Skip to main content
SpringerLink
Log in

The use of LA-SF-ICP-MS for nuclear forensics purposes: uranium isotope ratio analysis

  • Published:
Journal of Radioanalytical and Nuclear Chemistry Aims and scope Submit manuscript

Abstract

This work describes the utilization of the laser ablation sector field inductively coupled plasma mass spectrometry (LA-SF-ICP-MS) technique for the determination of uranium isotopic composition in a highly enriched uranium sample. The measurements were performed on a continuous ablation with low energy density and defocusing, which demonstrated to be the optimum to reach the best signal stability. The measurements were improved by adjusting the following parameters: RF power, laser beam diameter, defocusing of laser beam, laser energy, laser energy density, auxiliary gas and sample gas. The 235U/238U isotope ratio with its respective uncertainty was 16.36 ± 0.15 and its precision was 1.12 % relative standard deviation. The uncertainties were estimated following the ISO GUM, with a confidence level of 95.45 % (k = 2.00). When compared the isotope abundances to the Round Robin Exercise Number 3’s average results a difference of 0.46 % has been found and when compared to supplier’s value, the difference was 0.41 %. The results presented by the measurements revealed that the LA-ICP-MS technique offers a rapid and accurate alternative to measure uranium isotope ratios without any sample preparation, since it allows carrying out the measurements straight on the sample. Moreover, it preserves the testimony—very important for safeguards and nuclear forensics purposes.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1

Similar content being viewed by others

References

  1. Mayer K, Wallenius M, Ray I (2005) Nuclear forensics—a methodology providing clues on the origin of illicitly trafficked nuclear materials. Analyst 130:433–441

    Article  CAS  Google Scholar 

  2. Buchmann JH, Sarkis JES, Kakazu MH, Rodrigues C (2006) Environmental monitoring as an important tool for safeguards of nuclear material and nuclear forensics. J Radioanal Nucl Chem 270:291–298

    Article  CAS  Google Scholar 

  3. Marin RC, Sarkis JES (2011) Isotope ratio measurements of uranium by LA-HR-ICP-MS. In: INAC

  4. Furusawa HA, Sarkis JES, Kakazu MH, Rodrigues C (1999) Uranium isotopic analysis by using a Sector Field Inductively Coupled Plasma Mass Spectrometer. J Radioanal Nucl Chem 242:647–651

    Article  CAS  Google Scholar 

  5. Oliveira OP Jr, De Bolle W, Alonso A, Richter S, Wellum R, Ponzevera E, Sarkis JES, Kessel R (2010) Demonstrating the metrological compatibility of uranium isotope amount ratio measurement results obtained by GSMS, TIMS and MC-ICPMS techniques. Int J Mass Spectrom 291:48–54

    Article  Google Scholar 

  6. Pickhardt C, Dietze H-J, Sabine Becker J (2005) Laser ablation inductively coupled plasma mass spectrometry for direct isotope ratio measurements on solid samples. Int J Mass Spectrom 242:273–280

    Article  CAS  Google Scholar 

  7. Varga Z (2008) Application of laser ablation inductively coupled plasma mass spectrometry for the isotope analysis of single uranium particles. Anal Chim Acta 625:1–7

    Article  CAS  Google Scholar 

  8. Boulyga SF, Becker JS (2001) Determination of uranium isotopic composition and 236U content of soil samples and hot particles using inductively coupled plasma mass spectrometry. Fresenius J Anal Chem 370:612–617

    Article  CAS  Google Scholar 

  9. Becker JS, Dietze HJ (2000) Precise and accurate isotope ratio measurements by ICP-MS. Fresenius J Anal Chem 368:23–30

    Article  CAS  Google Scholar 

  10. Becker JS, Dietze H-J (1998) Spectrochim Acta B 53:1475

    Article  Google Scholar 

  11. Joint Committee for Guides in Metrology (2008) Evaluation of measurement data—guide to the expression of uncertainty in measurement. JCGM, Bureau International des Poids et Mesures, Sèvres Cedex, p 100

  12. Oliveira OP Jr, Sarkis JES (2002) Isotope measurements in uranium samples using a quadrupole inductively coupled plasma mass spectrometer (ICPMS). J Radioanal Nucl Chem 253:345–350

    Article  CAS  Google Scholar 

  13. Becker JS (2007) Isotope ratio measurements and their application. In: Inorganic mass spectrometry—principles and applications, 1st edn. Wiley, Chichester, p 229. ISBN 978-0-470-01200-0

  14. Bürger S et al (2010) Implementation of Guide to the expression of Uncertainty in Measurement (GUM) to multi-collector TIMS uranium isotope ratio metrology. Int J Mass Spectrom 294:65–76

    Article  Google Scholar 

  15. Hanlen R (2011) Round Robin 3 exercise after action and lessons learned report. Pacific Northwest National Laboratory (PNNL), Richmond, p 31

Download references

Author information

Authors and Affiliations

  1. Instituto de Pesquisas Energéticas e Nucleares (IPEN/CNEN-SP), Av. Professor Lineu Prestes 2242, São Paulo, SP, 05508-000, Brazil

    Rafael C. Marin & Jorge E. S. Sarkis

  2. Laboratório de Poços de Caldas (LAPOC/CNEN-MG), Rodovia Poços de Caldas/Andradas, km 13, Poços de Caldas, MG, 37701-970, Brasil

    Marcos R. L. Nascimento

Authors
  1. Rafael C. Marin
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Jorge E. S. Sarkis
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Marcos R. L. Nascimento
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Rafael C. Marin.

Rights and permissions

Reprints and permissions

About this article

Cite this article

Marin, R.C., Sarkis, J.E.S. & Nascimento, M.R.L. The use of LA-SF-ICP-MS for nuclear forensics purposes: uranium isotope ratio analysis. J Radioanal Nucl Chem 295, 99–104 (2013). https://doi.org/10.1007/s10967-012-1980-y

Download citation

  • Received:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10967-012-1980-y

Keywords

Search

Navigation