Simultaneous determination of picogram per gram concentrations of Ba, Pb and Pb isotopes in Greenland ice by thermal ionisation mass spectrometry

Abstract

A technique has been developed to simultaneously measure picogram per gram concentrations of Ba and Pb by isotope dilution mass spectrometry, as well as Pb isotopic ratios in polar ice by thermal ionisation mass spectrometry. \( {\text{BaPO}}^{ + }_{{\text{2}}} \) and Pb+ ions were employed for these determinations. A calibrated mixture of enriched 205Pb and 137Ba was added to the samples providing an accuracy of better than approximately 2% for Pb/Ba element ratio determinations. Interference by molecular ions in the Pb mass spectrum occurred only at 204Pb and 205Pb, but these contributions were negligible in terms of precisions expected on picogram-sized Pb samples. The technique is illustrated with measurements on Greenland firn, using a drill-core section that includes the Laki volcanic eruption of 1783–1784. The data show deviations from the element concentrations indicating volatile metal enrichments, but the Pb isotopic signature of the Laki lava could not be identified.

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

Fig. 1
Fig. 2

References

  1. 1.

    Murozumi M, Chow TJ, Patterson CC (1969) Geochim Cosmochim Acta 33:1247–1294

    Article  CAS  Google Scholar 

  2. 2.

    Boutron CF, Gorlack U, Candelone J-P, Bolshov MA, Delmas RJ (1991) Nature 353:153–156

    Google Scholar 

  3. 3.

    Candelone J-P, Hong S, Pellone C, Boutron CF (1995) J Geophys Res 100:16605–16616

    Article  CAS  Google Scholar 

  4. 4.

    Hong S, Candelone J-P, Boutron CF (1996) Earth Planet Sci Lett 144:605–610

    Article  CAS  Google Scholar 

  5. 5.

    Chisholm W, Rosman KJR, Boutron CF, Candelone J-P, Hong S (1995) Anal Chim Acta 311:141–151

    Article  CAS  Google Scholar 

  6. 6.

    Sturges WT, Barrie LA (1987) Nature 329:144–146

    Article  CAS  Google Scholar 

  7. 7.

    Rosman KJR, Chisholm W, Boutron CF, Candelone J-P, Gorlach U (1993) Nature 362:333–334

    Article  CAS  Google Scholar 

  8. 8.

    Rosman KJR, Chisholm W, Hong S, Candelone JP, Boutron CF (1997) Environ Sci Technol 31:3413–3416

    Article  CAS  Google Scholar 

  9. 9.

    Alleman LY, Veron AJ, Church TM, Flegal AR, Hamelin B (1999) Geophys Res Lett 26:1477–1480

    Article  CAS  Google Scholar 

  10. 10.

    Bollhoefer A, Rosman KJR (2001) Geochim Cosmochim Acta 65:1727–1740

    Article  Google Scholar 

  11. 11.

    Heumann KG (1992) Rev Mass Spectrom 11:41–67

    Article  CAS  Google Scholar 

  12. 12.

    Burton GR, Morgan VI, Boutron CF, Rosman KJR (2002) Anal Chim Acta 469:225–233

    Article  CAS  Google Scholar 

  13. 13.

    Candelone J-P, Hong S, Boutron CF (1994) Anal Chim Acta 299:9–16

    Article  CAS  Google Scholar 

  14. 14.

    Heumann KG (1988) Isotope dilution mass spectrometry. In Adams F, Gijbels R, Van Grieken R (eds) Inorganic mass spectrometry. Wiley, New York

    Google Scholar 

  15. 15.

    Li C-F, Chena F, Li X-H (2007) Int J Mass Spectrom (in press)

  16. 16.

    Rosman KJR, Loss RD, de Laeter JR (1984) Int J Mass Spectrom Ion Phys 56:218–291

    Google Scholar 

  17. 17.

    Cameron AE, Smith DH, Walker RL (1969) Anal Chem 41:525–526

    Article  CAS  Google Scholar 

  18. 18.

    Patterson CC, Settle DM (1987) Geochimi Cosmochim Acta 51:675–681

    Article  CAS  Google Scholar 

  19. 19.

    Vallelonga P, Van de Velde K, Candelone JP, Ly C, Rosman KJR, Boutron CF, Morgan VI, Mackey DJ (2002) Anal Chim Acta 453:1–12

    Article  CAS  Google Scholar 

  20. 20.

    McLennan SM (2001) Geochem Geophys Geosystems, paper number 2000GC000109

  21. 21.

    Webster RK (1960) ’Mass spectrometric isotopic dilution analysis. In Smales AA, Wager LR (eds) Methods in geochemistry. Interscience, New York, pp 202–246

    Google Scholar 

  22. 22.

    Eugster O, Tera F, Wasserburg GJ (1969) J Geophys Res 74:3897–3908

    Article  CAS  Google Scholar 

  23. 23.

    Bohlke JK, de Laeter JR, De Bievre P, Hidaka H, Peiser HS, Rosman KJR, Taylor PDP (1998) J Phys Chem Ref Data 34:57–67

    Article  Google Scholar 

  24. 24.

    Zindler A, Jagoutz E, Goldstein S (1982) Nature 298:519–523

    Article  CAS  Google Scholar 

  25. 25.

    Bollhoefer A, Rosman KJR (2002) Geochim Cosmochim Acta 66:1375–1386

    Article  Google Scholar 

  26. 26.

    Sun SS, Tatsumoto M, Schilling JG (1975) Science 190:143–147

    CAS  Google Scholar 

  27. 27.

    Sun SS, Jahn BM (1975) Nature 255:527–530

    Article  CAS  Google Scholar 

  28. 28.

    Vallelonga P, Candelone J-P, Van de Velde K, Curran MAJ, Morgan VI, Rosman KJR (2003) Earth Planet Sci Lett 211:329–341

    Article  CAS  Google Scholar 

Download references

Acknowledgments

We thank staff and students of Curtin University’s Isotope Science Research Laboratories who provided valuable discussion. We thank Dr Haukur Johannesson who provided the solidified lava from the Laki site. This laboratory is supported by research grants from the Australian Research Council and the Antarctic Science Advisory Committee. The collection and decontamination of the samples in Greenland was supported by the Commission of the European Communities and Switzerland, and the French Ministry of the Environment. We also thank three reviewers for helpful advice on improving the manuscript.

Author information

Affiliations

Authors

Corresponding author

Correspondence to Kevin J. R. Rosman.

Rights and permissions

Reprints and Permissions

About this article

Cite this article

Jimi, S.I., Rosman, K.J.R., Hong, S. et al. Simultaneous determination of picogram per gram concentrations of Ba, Pb and Pb isotopes in Greenland ice by thermal ionisation mass spectrometry. Anal Bioanal Chem 390, 495–501 (2008). https://doi.org/10.1007/s00216-007-1729-6

Download citation

Keywords

  • TIMS
  • Barium
  • Lead isotopes
  • Ice cores
  • Laki
  • Volcanoes