Detection of (135) Cs by accelerator mass spectrometry.

RATIONALE: The ability to measure both (135) Cs and (137) Cs can provide an estimate of the age and source of Cs isotopes in an environmental sample. Accelerator mass spectrometry (AMS) consistently reports lower abundance sensitivities than other techniques and, with the addition of an on-line reaction cell, simpler isobaric suppression. Therefore, an AMS methodology was developed to measure Cs isotopes using CsF2- as the initial anion. METHODS: The ion beam is passed through the Isobar Separator for Anions (ISA) where it is captured by radiofrequency quadrupoles in a gas cell before injection into the tandem accelerator. In the ISA, the beam reacts with O2 gas, selectively removing the BaF2- and leaving the Cs analyte to be reaccelerated and sent through the remainder of the AMS system. RESULTS: The BaF2- signal was attenuated by a factor of 10(5) in the ISA while 25% of the original CsF2- current was transmitted into the accelerator. (135) Cs was measured without any interference from (133) Cs to an abundance sensitivity of 1.3 × 10(-10) . The abundances of four stable Ba isotopes (masses 133, 134, 135 and 137) were measured and no isotope-dependent bias was detected using the ISA in vacuum. CONCLUSIONS: The results demonstrate the feasibility of measuring long-lived Cs isotopes without Ba interference by AMS with on-line isobar separation and the ability to use shorter lived Cs isotopes for yield tracing.

On-line HfF5(-)/WF5(-) separation in an O2-filled radiofrequency quadrupole gas cell.

RATIONALE: An experimental Isobar Separator for Accelerator Mass Spectrometry (ISAMS) instrument has been used to demonstrate an on-line separation of HfF5(-) from its isobar WF5(-). This is necessary, in addition to sample preparation chemistry, for measuring (182)Hf at natural levels by Accelerator Mass Spectrometry (AMS). METHODS: The device utilizes a radiofrequency quadrupole (RFQ) controlled gas cell, wherein anion-gas reactions at eV energies attenuate the interfering isobars of the analyte molecular anions, leaving HfF5(-) for AMS analysis. The RFQ also helps to control the multiple scattering resulting from the ion-gas collisions. RESULTS: O2 gas was used in the HfF5(-)/WF5(-) separation and WF5(-) was attenuated by nearly 3 orders of magnitude while maintaining ~75% transmission of HfF5(-). It is expected that the transmission and attenuation can be increased by further research. CONCLUSIONS: This result advances the possibility of detecting natural (182)Hf when AMS is supplemented with an isobar separator in the injection system.

Mass spectrometry with accelerators.

As one in a series of articles on Canadian contributions to mass spectrometry, this review begins with an outline of the history of accelerator mass spectrometry (AMS), noting roles played by researchers at three Canadian AMS laboratories. After a description of the unique features of AMS, three examples, (14)C, (10)Be, and (129)I are given to illustrate the methods. The capabilities of mass spectrometry have been extended by the addition of atomic isobar selection, molecular isobar attenuation, further ion acceleration, followed by ion detection and ion identification at essentially zero dark current or ion flux. This has been accomplished by exploiting the techniques and accelerators of atomic and nuclear physics. In 1939, the first principles of AMS were established using a cyclotron. In 1977 the selection of isobars in the ion source was established when it was shown that the (14)N(-) ion was very unstable, or extremely difficult to create, making a tandem electrostatic accelerator highly suitable for assisting the mass spectrometric measurement of the rare long-lived radioactive isotope (14)C in the environment. This observation, together with the large attenuation of the molecular isobars (13)CH(-) and (12)CH 2(-) during tandem acceleration and the observed very low background contamination from the ion source, was found to facilitate the mass spectrometry of (14)C to at least a level of (14)C/C ~ 6 × 10(-16), the equivalent of a radiocarbon age of 60,000 years. Tandem Accelerator Mass Spectrometry, or AMS, has now made possible the accurate radiocarbon dating of milligram-sized carbon samples by ion counting as well as dating and tracing with many other long-lived radioactive isotopes such as (10)Be, (26)Al, (36)Cl, and (129)I. The difficulty of obtaining large anion currents with low electron affinities and the difficulties of isobar separation, especially for the heavier mass ions, has prompted the use of molecular anions and the search for alternative methods of isobar separation. These techniques are discussed in the latter part of the review.

Characterization of the NIST seaweed Standard Reference Material.

The National Institute of Standards and Technology (NIST) Standard Reference Material (SRM) for seaweed was developed through an interlaboratory comparison with 24 participants from 16 countries. After evaluating different techniques to calculate certified values for the radionuclides, the median method was found to be the most representative technique. The certified values were provided for 13 radionuclides and information values were given for 15 more radionuclides. Results for the natural decay series showed disequilibrium in both the uranium and thorium series.

Radiocarbon dating with electrostatic accelerators: dating of milligram samples.

The recently developed direct counting technique for radiocarbon atoms has been used to measure the relative numbers of such atoms in various geological samples which had earlier been dated by the beta-ray counting method. Sample weights ranged from 3.5 to 15 milligrams. The dates determined by the two methods are consistent with each other. Further experience with the new method is also reported.

Radiocarbon dating using electrostatic accelerators: negative ions provide the key.

Mass spectrometric methods have long been suggested as ways of measuring (14)C/(12)C ratios for carbon dating. One problem has been to distinguish between (14)N and (14)C. With negative ions and a tandem electrostatic accelerator, the (14)N background is virtually absent and fewer than three (14)C atoms in 10(16) atoms of (12)C have been easily measured.