The isotopic composition of plutonium and uranium is needed for purposes of sample confirmation, or for interpreting results from calorimeters or neutron-coincidence measurement instruments to determine nuclear material mass. The authors have developed measurement methods and computer codes utilizing high-resolution gamma-ray spectrometry to measure the relative isotopic abundances of plutonium and uranium in various forms nondestructively. The computer codes, known as MGA and MGAU, have unique analysis methodologies that the authors briefly describe in this paper.

We discuss the general approach, computerized data analysis methods, and results of measurements used to determine the isotopic composition of plutonium by gamma-ray spectroscopy. The simple techniques are designed to be applicable to samples of arbitrary size, geometry, age, chemical, and isotopic composition. The combination of the gamma spectroscopic measurement of isotopic composition coupled with calorimetric measurement of total sample power is shown to give a totally nondestructive determination of sample plutonium mass with a precision of 0.6% for 1000-g samples of PuO2 with 12% 24°Pu content. The precision of isotopic measurements depends upon many factors, including sample size, sample geometry, and isotopic content. Typical ranges are found to be 238Pu, 1 to 10%; 239Pu, 0.1 to 0.5%; 24°Pu, 2 to 5%; 241Pu, 0.3 to 0.7%; 242Pu (determined by isotopic correlation); and 241Am, 0.2 to 10%.

A nondestructive gamma-ray technique has been developed to determine plutonium isotopic ratios. The technique is based on the high-intensity, low-energy gamma rays at 43.48, 45.23, 51.63, 59.54, and 64.83 keV for 238Pu, 24°Pu, 239Pu, 241Am, and 241Pu, respectively. The results demonstrate that this technique can accurately measure plutonium samples in a timely manner and in a wide range of masses, isotopic contents, chemical forms, and ages from chemical processing.

MGA calculates relative isotopic abundances of plutonium and other actinides in a sample. The code performs its analysis using data from a gamma-ray spectrum of the sample taken with a germanium detector. This volume describes the structure of the program and the procedures used for measuring samples and analyzing the spectra. It is assumed that the user is familiar with standard practices and equipment used in gamma-ray spectrometry.