Geiger, H. U.

Tobler, L.

Wyttenbach, A.

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Radiochim. Acta 83, 127-128 (1998) © R. Oldenbourg Verlag, München 1998 108mAg in Neutron Irradiated Silver Coins By A. Wyttenbach1, L. Tobler1 and H. U. Geiger2 1 Paul Scherrer Institut, 5232 Villigen PSI, Switzerland 2 Institute of History, University of Berne, 3012 Bern, Switzerland (Received June 9, 1998; accepted in final form September 30, 1998) Silver-108m / Neutron activation analysis / Coins / Residual activity Summary Six coins, which were irradiated with neutrons 33 years ago, were investigated for their residual activity. Only traces of 108mAg could be detected. An estimation of the formation cross section of 108mAg is in accord with published values. 1. Introduction The residual activity of samples analysed by instru-mental neutron activation analysis (INAA) is usually of little importance, as most samples are discarded after the analysis. An exception is samples that are kept after analysis because of their valuable or unique nature. Archaeological objects, especially coins, be-long to this category. INAA of coins was quite popular during the 60s and 70s, as this method is not restricted to the coin surface and is nondestructive in the sense that it does not cause visible changes of the samples. Already in 1972 the number of coins analysed by INAA was estimated to be more than 5000 [1]. If the residual activity was considered at all, it was assumed to be due to UOmAg (Γ1/2 = 250 d) because most ancient coins contain Ag, and was therefore assumed to vanish completely within a few years. An experi-mental verification of this point has never been con-ducted. We lately came across some coins that were irradiated 33 years ago and determined their present residual activity. 2. Experimental and results The sample analysed in 1964 comprised about 400 coins. These were irradiated in subgroups of 30 coins on a spinning wheel in front of the nuclear reactor SAPHIR. All coins were exposed to a mean flux den-sity of 2 · 109 n/cm2s. Subgroups were formed accord-ing to the coin weight. Irradiation time of the sub-groups varied between 40 min for the heaviest and 240 min for the lightest coins, in order to keep activi-ties as small as possible [2, 3]. Analysis for the major components Cu and Ag, and for traces of Au, was done by measuring "Cu, 110mAg, and 198Au; results were reported in [4], Six of these coins were recovered in 1997 and measured 90 h each with a HPGe-detector with known counting efficiency. The only y-lines not belonging to the detector background were due to 108mAg: 433.7, 614.4 and 722.9 keV, each with 90% abundance [5]. Sample activities calculated from the three lines varied in a nonsystematic way by 2.8% (with 12 degrees of freedom); this variation is completely explained by counting statistics. Mean 108mAg activities are given in Table 1, column 4. 3. Discussion The theoretical consideration of the 108mAg residual ac-tivity in silver coins was for a long time impossible due to the lack of necessary parameters. It was later discouraged by discrepancies in published values. The half-life of 108mAg has experienced a dramatic increase with time, being ^ 5 y in 1960 [6] with no indication Table 1. Activity of 108mAg in coins' Sample number Coin weight g (1) Silver conc. % (2) Silver weight g (3) Activity of the Bq (4) coins Bq/g (5) Specific silver activity Bq/g Ag (6) 1 0.894 37.5 0.335 1.309 1.464 3.893 2 0.916 29.5 0.270 1.004 1.096 3.715 3 0.985 35.0 0.345 1.152 1.170 3.343 4 1.812 64.0 1.160 0.939 0.518 0.809 5 2.199 44.2 0.972 0.760 0.346 0.782 6 2.265 48.0 1.087 0.811 0.358 0.746 • Coins are ordered according to their weight. They contain only Ag and Cu, except ~1% of unidentified constituents. Activities have a measuring error (reproducibility) of 2%. 128 A. Wyttenbach, L. Tobler and H. U. Geiger how this value was obtained, (127±7) y in 1970 [7], and (418±15)y in 1992 [8]. A recent compilation adopts a value of (433 ±15) y [9]. The reaction cross section for t07Ag(n,y)t08mAg with thermal neutrons was given as 3 b or 10 b in 1976 [10] and determined later as 0.35 b [11], 0.37 b [12] and 0.48 b [13]. All cross section determinations were done on samples enriched in 107Ag and assuming T in = 127 y, but they are some-times erroneously combined with Tin = 418 y [14]. The specific Ag activities in Table 1, column 6 show a decrease with increasing sample weight, as might be expected from the irradiation protocol. The allocation of the individual coins to the subgroups is no longer available. Assuming an irradiation time of 240 min for coin # 1 and of 40 min for coin # 6 leads to identical reaction cross sections of 1.0 b (with Tu2 = 433 y) or of 0.36 b (with Tin = 127 y), which is in good agreement with the values quoted above. The activities reported in Table 1 are all well be-low the exemption limit set by legislation for 108mAg [15], meaning that there are no legal restrictions as to the storage or the exhibition of these coins. Indeed, their activity is roughly equal to the naturally occur-ring "°K activity in a glass object of equal weight, for which no objections to display are met. 4. Conclusions The only residual activity found in Cu-Ag coins 33 years after their irradiation with neutrons is 108mAg. Albeit the activity is very small and below the legal exemption limit, its Tin is very long, even on the time scale relevant to museums. It is therefore questionable if INAA of coins is as nondestructive as one might wish. In any case it seems reasonable to restrict the applied neutron dose to an absolute minimum when investigating coins by INAA. References 1. Meyers, P.: Activation Analysis Methods Applied to Coins, a Review. In: Methods of Chemical and Metallurgical In-vestigation of Ancient Coinage (Ε. T. Hall, D. M. Metcalf, eds.). Royal Num. Soc. Spec. Publ. No. 8, London (1972). 2. Wyttenbach, Α., Hermann, H.: Archaeometry 9,139 (1966). 3. Wyttenbach, Α.: Helv. Chim. Acta 49, 2555 (1966). 4. Geiger, Η. U.: Der Beginn der Gold- und Dickmünzen-prägung in Bern. Thesis, University of Berne 1968, p. 217. 5. Erdtmann, G., Soyka, W.: The Gamma Rays of the Radio-nuclides, Verlag Chemie, Weinheim (1979), p. 862. 6. Wahlgren, Μ. Α., Meinke, W. H.: Phys. Rev. 118, 181 (1960). 7. Harbottle, G.: Radiochim. Acta 13, 132 (1970). 8. Schötzig, U., Schräder, H., Debertin, K.: Precision Measure-ments of Radioactive Decay Data. In: Nuclear Data for Sci-ence and Technology (S. M. Qaim, ed.). Springer, Berlin (1992), p. 562. 9. INDC Report: Activation Cross Sections for the Generation of Long-Lived Radionuclides of Importance in Fusion Reac-tor Technology (A. B. Pashchenko, ed.). INDC (NDS)-344, IAEA, Vienna 1997. 10. Erdtmann, G.: Neutron Activation Tables, Verlag Chemie, Weinheim (1976), p. 146. 11. Rao, D. V., Govelitz, G. F., Mallams, J. T.: Int. J. Appl. Rad. Isotopes 29, 405 (1978). 12. Ryves, Τ. B.: Nucl. Sei. Eng. 72, 357 (1979). 13. Gavrilas, M„ Guinn, V. P.: J. Radioanal. Nucl. Chem. 113, 327 (1987). 14. Pfennig, G., Klewe-Nebenius, H., Seelmann-Eggebert, W: Karlsruher Nuklidkarte, 6* edition, Forschungszentrum Karlsruhe 1995. 15. Swiss Federal Council: Radiological Protection Ordinance, 22 June 1994. 

108mAg in Neutron Irradiated Silver Coins

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