Improved limit on the electron capture decay branch of 176Lu

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Abstract

We have performed searches for the electron-capture decay branches of 176Lu to the ground state and first excited state of 176Yb. No evidence of either decay mode was observed. From these measurements we have established upper limits on both of these possible branches that are each >20 times more stringent than the single previously published limit.

Introduction

The long-lived naturally occurring nuclide 176Lu (Jπ=7) β decays to levels in 176Hf. This decay is the basis for a dating method increasingly applied to rocks and meteorites. The utility of this dating method has been hampered by uncertainty in the half-life, as recently reviewed by Begemann et al. (2001). To some extent the half-life estimates vary systematically according to the approach used for its determination, with the lowest values (3.50–3.57)×1010 years, implied from mass spectrometric measurements of Lu- correlated 176Hf excesses in meteorites whose ages were independently known (Patchett and Tatsumoto, 1980; Blichert-Toft et al., 2002; Bizzarro et al., 2003). A half-life value of (3.73±0.02)×1010 years obtained from the direct counting experiment of Nir-El and Lavi (1998) agrees with the (3.72±0.03)×1010 years value determined by Scherer et al. (2001) through age comparisons for terrestrial rocks. However, Browne and Junde (1998) evaluated the results of a large number of direct counting measurements and recommended a higher value of (4.00±0.22)×1010 years. Moreover, the recent and precise γ–γ coincidence measurement of the 176Lu half-life of (4.08±0.03)×1010 years by Grinyer et al. (2003), which agrees very well with the earlier direct γ-ray counting results of (4.08±0.24)×1010 years by Norman (1980) and (4.05±0.09)×1010 years by Gehrke et al. (1990), reaffirms a systematic difference of order 15% in the half-life deduced from these two approaches, which must be resolved before the 176Lu-176Hf method can be established as a reliable geo- and cosmo-chronometer.

It has been suggested that the discrepancies involving age comparisons could be reconciled if 176Lu also underwent significant electron capture decay. 176Lu is unstable with respect to electron-capture decay to 176Yb. The QEC for decay to the 176Yb ground state is 106.2 keV (Firestone, 1996). Thus, EC decays to both the Jπ=0+ ground state and Jπ=2+ 82-keV first excited state of 176Yb are possible. These EC decay branches would be 7th and 5th forbidden transitions, respectively, and thus are expected to be negligibly small. In fact, there are no observed cases of such highly forbidden transitions (Singh et al., 1998). The decay scheme of 176Lu is illustrated in Fig. 1. The published limit on the EC decay branch of 176Lu of < 10% was reported by Arnold (1954) in his study of the decay of 176Lu. This upper limit was deduced from a search for Yb K X-rays that would be produced by the EC decay of 176Lu. Because of the recent inconsistencies encountered in using the 176Lu/176Hf chronometer, it was felt that a new search for the EC decay of 176Lu was warranted.

Section snippets

Experimental

Two plastic bottles, each containing 5 g of 99.9% pure LuCl3·6H2O purchased from Alfa-Aesar were placed against the plastic endcap of a 110 cm3 high-purity germanium detector. X- and γ-ray data from approximately 20–800 keV were acquired in 4096 channels for a period of 65 h using an ORTEC PC-based acquisition system. The energy resolution of this system was measured to be 1.4 keV full-width at half-maximum at 88 keV. Portions of the spectrum obtained from the Lu sample are shown in Fig. 2, Fig. 3.

Results

As can be seen from the decay scheme shown in Fig. 1, all of the beta decays of 176Lu eventually produce γ-ray transitions through the 88-keV level in 176Hf. Thus, in order to establish a limit on the EC decay branch to the 82-keV level in 176Yb, we determined both the net area of the 88-keV peak and the gross area of an equal width energy interval centered on 82 keV in the spectrum obtained from the Lutetium chloride sample. The net area of the 88-keV peak was determined to be N88=79111±534 

Conclusion

As expected, no evidence for the EC decay of 176Lu to either the ground state or first excited state of 176Yb was observed. The upper limits we have been able to establish on these possible EC transitions are each >20 more stringent than the single previously published limit of <10% for the EC decay of 176Lu. Our results are also about a factor of two more stringent than that recently obtained from a mass spectrometric search for excess 176Yb in (1.0–2.7)×109 year-old Lu-bearing samples (Amelin

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