4.4 Article

Direct uranium isotope ratio analysis of single micrometer-sized glass particles

Journal

JOURNAL OF ENVIRONMENTAL RADIOACTIVITY
Volume 113, Issue -, Pages 8-15

Publisher

ELSEVIER SCI LTD
DOI: 10.1016/j.jenvrad.2012.03.017

Keywords

Laser ablation; Multi collector ICP-MS; Uranium isotope ratio analysis; Particle analysis; Nuclear forensics; Nuclear safeguards

Funding

  1. Austrian Science Fund FWF (START project) [267-N11]
  2. International Atomic Energy Agency

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We present the application of nanosecond laser ablation (LA) coupled to a 'Nu Plasma HR' multi collector inductively coupled plasma mass spectrometer (MC-ICP-MS) for the direct analysis of U isotope ratios in single, 10-20 mu m-sized, U-doped glass particles. Method development included studies with respect to (1) external correction of the measured U isotope ratios in glass particles, (2) the applied laser ablation carrier gas (i.e. Ar versus He) and (3) the accurate determination of lower abundant U-236/U-238 isotope ratios (i.e. 10(-5)). In addition, a data processing procedure was developed for evaluation of transient signals, which is of potential use for routine application of the developed method. We demonstrate that the developed method is reliable and well suited for determining U isotope ratios of individual particles. Analyses of twenty-eight Si glass particles, measured under optimized conditions, yielded average biases of less than 0.6% from the certified values for U-234/U-238 and U-235/U-238 ratios. Experimental results obtained for U-236/U-238 isotope ratios deviated by less than -2.5% from the certified values. Expanded relative total combined standard uncertainties U-c (k = 2) of 2.6%, 1.4% and 5.8% were calculated for U-234/U-238, U-235/U-238 and U-236/U-238, respectively. (c) 2012 Elsevier Ltd. All rights reserved.

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