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

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          Abstract

          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 μm-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 236U/ 238U 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 S1 glass particles, measured under optimized conditions, yielded average biases of less than 0.6% from the certified values for 234U/ 238U and 235U/ 238U ratios. Experimental results obtained for 236U/ 238U 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 234U/ 238U, 235U/ 238U and 236U/ 238U, respectively.

          Highlights

          ► LA-MC-ICP-MS was fully validated for the direct analysis of individual particles. ► Traceability was established by using an IRMM glass particle reference material. ► Measured U isotope ratios were in agreement with the certified range. ► A comprehensive total combined uncertainty evaluation was performed. ► The analysis of 236U/ 238U isotope ratios was improved by using a deceleration filter.

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          Most cited references 43

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          Enhanced sensitivity in laser ablation-ICP mass spectrometry using helium-argon mixtures as aerosol carrier

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            Precision and accuracy in isotope ratio measurements by plasma source mass spectrometry

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              The influence of ablation carrier gasses Ar, He and Ne on the particle size distribution and transport efficiencies of laser ablation-induced aerosols: implications for LA–ICP–MS

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                Author and article information

                Journal
                J Environ Radioact
                J Environ Radioact
                Journal of Environmental Radioactivity
                Elsevier Applied Science Publishers
                0265-931X
                1879-1700
                November 2012
                November 2012
                : 113
                : 8
                : 8-15
                Affiliations
                [a ]University of Natural Resources and Life Sciences Vienna, Department of Chemistry, Division of Analytical Chemistry, VIRIS-Laboratory, Konrad-Lorenz-Strasse 24, 3430 Tulln, Austria
                [b ]Safeguards Analytical Services, Department of Safeguards, International Atomic Energy Agency, Wagramer Strasse 5, 1400 Vienna, Austria
                Author notes
                []Corresponding author. Tel.: +43 1 47654 6092; fax: +43 1 47654 6059. thomas.prohaska@ 123456boku.ac.at
                Article
                JENR4073
                10.1016/j.jenvrad.2012.03.017
                3440598
                22595724
                8b9d76b4-1e6c-4692-b214-ddee9ae876e9
                © 2012 Elsevier Ltd.

                This document may be redistributed and reused, subject to certain conditions.

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