Radiogenic helium isotope fractionation: the role of tritium as 3He precursor in geochemical applications

Tolstikhin, I. N.; Lehmann, B. E.; Loosli, H. H.; Kamensky, I. L.; Nivin, V. A.; Orlov, S. P.; Ploschansky, L. M.; Tokarev, I. V.; Gannibal, M. A. (1999). Radiogenic helium isotope fractionation: the role of tritium as 3He precursor in geochemical applications. Geochimica et cosmochimica acta, 63(10), pp. 1605-1611. Elsevier Science 10.1016/S0016-7037(99)00105-2

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Reduced 4He/3He ratios, e.g., down to ≈1/100 times those expected from radiogenic production, were observed in sedimentary rocks. Formation and history of these rocks eliminate a contribution of mantle 3He-bearing fluid. To explain the difference between the observed and the calculated production 4He/3He ratios Loosli et al. (1995) and Tolstikhin et al. (1996) suggested a different behaviour of helium and tritium in damage tracks produced by emission of these nuclides. Generally, the tracks cross grain boundaries or some imperfections within a rock or mineral allowing a fast loss of noble 4He and 3He atoms. However, radiogenic 3He has the precursor 3H, generated in the exothermic 6Li(nt, α)3H + 4.5 MeV reaction. The energetic tritons produce damage tracks comparable with those from α-decay of U and Th series. If 3H is chemically bound within a track, and the track is able to recover via some diagenetic process before the 3H decay, then 3H and daughter 3He atoms are trapped within the recovered track. This mechanism would explain the shorter residence time of 4He in the rocks/minerals than of 3He; therefore, 4He/3He ratios could decrease through time.

To check this mechanism 4He, 3H, and 3He (from 3H-decay) were produced by the above reaction in special targets, consisting of layered composites of thin sections of quartz, sample, Li-bearing cover, sample, and quartz. The samples were the same rocks in which reduced 4He/3He ratios have been previously observed. Each target was placed in a quartz ampoule, which was then pumped out, sealed off, and then exposed to the flux of thermal neutrons in a reactor. After irradiation and cooling down (total duration 145 days), the nuclides produced during (3H, 3He, 4He) and after (3He) irradiation were measured in the gas phase above the targets and compared with their total quantities expected from the Li abundance and the integrated neutron flux. The ratios obtained were 3H(gas)/3H(total) < 0.05 and 3He(gas)/3He(total) varying from 0.2 to 0.9. The average residence times τ of 3H and 3He, respectively, were estimated to be ≈16 and ≈0.25 yr for this first time interval, which included the irradiation of the targets.

After these first measurements, the targets were kept in a vacuum system under room temperature for 210 days and the amounts of 3H and 3He, which accumulated above the targets during this second time interval under fully controlled conditions, were also measured. Much slower rates of gas loss from the same targets with average residence times of τ(3H) ≈ 600 yr and τ(He) ≈ 1.6 yr resulted for this second time interval. Probably these longer residence times are closer to those in the relevant natural environments, the 3H residence time being much longer than the 3H half-life.

In all cases the inequality τ(3He) ≪ τ(3H) is valid. This confirms the proposed scenario envisaging longer retention of 3H than He in damage tracks. Within the frame of this scenario the life-time of 3H gives a time constraint on diagenetic processes; at least one to several newly formed atomic layers should appear during ∼10 yr to recover the tracks.

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