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Resonance ionization mass spectrometry of ion beam sputtered neutrals for element- and isotope-selective analysis of plutonium in micro-particles

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Abstract

Micro-particles containing actinides are of interest for risk assessments of contaminated areas, nuclear forensic analyses, and IAEA as well as Euratom safeguards programs. For their analysis, secondary ion mass spectrometry (SIMS) has been established as the state-of-the-art standard technique. In the case of actinide mixtures within the particles, however, SIMS suffers from isobaric interferences (e.g., 238U/238Pu, 241Am/241Pu). This can be eliminated by applying resonance ionization mass spectrometry which is based on stepwise resonant excitation and ionization of atoms with laser light, followed by mass spectrometric detection of the produced ions, combining high elemental selectivity with the analysis of isotopic compositions. This paper describes the instrumental modifications for coupling a commercial time-of-flight (TOF)-SIMS apparatus with three-step resonant post-ionization of the sputtered neutrals using a high-repetition-rate (kHz) Nd:YAG laser pumped tunable titanium:sapphire laser system. Spatially resolved ion images obtained from actinide-containing particles in TOF-SIMS mode demonstrate the capability for isotopic and spatial resolution. Results from three-step resonant post-ionization of bulk Gd and Pu samples successfully demonstrate the high elemental selectivity of this process.

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Abbreviations

RIMS:

resonance ionization mass spectrometry

SEM:

scanning electron microscopy

SIMS:

secondary ion mass spectrometry

TOF:

time-of-flight

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Acknowledgments

The authors would like to thank Dr. M. Eriksson, IAEA-MEL, MC-98000 Monaco for providing the sediment particles associated with the Thule accident for the TOF-SIMS measurements.

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Authors and Affiliations

  1. European Commission Joint Research Centre, Institute for Transuranium Elements, P.O. Box 2340, 76125, Karlsruhe, Germany

    N. Erdmann

  2. Institute of Nuclear Chemistry, Johannes Gutenberg-University Mainz, Fritz-Strassmann-Weg 2, 55128, Mainz, Germany

    J.-V. Kratz & N. Trautmann

  3. Institute of Physics, Johannes Gutenberg-University Mainz, Staudinger Weg 7, 55128, Mainz, Germany

    G. Passler

Authors
  1. N. Erdmann
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  2. J.-V. Kratz
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  3. N. Trautmann
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  4. G. Passler
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Correspondence to N. Erdmann.

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Erdmann, N., Kratz, JV., Trautmann, N. et al. Resonance ionization mass spectrometry of ion beam sputtered neutrals for element- and isotope-selective analysis of plutonium in micro-particles. Anal Bioanal Chem 395, 1911–1918 (2009). https://doi.org/10.1007/s00216-009-2906-6

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  • DOI: https://doi.org/10.1007/s00216-009-2906-6

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