41Ca ultratrace determination with isotopic selectivity > 1012 by diode-laser-based RIMS

Abstract

⁴¹Ca ultratrace determination by diode-laser-based resonance ionization mass spectrometry with extremely high isotopic selectivity is presented. Application to environmental dosimetry of nuclear reactor components, to cosmochemical investigations of production cross sections, and biomedical isotope-tracer studies of human calcium kinetics are discussed. Future investigations are possible use in ⁴¹Ca-radiodating. Depending on the application, ⁴¹Ca isotopic abundances in the range of 10^–9 to 10^–15 relative to the dominant stable isotope ⁴⁰Ca must be determined. Either double- or triple-resonance optical excitation with narrow-band extended cavity diode lasers and subsequent non-resonant photoionization of calcium in a collimated atomic beam were used. The resulting photoions are detected with a quadrupole mass spectrometer optimized for background reduction and neighboring mass suppression. Applying the full triple-resonance scheme provides a selectivity of ∼ 5 × 10¹² in the suppression of neighboring isotopes and > 10⁸ for isobars, together with an overall detection efficiency of ∼ 5 × 10^–5. Measurements on a variety of sample types are discussed; the accuracy and reproducibility of the resulting ⁴¹Ca/⁴⁰Ca isotope ratios was better than 5%.