Isotopic measurements of items stored in shielded shipping containers presents a challenge to standard, nondestructive high-resolution gamma spectroscopy analysis. For example, some plutonium oxide material that will be shipped from Rocky Flats will be packaged in a combination of containers that places more than 12 mm of lead and 25 mm of steel between the material and the detector. This shielding effectively eliminates gamma rays below approximately 300 keV. Spectra were taken through simulated containers and analyzed using FRAM version 4.0 and a parameter set developed for use with highly attenuated items. The results indicate that 10% precision in measured 24°Pu content should be achievable with 2-hour measurements.

The goal of this work was to determine the effects on plutonium isotopic analysis of having plutonium inside of a 0.25 inch thick stainless steel can. To do this, they analyzed plutonium samples with a U-Pu InSpector (which uses a high-resolution gamma-ray detector and the analysis code MGA (Multi Group Analysis)), to determine both the 240-Pu/239-Pu ratio and the years since the plutonium was separated from americium. They analyzed a 1.6 kg plutonium sample that was placed inside of a 0.25 inch can at varying distances (0-2 meters) and count times (10 seconds-30 minutes). In separate experiments, they analyzed 0.4g plutonium sources with stainless-steel thickness' ranging from 0.125 to 1.0 inch. This report will show three effects of having plutonium in a stainless steel can: (1) 240-Pu/240-Pu can be quickly and accurately determined for a 1.6 kg plutonium sample inside of a 0.25 inch thick stainless-steel can, as this thickness of stainless steel acts as a perfect filter to reduce the intense 59 keV gamma peak from 241-Am. (2) The accuracy of determining the plutonium-americium separation date is not effected by 0.25 inch of stainless steel. (3) Both 240-Pu/239-Pu and the americium separation date can be accurately determined for stainless-steel thickness' up to 0.5 inches, requiring additional counting time with increasing thickness to obtain desired precision. For stainless-steel absorber thickness' greater than 0.5 inch, MGA analyses are not reliable.

The Lawrence Livermore National Laboratory develops sophisticated gamma-ray analysis codes for isotopic determinations of nuclear materials based on the principles of the MultiGroup Analysis (MGA). MGA methodology has been upgraded and expanded and is now comprised of a suite of codes known as MGA++. A graphical user interface has also been developed for viewing the data and the fitting procedure. The code suite provides plutonium and uranium isotopic analysis for data collected with high-purity germanium planar and/or coaxial detector systems. The most recent addition to the MGA++ code suite, MGAHI, analyzes Pu data using higher-energy gamma rays (200 keV and higher) and is particularly useful for Pu samples that are enclosed in thick-walled containers. Additionally, the code suite can perform isotopic analysis of uranium spectra collected with cadmium-zinc-telluride (CZT) detectors. We are currently developing new codes with will integrate into the MGA++ suite. These will include Pu isotopic analysis capabilities for data collected with CZT detectors, and U isotopic analysis with high-purity germanium detectors, which utilizes only higher energy gamma rays. Future development of MGA++ will include a capability for isotopic analyses on mixtures of Pu and U.

Nondestructive assay (NDA) measurements of Transuranic (TRU) waste at Los Alamos National Laboratory (LANL) packed in Pipe-over-Pack Containers (POC) contain a number of complexities. The POC is highly attenuating to both gamma rays and neutrons which presents a difficult waste matrix for correct quantification of material in the container. Currently there are a number ofPOC containers at LANL that require evaluation for shipment to the Waste Isolation Pilot Plant (WIPP) in Carlsbad, NM. Updated data has been evaluated that finalizes the evaluation of characterizing Pipe-Over-Pack Containers. Currently at LANL, a single instrument has been used to explore the appropriateness of both passive neutron and quantitative gamma ray methods for measuring POC's. The passive neutron approach uses the Reals coincidence count rate to establish plutonium mass and other parameters of interest for TRU waste. The quantitative gamma ray method assumes a homogeneous distribution of radioactive source material with the surrounding material throughout the drum volume. Drums are assayed with a calibration based on the known density of the matrix. Both methods are supplemented by a simultaneous isotopic measurement using Multi-Group Analysis (MGA) to determine the plutonium isotopic composition. If MGA fails to provide a viable isotopic result Fixed Energy Response function Analysis with Multiple efficiencies (FRAM) has been used to replace the MGA results. Acceptable Knowledge (AK) may also be used in certain instances. This report will discuss the two methods in detail. Included in the discussion will be descriptions of the setup parameters and calibration techniques for the instrument. A number of test measurements have been performed to compare HENC data with certified historical data. Empty POCs loaded with known sources have also been measured to determine the viability of the technique. A comparison between calorimetry data, historical measurements and HENC data will also be performed. The conclusion will show that the current calibration on the HENC units is viable for analysis of POCs.

We describe the new capability of and.present measurement results from the PC/FRAM plutonium isotopic analysis code. This new code allows data acquisition from a single coaxial germanium detector and analysis over an energy range from 120 keV to above I MeV. For the first time we demonstrate a complete isotopic analysis using only gamma rays greater than 200 keV in energy. This new capability allows the measurement of the plutonium isotopic composition of items inside shielded or heavy-walled containers without having to remove the items from the container. This greatly enhances worker safety by reducing handling and the resultant radiation exposure. Another application allows international inspectors to verify the contents of items inside sealed, long-term storage containers that may not be opened for national security or treaty compliance reasons. We present measurement results for traditional planar germanium detectors as well as coaxial detectors measuring shielded and unshielded samples.

The nondestructive assay of plutonium is important as a safeguard tool in accounting for stategic nuclear material. Several nondestructive assay techniques, e.g., calorimetry and spontaneous fission assay detectors, require a knowledge of plutonium and americium isotopic ratios to convert their raw data to total grams of plutonium. This paper describes a nondestructive technique for calculating plutonium-238, plutonium-240, plutonium-241 and americium-241 relative to plutonium-239 from measured peak areas in the high resolution gamma-ray spectra of solid plutonium samples. Gamma-ray attenuation effects have been minimized by selecting sets of neighboring peaks in the spectrum whose components are due to the different isotopes. Since the detector efficiencies are approximately the same for adjacent peaks, the accuracy of the isotopic ratios are dependent on the half-lives, branching intensities and measured peak areas. The data presented describes the results obtained by analyzing gamma-ray spectra in the energy region from 120 to 700 keV. The majority of the data analyzed was obtained from plutonium material containing 6% plutonium-240. Sample weights varied from 0.25 g to approximately 1.2 kg. The methods have also been applied to plutonium samples containing up to 23% plutonium-240 with weights of 0.25 to 200g. Results obtained by gamma-ray spectroscopy are compared to chemical analyses of aliquots taken from the bulk samples.