Decay data evaluation of Radium – 226 and its daughters V. Chisté, M. M. Bé, C. Dulieu Laboratoire National Henri Becquerel 1 Introduction * Important naturally occurring radioactive chain: 1 – calibration of gamma-ray detectors 2 – environmental controls * Ra-226 chain is included in the Coordinated Research Program – IAEA Laboratoire National Henri Becquerel 2 Ra-226 1600 (7) a a Ra-226 radioactive chain 100 % Rn-222 a 100 % b b Po-218 0.022 At-218 0.1 % % a 100 % a 99.9 % Rn-218 T1/2 = 36.0 (19) ms Pb-214 Po-214 T1/2 = 162.3 (12) ms - b- 100 % - Bi-214 a b- 99.98 % 0.02 % Tl-210 b- a a 100 % T1/2 = 22.23 (12) a 100 % Pb-210 b - a Hg-206 Bi-210 b- a b- Tl-206 Po-210 a b- Pb-206 Stable Laboratoire National Henri Becquerel 3 Global Characteristics of the Ra-226 chain. 10 a disintegrations and 9 b- disintegrations down to Pb-206 (stable nuclide). Half-lives between some years (Ra-226 and Pb-210) and some fraction of a second (Rn-218 (ms) and Po-214 (µs)). ~ 275 g-rays, mainly in: Pb-214 b- decay to Bi-214 (26 g-rays), Bi-214 b- decay to Po-214 (212 g-rays) and Tl-210 b- decay to Bi-214 (24 g-rays). Laboratoire National Henri Becquerel 4 Evaluation difficulties: 1st Group - Lack of data set (4 examples). - I) Half-lives Isotope Half-life (T1/2) % of DT1/2 N° of measurements Most recent experimental value Ra-226 1600 (7) a 0.4 12 [5] 1966, H. Ramthun Rn-222 3.8232 (8) d 0.02 9 2004, H. Schrader Po-218 3.094 (6) min 0.20 4 [3] 1986, G. V. Potapov At-218 1.4 (2) s 14 2 1989, D. G. Burke Rn-218 35.5 (13) ms 4 5 [4] 1971, A. Erlik Pb-214 26.8 (9) min 3.4 1 1931, M. Curie Bi-214 19.9 (4) min 2 1 1956, H. Daniel Po-214 161.7 (15) ms 0.9 10 [6] 1993, J. W. Zhou Tl-210 1.30 (3) min 2.3 3 [2] 1964, P. Weinzierl Pb-210 22.23 (12) a 0.5 14 [11] 2002, G. A. Rech Bi-210 5.012 (5) d 0.1 6 1959, J. Robert Po-210 138.3763 (17) d 0.001 9 [7] 1964, J. F. Eichelberger []: n° of measurements with uncertainty. Laboratoire National Henri Becquerel 5 - II) a and b- Emission probabilities: lack of measured values. Isotope Type of decay Situation Ra-226 a (100 %) Two measurements in 1963 and 2001. Rn-222 a (100 %) Last measurements in 1958. Po-218 a (99.978 %) b- (0.022 %) Last measurements in 1958. Last measurements in 1952. At-218 a (99.9 %) b- (0.1 %) Last measurements in 1958. Last measurements in 1948. Rn-218 a (100 %) No direct measurements available. Pb-214 b- (100 %) No direct measurements available. Bi-214 a (0.02 %) b- (99.98 %) Last measurements in 1960. No direct measurements available. Po-214 a (100 %) No direct measurements available. Tl-210 a (100 %) Last measurements in 1964. Pb-210 a (1.9 10-6 %) b- (~ 100 %) Three measurements in 1961, 1962 and 1964. Five measurements between 1953 and 1963. Bi-210 a (1.4 10-4 %) b- (~ 100 %) Five measurements between 1947 and 1962. No direct measurements available. Po-210 a (100 %) No direct measurements available. Laboratoire National Henri Becquerel 6 - III) X-ray emissions. Isotope Type of emission Situation Ra-226 X-rays Three measurements in 1973, 1983 and 2002. Rn-222 g-rays X-rays No direct measurements available. Po-218 X-rays No direct measurements available. At-218 X-rays No direct measurements available. Rn-218 X-rays No direct measurements available. Pb-214 X-rays Two measurements in 1969 and 1983. Bi-214 X-rays No recent measurements since 1983. Po-214 X-rays No direct measurements available. Tl-210 g-rays X-rays No recent measurements since 1964. Pb-210 X-rays Four measurements in: 1957, 1971, 1987 and 1990. Bi-210 g-rays X-rays No direct measurements available. Po-210 X-rays No direct measurements available. Laboratoire National Henri Becquerel 7 - IV) Example of decay scheme particularly unknown: Tl-210 b-decay to Pb-210 Laboratoire National Henri Becquerel 8 This decay scheme is based on the measurements of P. Weinzierl (1964): Energy (keV) 83(a) Relative g-ray Emission intensity (%) 2.0 97 4 (2) 296 80 (10) 356 (a) 4 (2) 382 (a) 3 (2) 480 670 Experimental data set of the relative g-ray emission intensities. 2 (1) (a) 799 100 860 7 (2) 910 (a) 3 (2) 1070 12 (5) 1110 7 (2) 1210 17 (4) 1316 21 (5) 1410 5 (2) 1490 (a) 2 (1) 1540 (a) 2 (1) 1590 1650 (a) 2010 2090 Laboratoire National Henri Becquerel (a) Not placed in the decay scheme 2 (1) (a) 2 (1) 2 (1) 7 (2) 5 (2) 2270 3 (2) 2360 8 (3) 2430 9 (3) 9 Experimental values of transition probabilities. b- Level Energy (keV) P. Weinzierl (1964We06) Adopted values 11 1380 (12) 25 % 2% 10 1603 (12) 9 1860 (12) 8 2024 (12) 7 2413 (12) 3 4290 (12) 31 % 2 4386 (12) 13 % Q(Audi) = 5482 (10) keV 7% 56 % 24 % 10 % 19 % Qeff = 4390 (1600) keV 10 % Pb- = 97 % Qeff = 5470 (1000) keV Conclusion: New measurements are strongly suggested. Laboratoire National Henri Becquerel 10 Evaluation difficulties: 2nd Group- g-ray emission intensity. Ra-226 radioactive chain: ~ 275 g-rays. 1. Good examples: many and recent articles found about direct measurements. A) Pb-214 b- decay to Bi-214, Bi-214 b- decay to Po-214 and Ra-226 a decay to Rn-222 We have: * 5 measurements of absolute g-ray emission intensities: E. W. A. Lingeman (1969), D. G. Olson (1983), U. Schötzig (1983), W. -J. Li (1991) and J. Morel (2004) * 14 measurements of relative g-ray emission intensities, where: 8 measurements not used because: a) a lack of information in articles – K. Ya. Gromov (1969), G. Wallace (1969) and M. A. Farouk (1982) b) values comes from the same laboratory: A. Hachem (1975), G. Mouze (1981), H. Akcay (1982), G. Mouze (1990) and G. Diallo (1993). Finally, 6 measurements used: G. T. Ewan (1964), V. Zobel (1977), G. Mouze (1990), D. Sardari (2000), J. U. Delgado (2002) and G. L. Molnar (2002). Laboratoire National Henri Becquerel 11 B) Pb-210 b- decay to Bi-210 We have 9 measurements of relative g-ray emission intensities (the most recent one in 1990), where 4 measurements were not used because of a lack of information in articles (D. K. Butt (1951), C. S. Wu (1953), P. E. Damon (1954) and I. Y. Krause (1958)). C) Po-210 a decay to Pb-206 We have 8 (no recent) measurements: M. A. Grace (1951), M. Riou (1952), W. C. Barber (1952), O. Rojo (1955), R. W. Hayward (1955), A. Ascoli (1956), N. S. Shimanskaia (1957) and V. V. Ovechkin (1957). Laboratoire National Henri Becquerel 12 Evaluation difficulties: 2nd Group - g-ray emission intensity. 2. Difficult examples: no articles found in the literature for direct gamma–ray measurements. A) Measurements of g-ray emission intensity found in the literature come from indirect measurements: * Rn-218 a decay: g-ray emission intensity was deduced from the U-230 decay chain. * Po-214 a decay: g-ray emission intensity was obtained from the Ra-222 decay. OR B) Adopted g-ray emission intensity comes from a and b- intensity measurements: * Rn-222, Po-218 and Bi-210 a decays Laboratoire National Henri Becquerel 13 Evaluation difficulties: 3rd Group- Decay scheme balance. 1) Pb-214 b- decay. Internal conversion coefficients (ICC’s) for g-ray transitions of Bi-214 have been deduced from Rösel’s tables. These coefficients lead to a better decay scheme. ICC’s given by Rösel Pb- = 100.6 % ICC’s given using BRICC computer code (Band’s values) Pb- = 102 % Eg (keV) Multiporality aT (Rösel) aT (BRICC) 53.2275 (21) M1 + E2, d = 0.030 (10) 1.288 (39) E+01 1.214 (19) E+01 241.997 (3) M1 (+E2), d = 0.00 (15) 8.88 (27) E-01 8.38 (18) E-01 295.224 (2) M1 + E2, d = 0.30 (13) 4.82 (14) E-01 4.6 (3) E-01 351.932 (2) M1 (+E2), d = 0.00 (32) 3.19 (10) E-01 3.00 (25) E-01 Q(Audi) = 1019 (11) keV Qeff = 1024 (11) keV Rel. Error = 0.51 % Qeff = 1029 (15) keV Rel. Error = 0.99 % Laboratoire National Henri Becquerel 14 Evaluation difficulties: 3rd Group - Decay scheme balance. 2) Tl-210 b- decay. All decay scheme is based on the only measurement found in the literature given by P. Weinzierl (1964) and several inconsistencies appeared, as shown previously. Because of these inconsistencies, there is a lack of 3 % in decay scheme balance (Pb = 97 %) and we wait for new measurements to solve these problems. Laboratoire National Henri Becquerel 15 Conclusions Taking into account the experimental values of g-ray emission intensities, we have done a new evaluation of the Ra-226 decay chain down to Pb-206. A total of twelve radionuclides have been reviewed ( ~ 275 g-rays). For other nuclear data like half-life, X-rays, b- and a emission intensities, the situation is as follows: A - Half-lives. Critical cases: Pb-214 (1 measurement by M. Curie in 1931) Bi-214 (1 measurement by H. Daniel in 1956). For four nuclides (Ra-226, Tl-210, Bi-210 and Po-210): no recent measurements since the 1960’s. B – X-rays. Only few measurements for Ra-226, Pb-214, Bi-214, Tl-210 and Pb-210. For the other radionuclides: no direct measurements available. C - b- and a emission intensities. Except for Ra-226 (last measurement in 2001), no recent measurement were found in the literature since 1960’s. To solve all problems in decay scheme of nuclides that belong to Ra-226 decay chain,we need new measurements of these nuclear data. Laboratoire National Henri Becquerel 16 More information about evaluations can be obtained at: http://www.nucleide.org/NucData.htm Laboratoire National Henri Becquerel 17