, which is expected to provide more counts at longer slowing-down times to help identify discrepancies between experimental data and MCNPX simulations. RPI measurements will include the assay of an entire fresh fuel assembly for the study of self-shielding effects as well as the ability to detect diversion by detecting a missing fuel pin in the fuel assembly. The development of threshold neutron sensors will continue, and UNLV will calibrate existing ultra-depleted uranium deposits at ISU

Lead Slowing-Down Spectrometry Time Spectral Analysis for Spent Fuel Assay: FY11 Status Report

Developing a method for the accurate, direct, and independent assay of the fissile isotopes in bulk materials (such as used fuel) from next-generation domestic nuclear fuel cycles is a goal of the Office of Nuclear Energy, Fuel Cycle R&D, Material Protection and Control Technology (MPACT) Campaign. To meet this goal, MPACT supports a multi-institutional collaboration, of which PNNL is a part, to study the feasibility of Lead Slowing Down Spectroscopy (LSDS). This technique is an active nondestructive assay method that has the potential to provide independent, direct measurement of Pu and U isotopic masses in used fuel with an uncertainty considerably lower than the approximately 10% typical of today's confirmatory assay methods. This document is a progress report for FY2011 PNNL analysis and algorithm development. Progress made by PNNL in FY2011 continues to indicate the promise of LSDS analysis and algorithms applied to used fuel. PNNL developed an empirical model based on calibration of the LSDS to responses generated from well-characterized used fuel. The empirical model, which accounts for self-shielding effects using empirical basis vectors calculated from the singular value decomposition (SVD) of a matrix containing the true self-shielding functions of the used fuel assembly models. The potential for the direct and independent assay of the sum of the masses of 239Pu and 241Pu to within approximately 3% over a wide used fuel parameter space was demonstrated. Also, in FY2011, PNNL continued to develop an analytical model. Such efforts included the addition of six more non-fissile absorbers in the analytical shielding function and the non-uniformity of the neutron flux across the LSDS assay chamber. A hybrid analytical-empirical approach was developed to determine the mass of total Pu (sum of the masses of 239Pu, 240Pu, and 241Pu), which is an important quantity in safeguards. Results using this hybrid method were of approximately the same accuracy as the pure empirical approach. In addition, total Pu with much better accuracy with the hybrid approach than the pure analytical approach. In FY2012, PNNL will continue efforts to optimize its empirical model and minimize its reliance on calibration data. In addition, PNNL will continue to develop an analytical model, considering effects such as neutron-scattering in the fuel and cladding, as well as neutrons streaming through gaps between fuel pins in the fuel assembly

Lead Slowing-Down Spectrometry for Spent Fuel Assay: FY11 Status Report

Executive Summary Developing a method for the accurate, direct, and independent assay of the fissile isotopes in bulk materials (such as used fuel) from next-generation domestic nuclear fuel cycles is a goal of the Office of Nuclear Energy, Fuel Cycle R&D, Material Protection and Control Technology (MPACT) Campaign. To meet this goal, MPACT supports a multi-institutional collaboration to study the feasibility of Lead Slowing Down Spectroscopy (LSDS). This technique is an active nondestructive assay method that has the potential to provide independent, direct measurement of Pu and U isotopic masses in used fuel with an uncertainty considerably lower than the approximately 10% typical of today’s confirmatory assay methods. This document is a progress report for FY2011 collaboration activities. Progress made by the collaboration in FY2011 continues to indicate the promise of LSDS techniques applied to used fuel. PNNL developed an empirical model based on calibration of the LSDS to responses generated from well-characterized used fuel. The empirical model demonstrated the potential for the direct and independent assay of the sum of the masses of 239Pu and 241Pu to within approximately 3% over a wide used fuel parameter space. Similar results were obtained using a perturbation approach developed by LANL. Benchmark measurements have been successfully conducted at LANL and at RPI using their respective LSDS instruments. The ISU and UNLV collaborative effort is focused on the fabrication and testing of prototype fission chambers lined with ultra-depleted 238U and 232Th, and uranium deposition on a stainless steel disc using spiked U3O8 from room temperature ionic liquid was successful, with improving thickness obtained. In FY2012, the collaboration plans a broad array of activities. PNNL will focus on optimizing its empirical model and minimizing its reliance on calibration data, as well continuing efforts on developing an analytical model. Additional measurements are planned at LANL and RPI. LANL measurements will include a Pu sample, which is expected to provide more counts at longer slowing-down times to help identify discrepancies between experimental data and MCNPX simulations. RPI measurements will include the assay of an entire fresh fuel assembly for the study of self-shielding effects as well as the ability to detect diversion by detecting a missing fuel pin in the fuel assembly. The development of threshold neutron sensors will continue, and UNLV will calibrate existing ultra-depleted uranium deposits at ISU

Lead Slowing-Down Spectrometry for Spent Fuel Assay: FY12 Status Report

Executive Summary The Office of Nuclear Energy, Fuel Cycle R&D, Material Protection and Control Technology (MPACT) Campaign is supporting a multi-institutional collaboration to study the feasibility of using Lead Slowing Down Spectroscopy (LSDS) to conduct direct, independent and accurate assay of fissile isotopes in used fuel assemblies. The collaboration consists of Pacific Northwest National Laboratory (PNNL), Los Alamos National Laboratory (LANL), Rensselaer Polytechnic Institute (RPI), Idaho State University (ISU). There are three main challenges to implementing LSDS to assay used fuel assemblies. These challenges are the development of an algorithm for interpreting the data with an acceptable accuracy for the fissile masses, the development of suitable detectors for the technique, and the experimental benchmarking of the approach. This report is a summary of the progress in these areas made by the collaboration during FY2012. Significant progress was made on the project in FY2012. Extensive characterization of a “semi-empirical” algorithm was conducted. For example, we studied the impact on the accuracy of this algorithm by the minimization of the calibration set, uncertainties in the calibration masses, and by the choice of time window. Issues such a lead size, number of required neutrons, placement of the neutron source and the impact of cadmium around the detectors were also studied. In addition, new algorithms were developed that do not require the use of plutonium fission chambers. These algorithms were applied to measurement data taken by RPI and shown to determine the 235U mass within 4%. For detectors, a new concept for a fast neutron detector involving 4He recoil from neutron scattering was investigated. The detector has the potential to provide a couple of orders of magnitude more sensitivity than 238U fission chambers. Progress was also made on the more conventional approach of using 232Th fission chambers as fast neutron detectors. For benchmarking measurements, we continue to improve our understanding of the experimental setup by studying issues such as the effect of room return and impurities in the lead. RPI performed a series of experiments with a fresh fuel pin and various 235U and 239Pu sources. A comparison between simulations and measurements shows significant deviations after 200 µs for both 235U and 239Pu samples, as well as significant deviations at earlier times for the 239Pu sample. The FY2013 effort will shift focus to planning for a Technical Readiness Level 5 demonstration. The primary deliverable for the year will be a plan on how to do this demonstration. The plan will include measurement design, sample acquisition, sample handling, cost estimate, schedule and assumptions. Research will continue on the 4He detector, algorithms development, thorium fission chambers and benchmarking measurements involving sub assemblies of fresh fuel