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Application of resonance ionisation mass spectrometry for the determination of trace amounts of transuranium elements in environmental samples

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Leistungen

The goal of this project was the determination of transuranium elements in various environmental samples from the Ukraine and other regions by means of Resonance Ionisation Mass Spectrometry (RIMS). For this efficient RIMS facilities had to be built up in Kiev based on the experience in Mainz. Cross checks with respect to accuracy and reproducibility of the method should be performed by the participants in Leeuwarden, Sevilla and Mainz. In Kiev an improved RIMS set-up with laser ablation of the samples was designed constructed and applied for trace analysis. In tests with various model elements the optimal conditions for the ablation step including sample preparation and for the RIMS facility were explored. Furthermore, two environmental samples were calibrated by alpha-spectroscopy and Pu-containing samples measured by means of RIMS under optimised conditions (Institute for Nuclear Research). At the Institute of Physics the RIMS facility consisting of a Nd:YAG pump laser and three dye-lasers was modernised, a laser wavelength meter was built, radiochemical procedures for the separation of Pu from environmental samples have been worked out and the RIMS technique applied for the determination of actinide elements in the environment yielding a sensitivity of better than 0.5 x 10-8 ion/atom. A computer program for the calculation of the ion yield was developed and used to study the influence of different parameters and to optimise the performance of RIMS. In Troitsk a new laser wavelength meter (LambdaMeter) was designed and constructed with a zerodur glass optical arrangement and an active temperature stabilisation. A slit spatial filter enables a high sensitivity. The LambdaMeter is equipped with new spectrum acquisition electronics and has in the operation range 300 - 1060 nm a resolution of 0.0005 nm and a time drift SUP>6 atoms of Pu has been achieved with RIMS. Different soil samples from the Chernobyl area and from the Mururoa Atoll as well as urine have been investigated with respect to their isotopic composition and the total amount of plutonium. Intercalibration measurements of two soil samples by alpha-spectroscopy and with the RIMS method were done enabling the determination of the total amount of different Pu-isotopes and the isotopic ratio. Furthermore, help and advice were given to the partners in Kiev in connection with the construction of a time-of-flight mass spectrometer and data acquisition systems as well as in chemical separation procedures.

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