Accelerator mass spectrometry of actinides

Abstract

Accelerator mass spectrometry (AMS) is a sensitive and robust technique typically applied to the quantification of long-lived radioisotopes in samples too small to be decay-counted. AMS is characterized by a high rejection of interferences and a low susceptibility to matrix components, which reduce the demands on sample preparation chemistry. At Lawrence Livermore National Laboratory (LLNL), Center for Accelerator Mass Spectrometry (CAMS), we have developed an AMS capability for the measurement of actinide concentrations and isotopic ratios. To date, this capability has been primarily devoted to the measurement of 239Pu and 240Pu in bioassay and environmental samples including soils, sediments, waters, and human urine. For these analyses, a known amount of 242Pu is added to the samples as a reference isotope for normalization. Measurements of standard and intercomparison samples have shown that quantification is accurate and precise from at least 106 to 1011 atoms/sample. Recently, the ratios of 240Pu, 241Pu, 242Pu, and +Pu to intrinsic 239Pu have been successfully measured in soil samples from nuclear test sites. In addition, initial measurements of U and Np isotopes have yielded results consistent with the Pu measurements with respect to sensitivity, accuracy, precision, and linear range.