Feasibility study for the development of plutonium reference materials for age dating in nuclear forensics

Isotopic reference materials certified for the age of nuclear material (uranium, plutonium) are needed in the fields of nuclear forensics and environmental measurements. Therefore a feasibility study for the development of plutonium reference materials for age dating has been started recently at the Institute for Reference Materials and Measurements (EC-JRC-IRMM). The "age" of the material is defined as the time that has passed since the last chemical separation of the mother and daughter isotopes (e.g. 241Pu and 241Am). Assuming that the separation has been complete and all the daughter isotopes have been removed from the original material during this last separation, the age of the material can be determined by measuring the ratio of daughter and mother radio-nuclides, e.g. 241Am/241Pu. At a given time after the last separation and depending on the half lives of the radio-nuclides involved, a certain amount of the daughter radionuclide(s) will be present. For the determination of the unknown age of a material different "clocks" can be used; "clocks" are pairs of mother and daughter radio-nuclides, such as 241Am/241Pu, 238Pu/234U, 239Pu/235U, 240Pu/236U, and possibly 242Pu/238U. For the age estimation of a real sample, such as material seized in nuclear forensics investigations or dust samples in environmental measurements, it is advisable to use more than one clock in order to ensure the reliability of the results and to exclude the possibility that the sample under question is a mixture of two or more materials. Consequently, a future reference material certified for separation date should ideally be certified for more than one "clock" or several reference materials for different "clocks" should be developed. The first step of this study is to verify the known separation dates of different plutonium materials of different ages and isotopic compositions by measuring the mother (238Pu, 239Pu, 240Pu, 241Pu, 242Pu) and daughter (234U, 235U, 236U, 238U and 241Am) isotope abundances and to estimate the achievable uncertainties of the calculated ages. Thermal ionisation mass spectrometry (TIMS) is applied for the measurement of the plutonium and uranium isotope ratios after chemical separation of the plutonium and uranium fractions from the sample matrix, while 241Am is measured by gamma-ray spectrometry. In the course of this work the reference materials NBS SRM 946, 947 and 948 (NBL CRM 136, 137 and 138) will be investigated among others.JRC.E.7-Nuclear Safeguards and Forensic