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Title: Measurement of high-dynamic-range thorium isotopic ratios using continuous-wave resonance ionization mass spectrometry

Journal Article · · Analytical Chemistry (Washington); (United States)
DOI:https://doi.org/10.1021/ac00080a014· OSTI ID:7267689
 [1]; ;  [2]
  1. Virginia Polytechnic Inst. and State Univ., Blacksburg, VA (United States)
  2. Los Alamos National Lab., NM (United States)

We have developed continuous-wave resonance ionization mass spectrometry (cw-RIMS) methods to measure [sup 230]Th/[sup 232]Th isotopic ratios. The overall Th ionization detection efficiency using a 1 + 1 RIMS process (narrow-band laser for the resonant step and a high-power ultraviolet- (UV-) Ar[sup +] laser for the ionization step) is 0.10%. Measurement of the [sup 230]Th/[sup 232]Th ratio (4.096 x 10[sup [minus]4]) of a laboratory standard shows that the cw-RIMS method has internal precision comparable to thermal ionization mass spectrometry measurements ([approximately] 0.5%, 2[sigma][sub m]), but introduces a small bias (2-4%), which is correctable by calibration with an isotopic standard. The bias is due to intrinsic laser-induced biases in the 1 + 1 RIMS process and in a nonresonant process due to the UV-Ar[sup +] laser alone, which contributes approximately 3% to the total Th[sup +] signal. Laser power dependence experiments show that neither the resonant nor the ionization step is entirely saturated; therefore, the isotopic bias is probably due to differences in the transition strengths of the isotopes. The reproducibility of the RIMS-induced bias is dependent on the reproducibility of the laser parameters, but can be kept within the precision of the measurements ([approximately] 0.5%). Ratio measurements of the 4.096 x 10[sup [minus]4] standard and of a sample of Table Mountain Latite demonstrates that cw-RIMS can accurately measure [sup 230]Th/[sup 232]Th ratios when the laser-induced biases are calibrated and kept constant. 41 refs.., 8 figs., 3 tabs.

DOE Contract Number:
W-7405-ENG-36
OSTI ID:
7267689
Journal Information:
Analytical Chemistry (Washington); (United States), Vol. 66:8; ISSN 0003-2700
Country of Publication:
United States
Language:
English