Extension of recommended cross section database for production of therapeutic isotopes

Tárkányi, F.; Hermanne, A.; Ignatyuk, A. V.; Ditrói, F.; Takács, S.; Capote Noy, R.

doi:10.1007/s10967-023-09283-8

Extension of recommended cross section database for production of therapeutic isotopes

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Published: 09 January 2024

Volume 333, pages 717–804, (2024)
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Extension of recommended cross section database for production of therapeutic isotopes

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F. Tárkányi¹,
A. Hermanne²,
A. V. Ignatyuk³,
F. Ditrói ORCID: orcid.org/0000-0002-3520-157X¹,
S. Takács¹ &
…
R. Capote Noy⁴

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Abstract

Radionuclide-based diagnostics and therapy require proper selection of production nuclear reaction based on knowledge of the production excitation functions and the achievable yields completed with data on the formation of possible impurities. In the present work the existing IAEA recommended cross section data database for production of therapeutic isotopes is extended to production of the ⁴⁷Sc,⁴⁷Ca(⁴⁷Sc), ^58mCo, ⁷¹As(⁷¹Ge), ⁷¹Ge, ⁷⁷Br, ⁷⁷Kr(⁷⁷Br), ^80mBr, ¹⁰³Pd, ¹⁰³Pd(^103mRh), ¹⁰³Ru(^103mRh), ¹⁰⁵Rh, ^117mSn, ¹¹⁹Sb, ^119mTe(¹¹⁹Sb), ¹³⁴Ce, ¹³⁵La, ^149gTb, ¹⁶¹Tb, ¹⁶⁵Er, ¹⁶⁵Tm(¹⁶⁵Er), ¹⁶⁷Tm, ^197mHg, ^197gHg, ^198gAu, and ²³⁰Pa(²³⁰U) radioisotopes. Nearly 60 nuclear reactions are presented and discussed. The new recommended cross-section data and their uncertainties for the production of these 21 radionuclides will be available on the Web page of the IAEA Nuclear Data Section at https://nds.iaea.org/radionuclides and also at the IAEA medical portal https://nds.iaea.org/medportal.

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Discussion of the evaluated nuclear reactions

Following a short comment on the therapeutic application and the decay scheme, subSects. "Production of 47Sc" to "198gAu production" include the figures of all experimental data compared to theoretical TENDL predictions, the selected data with Padé fits and statistical uncertainties. The yields for the evaluated reactions, calculated from recommended data derived from the Padé fit, are presented at the end of each subsection in one or two figures. The full reference list for all compiled reactions related to the production of the discussed therapeutic isotopes is at the end of the publication.

Production of ⁴⁷Sc

⁴⁷Sc is a promising β¯-emitter for targeted radionuclide therapy that forms a theranostic pair with the positron emitters ⁴⁴Sc or ⁴³Sc. Moreover, it is a theranostic radionuclide as such, as its single dominant 159keV gamma line is suitable for imaging via single photon emission computed tomography (SPECT). It may be produced directly or through the decay of its parent, ⁴⁷Ca (T_1/2 = 4.54 d, 100% by β¯). The decay scheme is available in [15] and decay data are displayed in Table 2.

Evaluated nuclear reactions for ⁴⁷Ca and ⁴⁷Sc formation

The ^natV(p,x)⁴⁷Ca, ^natV(p,x)⁴⁷Sc, ^natV(d,x)⁴⁷Sc, ^natV(d,x)⁴⁷Ca, ^natTi(p,x)⁴⁷Sc, ^natTi(p,x)⁴⁷Ca, ^natTi(d,x)⁴⁷Sc, ⁴⁸Ca(p,2n)⁴⁷Sc and ⁴⁸Ti(p,2p)⁴⁷Sc reactions were evaluated.

Information on the reactions for formation of ⁴⁷Ca is important for either limitation of impurity or considering a cumulative production, especially at higher particle energy.

^natV(p,x)⁴⁷Ca

Three data sets were found: Heinninger [16], Hontzeas [17] and Michel [18]. Corrections for outdated decay and monitor data were done. The Hontzeas 1963 [17] data, unrealistic too high, were deselected for fit.

All data, in comparison with TENDL theoretical predictions, are shown in Fig. 1. Selected data and Padé fit are in Fig. 2. The calculated yields, based on the recommended values from the Padé fit, are shown in Fig. 19. No experimental yield data were found in the literature.

^natV(p,x)⁴⁷Sc

Seven experimental data sets were found, published by Heininger [13], Hontzeas [14], Michel [19], Michel [18], Levkovskij [20], Pupillo [21] and Barbaro [22]. The cross sections are cumulative, measured after the complete decay of parent ⁴⁷Ca.

In Hontzeas [17], Michel [18] and Levkovskij [20] cross sections are reported for the ⁵¹V(p,x)⁴⁷Sc reaction (⁵¹V has 99.75% abundance in ^natV). The Pupillo [21] and Barbaro [22] data were found to be identical (two separate reports on the same experiment). Only Barbaro [22] was considered further and was multiplied by a factor of 1.2. The outlying Heiniger [16] and Hontzeas [17] sets were deselected.

All data (with comparison to TENDL theoretical predictions) and Padé fitted selected data are shown in Figs. 3 and 4. The calculated yields, based on the recommended cross sections obtained from the fit, are shown in Fig. 20. Experimental yields were reported by Acerbi [23] and Dmitriev [24].

^natV(d,x)⁴⁷Ca

Qaim [25] and Tárkányi [26] reported cross section data for the ^natV(d,x)⁴⁷Ca reaction. In Qaim [25] results are reported as ⁵¹V(d,x)⁴⁷Ca. Both data sets were selected and are shown, in comparison with TENDL theoretical predictions, in Fig. 5 while the Padé fit is in Fig. 6. The calculated yields are shown in Fig. 19. No experimental yield data were found.

^natV(d,x)⁴⁷Sc

Three data sets were published: Sonzogni [27], Qaim [25], and Tárkányi [26]. In Qaim [25] and Sonzogni [27] cross sections for the ⁵¹V(d,x) ⁴⁷Sc reaction (99.75% ⁵¹V abundance in ^natV) are reported. The data are cumulative as they were measured after the complete decay of the ⁴⁷Ca parent. All sets were selected for fitting. All data, in comparison with TENDL theoretical predictions, are presented in Fig. 7, while the Padé fit is in Fig. 8. The calculated yields are shown in Fig. 20. No experimental yield data were found.

^natTi(p,x)⁴⁷Ca

Three data sets were found in the literature: Michel [18], Michel [28] and Neumann [29]. All sets were selected and fitted and are shown in Figs. 9 and 10. The calculated yields are shown in Fig. 19. No experimental yield values were found.

^natTi(p,x)⁴⁷Sc

A total of 15 data sets were found in literature: Michel [30], Michel [31], Michel [18], Fink [32], Brodzinski [33], Kopecky [34], Michel [28], Neumann [29], Zarie [35], Khandaker [36], Garrido [37], Parashari [38], Cervenak [39], Azzam [40], Voyles [41] and Liu [42].

Three low-energy data points of Khandaker [36] and 4 low-energy points of Azzam [40] were deselected as they are below the threshold of the ⁴⁸Ti(p,2p)⁴⁷Sc reaction. The Liu [42] set was deselected as values contradict other low energy data. Moreover, it is in disagreement with the shape of the excitation function of the ⁴⁸Ti(p,2p)⁴⁷Sc reaction (see Sect. 4.1.8). The Fink [32] and Brodzinski [33] data above 100 MeV were not used. All available sets, in comparison with theoretical TENDL predictions, are shown in Fig. 11, and the selected data with Padé fit are in Fig. 12.

The calculated yields are shown in Fig. 20. Thick target yields were reported by Dmitriev [43] and Sabbioni [44].

^natTi(d,x)⁴⁷Sc

Eight experimental data sets were found in literature: Takács [45], Hermanne [46], Takács [47], Gagnon [48], Khandaker [49], Khandaker [50], Lebeda [51] and Duchemin [52] (Fig. 13). All data were selected and fitted (Fig. 14). The calculated yields are shown in Fig. 20. Experimental yield was reported by Dmitriev [43].

⁴⁸Ti(p,x)⁴⁷Sc

Two experimental data sets, measured by Gadioli [53] and Levkovskij [54], are available in the literature and were selected. All experimental data, in comparison with the TENDL predictions, are shown in Fig. 15, and the Padé fit in Fig. 16. The calculated yield is in Fig. 20. No experimental yield data were found.

⁴⁸Ca(p,2n)⁴⁷Sc

In the investigated energy range 3 data sets are available, published by Levenberg [55] (above 100 MeV), Carzaniga [56] and Sitarz [57] (Fig. 17). Sitarz [57] data were converted from differential yield measurements and were multiplied by a factor of 1.4 as was done when using other reactions of this publication in our evaluations. Still no reason was found for the systematic disagreement.

Selected data and Padé fit are shown in Fig. 18. The calculated integral yields are shown in Fig. 20. Thick target yields were measured by Dmitriev [43] and Misiak [58]. The Misiak [58] differential yield data cannot be converted to cross section because two reactions on ⁴⁶Ca and ⁴⁸Ca contribute to the production of ⁴⁷Sc.

Integral yields for ⁴⁷Ca and ⁴⁷Sc formation

Integral yields of reactions related to the production of ⁴⁷Sc and parent ⁴⁷Ca are deduced from the recommended values obtained from Padé fittings and are shown in Figs. 19 and 20.

Production of ^58mCo

Being an Auger emitter ^58mCo (T_1/2 = 9.10 h, IT = 100%) forms a theranostic pair with ⁵⁵Co (T_1/2 = 17.53 h, β⁺ = 77%) used in PET imaging. The decay schemes are available in NUDAT 3.0 [15] and decay data are displayed in Table 2.

Evaluated nuclear reactions for ^58mCo formation

The ⁵⁸Fe(p,n)^58mCo and ⁵⁵Mn(α,n)^58mCo reactions were evaluated.

⁵⁸Fe(p,n)^58mCo

Two experimental data sets exist, reported by Zarubin [59] and Sudar [60] and were selected. The experimental data, in comparison with the theoretical predictions, are shown in Fig. 21, the selected data with Padé fit in Fig. 22 and the calculated physical yield in Fig. 25. No experimental yield data were found.

⁵⁵Mn(α,n)^58mCo

Matsuo [61], Long Xianguan [62] and Sudar [60] presented experimental cross section data (Fig. 23). All data were selected and fitted (Fig. 24). The calculated physical yields are shown in Fig. 25. No experimental yield data were found.

Integral yields for ^58mCo formation

Integral yields of reactions related to the production of.^58mCo are deduced from the recommended values obtained from Padé fittings and are shown in Fig. 25

⁷¹Ge production

The ⁷¹Ge (T_1/2 = 11.43 d) decays by pure electron capture (EC) with subsequent Auger electron emission, making it a potential therapeutic isotope. It forms a theranostic pair with the attractive PET isotope ⁶⁹Ge (T_1/2 = 39 h, 21% β⁺, E_max = 1205 keV). ⁷¹Ge can be produced directly and through the decay of the shorter-lived ⁷¹As parent isotope (T_1/2 = 65.28 h). The decay schemes are available in [15] and decay data are displayed in Table 2.

Evaluated nuclear reactions for ⁷¹As and ⁷¹Ge formation

The ⁶⁸Zn(α,n)⁷¹Ge, ^natGa(α,x)⁷¹As, ^natGe(p,xn)⁷¹As, ^natGe(d,x)⁷¹As, ⁷⁰Ge(d,n)⁷¹As and ⁷²Ge(p,2n)⁷¹As reactions were evaluated.

⁶⁸Zn(α,n) ⁷¹Ge

Two data sets were found, published by Stelson [63] and Antropov [64]. Antropov [64] data were energy shifted to correspond better with the TENDL predictions and the highest energy point at 24.2 MeV was deleted. The experimental data, with comparison to the TENDL predictions, are shown in Fig. 26 and the Padé fit on the selected data is displayed in Fig. 27. The calculated integral yield is shown in Fig. 39. No experimental yield was found.

^natGa(α,x)⁷¹As

A total of 5 data sets were found in literature: Rizvi 1989 (results on ^natGa and ⁶⁹Ga targets) [65], Ismail [66], Levkovskij [54] and Didik [67]. The Rizvi [65] data on natural targets were deleted for the following reasons. According to the publication, ^natGa targets were used but results for ⁶⁹Ga(α,2n) ⁷¹As + ⁷¹Ga(α,4n) ⁷¹As cross sections were presented, which is not identical to ^natGa(α,xn). No information is given how the (α,4n) data were obtained. In addition, the first two points of normalized values of Rizvi [62] obtained on ⁶⁹Ga targets were deleted.

All data, in comparison with TENDL predictions, are shown in Fig. 28, Padé fitted selected data in Fig. 29, and calculated integral yields in Fig. 38. Experimental yield data were reported by Dmitriev [43].

^natGe(p,xn)⁷¹As

A total of five data sets were found in the literature: Basile [68], Horiguchi [69], Levkovskij [54], Spahn [70] and Barabanov [71]. All data were selected. All data, compared to the theoretical predictions, are shown in Fig. 30 while the Padé fit is seen in Fig. 31. The calculated yields are shown in Fig. 38. Dmitriev [43] reported experimental yield data.

^natGe(d,x)⁷¹As

For the ^natGe(d,x)⁷¹As reaction two experimental data sets exist: Otozai [72] and Takács [73]. Both sets were selected but the uncertainties of the Otozai [72] data at energies above 10 MeV were enlarged.

The experimental data, compared to the TENDL predictions, are shown in Fig. 32, the Padé fit on selected data in Fig. 33, and the calculated integral yield in Fig. 38. An experimental yield at 22 MeV was reported by Dmitriev [24].

⁷⁰Ge(d,n)⁷¹As

Two data sets were published: Otozai [72] and Takács [73] and were selected. The experimental and TENDL theoretical predictions are shown in Fig. 34, and the selected data with the Padé fit in Fig. 35. The calculated physical yields are shown in Fig. 38. No experimental yield data were found.

⁷²Ge(p,2n)⁷¹As

Three data sets were found in the investigated energy range: Basile [68], Levkovskij [54] and Spahn [74]. All data sets were selected. The uncertainty on Basile's [68] data was enlarged. The experimental data, the theoretical TENDL predictions and the Padé fit are shown in Figs. 36 and 37. The calculated integral yields are presented in Fig. 38.

Integral yields for ⁷¹As and ⁷¹Ge formation

Integral yields of reactions related to the production of ⁷¹As and parent.⁷¹Ge are deduced from the recommended values obtained from Padé fittings and are shown in Figs. 38 and 39

Production of ⁷⁷Br

The radioisotope ⁷⁷Br, decaying by electron capture with a half-life of 57 h, can be used in Auger therapy and the emission of a 239 keV γ-line allows imaging by SPECT. It can be produced directly or through the decay of its ⁷⁷Kr parent isotope. The ⁷⁷Kr and ⁷⁷Br decay schemes are available in [15] and decay data are displayed in Table 2.

Evaluated nuclear reactions for ⁷⁷Kr and ⁷⁷Br formation

The ⁷⁷Se(p,n)⁷⁷Br, ⁷⁸Se(p,2n)⁷⁷Br, ⁷⁹Br(p,xn)⁷⁷Kr, ⁷⁵As(α,2n)⁷⁷Br and ^natKr(p,x)⁷⁷Br reactions were evaluated. For each of the possibly interesting reactions ⁸¹Br(p,x)⁷⁷Kr (E_max = 85 MeV), ^natSe(d,x)⁷⁷Br (E_max = 21 MeV), ⁸⁰Kr(p,x)⁷⁷Br (E_max = 38.8) MeV) and ⁷⁸Se(α,2n)^80mBr (E_max = 46 MeV) only a single set of experimental data is available and no evaluation or fit was performed.

⁷⁷Se(p,n)⁷⁷Br

Ten data sets were found in the literature: Johnson [75], Johnson [76], Johnson [77], Nozaki [78], Levkovskij [54], Gyurky [79], Hassan [80], El Azony [81], Spahn [82] and Foteinou [83]. The three sets Johnson [75,76,77] were multiplied by a factor of 0.5 and the uncertainty was considered to be 17%. The 5 data points between 19 and 27 MeV of Hassan [80] were deselected (normalized from data on ^natSe). The too low set by Foteinou [83] was deselected. All data sets and comparison with TENDL prediction are shown in Fig. 40, and the selected data with Padé fit in Fig. 41. The yields for production of ⁷⁷Br calculated from the fitted results are collected in Fig. 51. Experimental yield data were reported by Janssen [84], Dmitriev 1982 [85] and Nickles [86].

⁷⁸Se(p,2n)⁷⁷Br

Two data sets were found: Levkovskij [54] and Spahn [82]. The five data points below 30 MeV of Spahn [82] were deselected, due to large disagreement. Data, theory and fit are presented in Figs. 42. and 43. Calculated yields based on recommended fit results are presented in Fig. 51. Experimental yields are reported by Madhusudhan [87] and Janssen [84].

⁷⁹Br(p,3n)⁷⁷Kr

Ten experimental data sets were found: Lundqvist [88], Diksic [89], Nozaki [78], De Jong [90], Weinreich [91], Sakamoto [92], Deptula [93], Levkovskij [54], Zaitseva [94] and De Villiers [95]. Based on corrections already applied on cross sections for other reactions the Diksic [89] were normalized by a factor of 0.8. and the point at 30 MeV was deselected. The results of Nozaki [78] were normalized by a factor of 0.6. The De Jong [90] high energy data were deselected (above 52 MeV). An outlying point of Lundqvist [88] was not represented and deselected (> 800mb). Results obtained by experiments on ^natBr targets from 25 MeV on to below the threshold of ⁸¹Br(p,5n) were normalized (Lundqvist [85], Nozaki [75], Weinreich [88], Deptula [90], Zaitseva [91], De Villiers [92].

The available data with TENDL predictions are shown in Fig. 44, and the fitted selected data in Fig. 45. The integral yields, calculated from the recommended cross sections obtained through Padé fitting, are shown in Fig. 50. No experimental yield data were found.

⁷⁵As(α,2n)⁷⁷Br

Five data sets are available in the literature: Waters [96], Nozaki [78], Alfassi [97], Qaim [98] and Breunig [99] (Fig. 46). All data were selected and fitted as shown in Fig. 47. Calculated yields are presented in Fig. 51. Experimental yield are reported by Dmitriev [85].

^natKr(p,x)⁷⁷Br

Two data sets are available: Steyn [100] and Tárkányi [101]. Both data sets were selected. All data, theoretical TENDL predictions and the Padé fits are presented in Figs. 48 and 49, the calculated yield values in Fig. 51. No experimental yield data were found.

Integral yields for ⁷⁷Kr and ⁷⁷Br formation

Integral yields of reactions related to the production of ⁷⁷Kr and ⁷⁷Br are deduced from the recommended values obtained from Padé fittings and are shown in Figs. 50 and 5

^80mBr production

The Auger electron-emitting nuclide ^80mBr (T_1/2 = 4.43 h) can be used for therapeutic application. In combination with other radioisotopes of bromine (⁷⁵Br (T_1/2 = 96.7 min PET) and ⁷⁶Br (T_1/2 = 16.2 h, PET), ⁷⁷Br (T_1/2 = 57.04 h, SPECT) it forms a theranostic ensemble. The decay schemes are available in [15] and decay data are displayed in Table 2.

Evaluated nuclear reactions for ^80mBr formation

The ⁸⁰Se(p,n)^80mBr, ^natSe(d,xn)^80mBr, ^natSe(p,x)^80mBr, ⁸⁰Se(d,2n)^80mBr and ^natSe(α,x)^80mBr reactions were evaluated.

⁸⁰Se(p,n)^80mBr

Five experimental cross section data sets were found: Blaser [102], Debuyst [103], Levkovskij [54], Al-Azony [81] and Spahn [82]. All data were selected and are shown in Figs. 52 and 53 together with the theoretical predictions and the Padé fit. The calculated integral yields for the production of ^80mBr are collected in Fig. 62. Nickles [86] reported experimental yield data.

^natSe(d,xn)^80mBr

For the ^natSe(d,xn)^80mBr reaction two data sets are available: Debuyst [103] (results on ⁸⁰Se, normalised) and Tárkányi [104]. The outlying cross section point of Debuyst 1968 [103] at 9.52 MeV was deselected. All data with TENDL predictions are shown in Fig. 54, the Padé fitted selected data in Fig. 55 and the calculated yield in Fig. 62. No experimental yield data were found.

^natSe(p,x)^80mBr

Five experimental data sets were published: Blaser [102], Debuyst [103], Levkovskij [54], El-Azony [81] and Spahn [82]. All sets were selected. The too-high value of Spahn [82] at 11.7 MeV was deselected. Experimental data and the TENDL theoretical excitation functions are shown in Fig. 56, the selected experimental works and Padé fit in Fig. 57. Integral yield based on the recommended values obtained from the fit are displayed in Fig. 62. No experimental yield data were found.

⁸⁰Se(d,2n)^80mBr

Two data sets by Debuyst [103] and Tárkányi [104] (obtained on ^natSe, normalized in appropriate energy domain to ⁸⁰Se abundance for use here) exist. Both were selected, except one outlying point of Debuyst [103] at 9.32 MeV. All data and the TENDL prediction are shown in Fig. 58, selected data with Padé fit in Fig. 59, and the calculated yields in Fig. 62. Vakilova [105] reported experimental yield data.

^natSe(α,x)^80mBr

Two data sets by Debuyst [103] and Levkovskij [54] exist. Levkovskij [54] has data only for reactions on ⁷⁸Se (23.78% abundance in ^natSe) and ⁸⁰Se (49.61%) targets: the two results were weighted and summed. The contribution of activation on ⁷⁷Se (7.63% abundance in ^natSe) was considered to be negligible above 20 MeV. The two lowest points of Levkovskij [54] are deselected as they are too low, most probably because no contribution of ⁷⁷Se is available.

Experimental data, TENDL theoretical predictions, and selected data with Padé fit are shown in Figs. 60 and 61, the calculated yields in Fig. 62. No experimental yield data were found.

Integral yields for ^80mBr formation

Integral yields of reactions related to the production of ^80mBr are deduced from the recommended values obtained from Padé fittings and are shown in Fig. 62.

¹⁰³Pd and ¹⁰³Ru production

Palladium-103 (T_1/2 = 16.991 d) and Ruthenium-103 (T_1/2 = 39.247 d) are the parent isotopes of ^103mRh (T_1/2 = 56.1 min), which is applied for Auger electron therapy in permanent implants.

The ¹⁰³Pd and ¹⁰³Ru decay schemes and decay data are available in [15] and are displayed in Table 2.

Evaluated nuclear reactions for ¹⁰³Ru and ¹⁰³Pd formation

The ^natAg(p,x)¹⁰³Pd, ^natRu(p,x)¹⁰³Ru, ^natRu(d,x)¹⁰³Ru and ¹⁰⁰Mo(α,n)¹⁰³Ru reactions were evaluated.

The ¹⁰³Rh(p,n)¹⁰³Pd and ¹⁰³Rh(d,2n)¹⁰³Pd reactions were evaluated by us earlier [8] and recommended cross section values are available in the IAEA NDS medical database [106].

^natAg(p,x)¹⁰³Pd

Two data sets were found: Fassbender [107] and Uddin [108]. The 3 high energy points of Uddin [108] were deselected as they are outlying compared to the TENDL predictions (good summed description of the reactions on the two stable Ag target isotopes) and the Fassbender [107] results. All data, in comparison with the TENDL predictions, are shown in Fig. 63. The selected data with the Padé fit can be seen in Fig. 64. The calculated yields are displayed in Fig. 71. No experimental yield data were found in the literature.

^natRu(p,x)¹⁰³Ru

Gagnon [109] and Hermanne [110] presented experimental cross section data that are shown in Fig. 65 in comparison with the TENDL theoretical predictions. Both sets were selected and fitted (Fig. 66). Calculated physical yields are shown in Fig. 72. No experimental yield data were found.

^natRu(d,x)¹⁰³Ru

Two data sets are available: Mito [111] (only data on ¹⁰²Ru target, useful in lower energy range after normalization) and Tárkányi [112] up 50 MeV.

All experimental data, in comparison with the TENDL theoretical prediction, are shown in Fig. 67, the fitted selected data in Fig. 68 and the calculated physical yield in Fig. 72. No experimental yield data were found.

¹⁰⁰Mo(α,n)¹⁰³Ru

Four data sets are available in the literature: Esterlund [113], Graf [114], Ditrói [115] and Tárkányi [116]. The Esterlund [113] data were multiplied by a factor of 2 (correction for incoming particle flux, alpha Z = 2) and the lowest energy point was deselected (below the threshold). All data, in comparison with the TENDL theoretical predictions, are shown in Fig. 69. The selected data and the Padé fit are displayed in Fig. 70, the calculated yield in Fig. 72. No experimental yield data were found.

Integral yields for ¹⁰³Pd and ¹⁰³Ru formation

Integral yields of reactions related to the production of ¹⁰³Pd and ¹⁰³Ru are deduced from the recommended values obtained from Padé fittings and are shown in Figs. 71,72.

¹⁰⁵Rh production

Rhodium-105 (T_1/2 = 35.4 h), a mostly reactor-produced radionuclide, decays by β⁻ emission with moderate energy which makes it suitable for radiotherapy. It also emits γ-rays that are used for SPECT diagnostic experiments. The decay scheme is available in [15] and decay data are displayed in Table 2.

Evaluated nuclear reaction for ¹⁰⁵Rh formation

The ¹⁰⁴Ru(d,n)¹⁰⁵Rh reaction was evaluated.

¹⁰⁴Ru(d,n)¹⁰⁵Rh

Two experimental data sets obtained by Sitarz [57] and Tárkányi [116] were found. The Sitarz [57] data were multiplied by a factor of 1.4 on the basis that all data in this publication show systematically significantly lower values when compared to the results of other authors (see also Sect. 4.1.9). All data, in comparison with TENDL predictions, and selected data with Padé fit are shown in Figs. 73 and 74. The calculated yield data are displayed in Fig. 75. No experimental yield data were found.

Integral yields for ¹⁰⁵Rh formation

Integral yield for the ¹⁰⁴Ru(d,n)¹⁰⁵Rh reaction are deduced from the recommended values obtained from Padé fitting and is shown in Fig. 75.

^117mSn production

The radio-isotope ^117mSn (T_1/2 = 14 d) decays for 100% by internal transition to stable ¹¹⁷Sn but emits Auger and conversion electrons, making it a candidate for radiotherapy. The decay scheme is available in [15] and decay data are displayed in Table 2.

Evaluated nuclear reactions for ^117mSn formation

The ¹¹⁴Cd(α,n)^117mSn, ¹¹⁶Cd(α,3n)^117mSn, ^natCd(α,xn)^117mSn, ¹¹⁵In(α,pn)^117mSn and ^natSb(p,x)^117mSn reactions were evaluated. For the ^natSb(d,x)^117mSn reaction only one data set (up to 49.2 MeV) was found.

¹¹⁴Cd(α,n)^117mSn

Five data sets were found in the literature: Qaim [117], Rebeles [118], Hermanne [119], Khandaker [120] and Ditrói [121]. Only the Rebeles [118] data were obtained on a ¹¹⁴Cd target, all other sets were normalized from data obtained on ^natCd. The Qaim [117] data were deselected due to large scatter (see also Sects. 4.8.2 and 4.8.3). All data, in comparison with the TENDL theoretical prediction, are shown in Fig. 76. anThe selected data and the Padé fit are displayed in Fig. 77. The calculated physical yields for the production of ^117mSn are displayed in Fig. 86. No experimental yield data were found.

¹¹⁶Cd(α,3n)^117mSn

Nine data sets were found: Montgomery [122], Qaim [117], Rebeles [118], Hermanne (nat) [119], Khandaker (nat) [120], Ditrói [123], Ditrói (nat) [121], Duchemin (nat) [124]. In Qaim [117] an incident 120 MeV energy beam and a stack with many foils was used, unfortunately resulting in a shifted energy scale. A linear downward energy shift was tried out but when agreement for the second peak is attempted, the lowest energy point is shifted nearly 16 MeV to zero MeV.). As part of these corrected data are still scattered, all Qaim [117] data were hence deselected. For the 4 sets obtained on ^natCd targets, the contribution from the reaction on ¹¹⁴Cd in the natural target was subtracted based on the ¹¹⁴Cd (α,n) results (recommended values after fit) (see Sect. "Evaluated nuclear reactions for 117mSn formation").

The experimental data, the TENDL predictions and the selected data with Padé fit are shown in Figs. 78 and 79. The calculated yield data are displayed in Fig. 86. No experimental yield data were found.

^natCd(α,xn)^117mSn

Five data sets obtained on ^natCd targets were found: Qaim [117], Hermanne [119], Khandaker [120], Duchemin [124], Ditrói [123]. By adding the normalized (in relevant limited energy domains) and weighted sums data obtained on enriched ¹¹⁴Cd and ¹¹⁶Cd targets (Montgomery [122] on ¹¹⁶Cd, Rebeles [118] on ¹¹⁴Cd, Rebeles [118] on ¹¹⁶Cd, Ditrói [123] on ¹¹⁶Cd) a total of nine sets became available.

As motivated in the previous section the Qaim [117] set was deselected. The point at 39.5 MeV of Khandaker [120] was also deselected. All data, in comparison with the TENDL prediction, are shown in Fig. 80. The Padé fit of the selected data is displayed in Fig. 81 and the yield calculated from the recommended values based on the Padé fit in Fig. 86. Experimental yields were measured by Dmitriev [125] and Fukushima [126].

¹¹⁵In(α,pn)^117mSn

Four data sets were found in literature: Fukushima [127], Qaim [117], Bhardwaj [128], and Aikawa [129]. As the data are very contradicting (Fig. 90), we tried to make reasonable corrections and took the Aikawa [129] values for reference. As mentioned earlier (see Sect. 4.8.2) for all sets in Qaim [117] an important energy shift due to the long stack is noticed and a downward correction of the energy scale was made. Bhardwaj [128] data were divided by a factor of 2 (beam current, Z = 2 for α-particles), while Fukushima [127] data were multiplied by a factor of 4 (beam current). All original data, in comparison with the TENDL theoretical predictions, are shown in Fig. 82. The 4 selected (3 corrected) sets and the Padé fit are displayed in Fig. 83, and the calculated yield in Fig. 86. Dmitriev [125] reported experimental integral data.

^natSb(p,x)^117mSn

Four experimental cross section data sets are available: Ermolaev [130], Takács [131], Mosby [132], and Ermolaev [133]. All data with TENDL predictions and the selected data with Padé fit are shown in Figs. 84 and 85. The deduced integral yields are displayed in Fig. 86. No experimental integral yield data were found.

Integral yields for ^117mSn formation

Integral yields of reactions related to the production of ^117mSn are deduced from the recommended values obtained from Padé fittings and are displayed in Fig. 86.

¹¹⁹Sb production

The ¹¹⁹Sb (T_1/2 = 38.19 h) decays by EC followed by emission of low energy Auger electrons (∼20 keV, short biological path lengths of∼10 μm) and is hence a candidate for targeted radiotherapy. It can be produced directly and through generator decay of its longer-lived ^119mTe parent (T_1/2 = 4.76 d). The decay scheme is available in [15] and decay data are displayed in Table 2.

Evaluated nuclear reactions for ^119mTe and ¹¹⁹Sb formation

The ¹¹⁹Sn(p,n)¹¹⁹Sb and ^natSb(p,xn)^119mTe reactions were evaluated. For each of the ^natSb(d,xn)¹¹⁹Sb (up to 49.2 MeV) and ^natSb(d,xn)¹¹⁹Te (49.2 MeV) reactions four data sets exist.

¹¹⁹Sn(p,n)¹¹⁹Sb

Four data sets were found: Klyucharev [134], Johnson [135], Lovchikova [136] and Thisgaard [137]. The Klyucharev [134] data were published as relative and were normalized to the data of Johnson [135]. All available data and the theoretical predictions are shown in Fig. 87, the Padé fit on the selected data in Fig. 88, and the calculated yield in Fig. 100. No experimental yield data were found.

^natSb(p,xn)^119mTe

Four experimental data sets are presently available: Lagunas-Solar [138], Yi [139], Takács [131] and Mosby [132] (Fig. 89). All Yi [139] data were deselected because of outlying values in the 35–40 MeV region The Lagunas-Solar [138] data show a strong upward energy shift when compared to the two remaining sets and to the TENDL predictions. is seen for. As this set contains the only data available at high energies they were normalized to recent data (multiplied by a factor of 1.4) and energy corrected via a linear energy shift down to the threshold. The selected data and the Padé fit are shown in Fig. 90, and the calculated integral yield in Fig. 91. Lagunas-Solar [138] reported experimental integral yield data.

Integral yields for ¹¹⁹Sb and ¹³⁹Te formation

Integral yields of reactions related to the production of ¹¹⁹Sb and ¹³⁹Te are deduced from the recommended values obtained from Padé fittings and are shown in Fig. 91.

¹³⁴Ce/¹³⁴La production

The radio-isotope ¹³⁴Ce (T_1/2 = 3.16 d) decays for 100% by EC (accompanied by Auger electrons interesting for therapy) to ¹³⁴La (T_1/2 = 6.45 min, 100% β⁺, 2.7 MeV β⁺). It combines the emission of high-energy beta particles with Auger electrons and can be called a PET “in vivo generator”. The decay schemes are available in [15] and decay data are displayed in Table 2.

Evaluated nuclear reaction for ¹³⁴Ce formation

The ¹³⁹La(p,6n)¹³⁴C e reaction was evaluated.

¹³⁹La(p,6n)¹³⁴Ce

We found 3 experimental sets published by Tárkányi [140], Morell [141] and Becker [142]. All sets were selected and are shown in Fig. 92 with TENDL predictions and in Fig. 93 with the Padé fit. The yield data are presented in Fig. 94. No experimental yields were found in the literature.

Integral yields for ¹³⁴Ce formation

Integral yield of the ¹³⁹La(p,6n)¹³⁴Ce reaction is deduced from the recommended values obtained from Padé fitting and is shown in Fig. 94.

¹³⁵La production

¹³⁵La (T_1/2 = 19.5 h) decays for 100% to stable ¹³⁵Ba by electron capture and has favorable nuclear and chemical properties for Auger-based targeted internal radiotherapy. The decay scheme is available in [15] and decay data are displayed in Table 2.

Evaluated nuclear reaction for ¹³⁵La formation

The ^data (p,xn)¹³⁵La reaction was evaluated. For the ^natBa(d,x)¹³⁵La reaction only a single experimental data set (up to 49.37 MeV) is available.

^natBa(p,xn)¹³⁵La

Two data sets published by Prescher [143] and Tárkányi [144] were found. Both sets were selected. The experimental and theoretical cross sections are shown in Fig. 95, the Padé fit In Fig. 96 while the calculated yields are seen in Fig. 97. Dmitriev [43] reported experimental integral yield data.

Integral yields for ¹³⁵La formation

Integral yield of the ^natBa(p,xn)¹³⁵La reaction is deduced from the recommended values obtained from Padé fitting and are shown in Fig. 97.

^149gTb production

The ground state of ¹⁴⁹Tb (^149gTb, T_1/2 = 4.118 h) has a complex decay pattern (EC 83.3%; α 16.7%; E_α 3970 keV). As a high-energy alpha-emitter, it has great potential application for radiotherapy.

^149gTb can be obtained in direct nuclear reactions and as an “in production equilibrium” decay product of short-lived ^149m,gDy (half-lives of 0.5 s and 4.2 min). The decay scheme is available in [15] and decay data are displayed in Table 2.

Evaluated nuclear reaction for ¹⁴⁹ Tb formation

The ^natGd(p,xn)^149gTb reaction was evaluated. For the ¹⁵²Gd(p,xn)¹⁴⁹ Tb reaction (threshold of 62.5 MeV) only a single experimental data set exists.

^natGd(p,xn)¹⁴⁹Tb

Three data sets are reported in literature: Mironov [145], Steyn [146] and Formento-Cavaier [147]. Mironov data [145] were energy shifted. All data and the comparison with disagreeing theoretical TENDL predictions are shown in Fig. 98. The selected data and Padé fit are displayed in Fig. 99, and the Padé fit based integral yield in Fig. 100. No experimental yield values were found.

Integral yields for ¹⁴⁹Tb formation

Integral yield of the ^natGd(p,xn)¹⁴⁹Gd reaction was deduced from the recommended values obtained from Padé fitting and is shown in Fig. 100.

¹⁶¹Tb production

During low-energy β⁻ decay ¹⁶¹Tb (T_1/2 = 6.89 d) emits conversion and Auger electrons making it interesting for radiotherapy. It also emits low-energy photons that could be used for SPECT imaging. The decay schemes are available in [15] and decay data are displayed in Table 2.

Evaluated nuclear reaction for ¹⁶¹ Tb formation

The ^natGd(p,xn)¹⁶¹Tb reaction was evaluated.

¹⁶⁰Gd(d,n)¹⁶¹Tb

Two data sets are available: Tárkányi [148] and Szelecsenyi [149]. The data show some disagreement. In Tárkányi [148] results obtained in two irradiations at 50 MeV and 20 MeV incident deuterons are discussed and the 20 MeV irradiation shows a better agreement with the data of Szelecsenyi [149] in the 15–20 MeV energy range. All data, in comparison with TENDL predictions, are shown in Fig. 101. The selected data with the Padé fit is in Fig. 102, and the Padé fit based integral yields are in Fig. 103. No experimental yield data were found.

Integral yields for ¹⁶¹Tb formation

Integral yield of the ¹⁶⁰Gd(d,n)¹⁶¹Tb reaction was deduced from the recommended values obtained from Padé fitting and is shown in Fig. 103.

¹⁶⁵Er production

As ¹⁶⁵Er (T_1/2 = 10.4 h) decays by electron capture (EC), followed by the emission of Auger electrons and low-energy X-rays, it is a candidate for targeted radionuclide therapy.

It can be produced directly and through the EC, β⁺ decay of the ¹⁶⁵Tm parent (T_1/2 = 30.06 h).

Evaluated nuclear reactions for ¹⁶⁵Tm and ¹⁶⁵Er formation

The ¹⁶⁵Ho(p,n)¹⁶⁵Er, ¹⁶⁶Er(p,2n)¹⁶⁵Tm, ¹⁶⁵Ho(d,2n)¹⁶⁵Er, ^natEr(p,xn)¹⁶⁵Tm, ^natEr(d,xn)¹⁶⁵Tm and ¹⁶⁶Er(d,3n)¹⁶⁵Tm reactions were evaluated.

1¹⁶⁵Ho(p,n)¹⁶⁵Er

Three data sets were found: Beyer [150], Tárkányi [151] and Gracheva [152]. As Beyer [150] data are energy shifted compared to the two other sets, a linear shift of the energy scale was applied. All data, in comparison with TENDL predictions, are shown in Fig. 104, the Padé fitted selected data in Fig. 105. The calculated integral yields are displayed in Fig. 116. Experimental yield data were reported in Gracheva [152].

¹⁶⁶Er(p,2n)¹⁶⁵Tm

Two experimental data sets obtained on ^natEr targets by Tárkányi [153] and Tárkányi [154] are available in the literature and agree well. The experimental data, the comparison with the TENDL predictions and the Padé fit are shown in Figs. 106 and 107. The calculated yield is displayed in Fig. 115. Dmitriev [43] reported experimental thick target yields.

¹⁶⁵Ho(d,2n)¹⁶⁵Er

Two data sets were reported for the ¹⁶⁵Ho(d,2n)¹⁶⁵Er reaction cross sections by Tárkányi [155] and Hermanne [156]. The outlying data points at 25.2 and 27.3 MeV of Hermanne 2013 [156] were deselected. The original data, with comparison to the TENDL theoretical excitation functions, are in Fig. 108 while the selected data and Padé fit are shown in Fig. 109. The integral yields calculated from the recommended cross sections obtained from the fitted curve are shown in Fig. 116. No experimental yield data were found.

^natEr(p,xn)¹⁶⁵Tm

Two data sets are available: Tárkányi [153] and Song [157]. Both sets were selected and presented, in comparison with TENDL predictions, in Fig. 110 and with Padé fit in Fig. 111. The calculated integral yields are displayed in Fig. 115. Experimental yields were measured and published by Dmitriev [158] and Dmitriev [43].

^natEr(d,xn)¹⁶⁵Tm

Three data sets were found: Tárkányi [159], Tárkányi [160] and Khandaker [161]. All data were selected and are shown, in comparison with TENDL predictions, in Fig. 112 and with Padé fit in Fig. 113. The calculated yields are presented in Fig. 115. Dmitriev reported experimental integral yield data in [158] and in [24].

¹⁶⁶Er(d,3n)¹⁶⁵Tm

Only by Hermanne [162] data for the ¹⁶⁶Er(d,3n)¹⁶⁵Tm reaction were published. Two additional sets were deduced from results obtained on ^natEr targets by Tárkányi [159] and Khandaker [161] after subtracting the weak ¹⁶⁴Er(d,n) ¹⁶⁵Tm contribution, obtained from TENDL prediction and normalization for abundance of the target isotope. Therefore, the additional data are limited up to the ¹⁶⁷Er(d,4n)¹⁶⁵Tm threshold energy of 19,720.8 keV. All these data were selected and are, in comparison with theoretical TENDL predictions, presented in Fig. 114. The Padé fit is displayed in Fig. 115, and the calculated yield data, based on the recommended values in Fig. 116. Experimental integral yield data were obtained by Dmitriev [158] and Dmitriev [43].

Integral yields for ¹⁶⁵Tm and ¹⁶⁵Er formation

Integral yields of reactions related to the production of ¹⁶⁵Tm and ¹⁶⁵Er are deduced from the recommended values obtained from Padé fittings and are shown in Figs. 116,117.

¹⁶⁷Tm production

¹⁶⁷Tm is useful for therapy by emission of Auger-electrons (T_1/2 = 9.25 d, E_e(average) = 124.2 keV) and also for SPECT diagnostics by emitting low energy gamma lines. The decay scheme is available in [15] and decay data are displayed in Table 2.

Evaluated nuclear reactions for ¹⁶⁷Tm formation

The ¹⁶⁹Tm(p,x)¹⁶⁷Tm, ¹⁶⁹Tm(d,x)¹⁶⁷Tm, ^natEr(d,xn)¹⁶⁷Tm, ^natEr(p,xn)¹⁶⁷Tm, ¹⁶⁷Er(p,n)¹⁶⁷Tm and ¹⁶⁵Ho(α,2n)¹⁶⁷Tm reactions were evaluated. For the ^natYb(d,x)¹⁶⁷Tm (up to 48.2 MeV) and ¹⁶⁷Er(d,2n)¹⁶⁷Tm (up to 20.4 MeV) reactions only a single data set is available.

¹⁶⁹Tm(p,x)¹⁶⁷Tm

Two data sets were available and were selected: Tárkányi [163] and Saito [164]. In Saito [164] cross sections at only 3 energies, all below 20 MeV, are given.

All data and comparison with TENDL predictions are shown in Fig. 118, the Padé fit in Fig. 119, and the calculated integral yields in Fig. 130. No experimental yield data were found.

¹⁶⁹Tm(d,x)¹⁶⁷Tm

Four experimental data sets are available: Tárkányi [165], Hermanne [166], Hermanne [167] and Saito [168]. All cross sections and the predictions obtained from TENDL are shown in Fig. 120. All data were selected and Padé fitted (Fig. 121). The calculated yields are shown in Fig. 130. No experimental yield data were found.

^natEr(d,xn)¹⁶⁷Tm

Three data sets published in Tárkányi [159], Tárkányi [160] and Khandaker [161] were found. All data were selected. The experimental data, in comparison with TENDL theoretical excitation functions, are presented in Fig. 122. The Padé fit is displayed in Fig. 123 and the calculated integral yield in Fig. 130. Experimental yield data were presented by Dmitriev [158] and Dmitriev [24, 43].

^natEr(p,xn)¹⁶⁷Tm

Four experimental cross section data sets are available: Rayudu [169], Tárkányi [170], Tárkányi [154] and Hermanne [171] (Fig. 124). Outlying points of Rayudu 1963 [169] at 14 MeV and Tárkányi [170] at 3.1 MeV were deselected. The Padé fit on the selected data is seen in Fig. 125. The calculated integral yield, based on the recommended values from the Padé fit, is shown in Fig. 130. Experimental yields were reported in Dmitriev [158] and Dmitriev [43].

¹⁶⁷Er(p,n)¹⁶⁷Tm

Three data sets were published: Tárkányi [170], Tárkányi [154] and Hermanne [171] (Fig. 126). The two lowest energy points of Tárkányi [170] were deleted. The selected data and the Padé fit are presented in Fig. 127. The calculated integral yield is displayed in Fig. 130. No experimental yield data were found.

¹⁶⁵Ho(α,2n)¹⁶⁷Tm

A large number of sets with cross section data are available in literature: Wilkinson [172], Martin [173], Sau [174], Homma [175], Rama Rao [176], Mukherjee [177], Singh [178], Singh [179], Gadkari [180], Tárkányi [181], Usman [182] (Fig. 128). The sets of Sau [174], Wilkinson [172] and Martin [173] were deselected as all their cross section values are outlying. The too-low values of Gadkari [180], Singh [178] and Rama Rao [176] were multiplied by a factor of 1.8. The values of Singh [179] and Homma [175] were multiplied by a factor of 2. Probably all these authors have a problem with the incoming particle flux by a factor of 2, due to not considering the double charge of the α-particle. The approximation by the factor of 1.8 is due to an additional needed correction for beam intensity. The selected data and the Padé fit are shown in Fig. 129, and the calculated integral yield in Fig. 130. Experimental yield was reported by Dmitriev [158].

Integral yields for ¹⁶⁷Tm formation

Integral yields of reactions related to the production of ¹⁶⁷Tm are deduced from the recommended values obtained from Padé fittings and are shown in Fig. 130.

^197mHg/^197gHg production

The γ-emitting isomers ^197mHg (T_1/2 = 23.8 h, E_γ 134 keV, 34%) and ^197gHg (T_1/2 = 64.14 h, E_γ 77 keV, 19%, 279 keV, 6%) are suitable for SPECT imaging. Moreover, as their IT and EC decay is accompanied by Auger and conversion electron emission, they have an additional potential interest for therapeutic application. The decay schemes are available in [15] and decay data are displayed in Table 2.

Evaluated nuclear reactions for ^197mHg and ^197gHg formation

The ¹⁹⁷Au(p,n)^197mHg, ¹⁹⁷Au(d,2n)^197mHg, ¹⁹⁷Au(p,n)^197gHg and ¹⁹⁷Au(d,2n)^197gHg reactions were evaluated.

¹⁹⁷Au(p,n)^197mHg

In ten publications (Vandenbosch [183], Hansen [184], Gritsyna [185], Szelecsenyi [186], Michel [28], Szelecsenyi [187], Elmaghraby [188], Satheesh [189], Ditrói [190] and Lebeda [191]) experimental cross section data for the ¹⁹⁷Au(p,n)^197mHg reaction are reported. The sets of Vandenbosch [183] and Satheesh [189] were deselected, as their values are significantly outlying near the maximum of the excitation curve. All data, in comparison with predictions in the TENDL databases, are shown in Fig. 131. The selected data and the Padé fit are in Fig. 132 while the calculated integral yields for production of ^197mHg and ^197gHg are presented in Fig. 139. Experimental yields were reported by Abe [192] and Birattari [193].

¹⁹⁷Au(d,2n)^197mHg

Eight experimental data sets were found: Vandenbosch [183], Chevarier [194], Khrisanfov [195], Long [196], Zhao Wenrong [197], Tárkányi [198], Tárkányi [199], Lebeda [191]. The available data, in comparison with the TENDL predictions; are presented in Fig. 133. All data were selected and used for Padé fitting (Fig. 134), the calculated integral yields are shown in Fig. 139. No experimental yield data were found.

¹⁹⁷Au(p,n)^197gHg

Eight authors reported experimental cross section data for the ¹⁹⁷Au(p,n)^197gHg reaction: Vandenbosch [183], Hansen [200], Gritsyna [185], Chodil [201], Elmaghraby [188], Satheesh [189], Ditrói [190] and Lebeda [191]. Three whole sets were deselected (Vandenbosch [183], Satheesh [189] and Chodil [201]) as they are outlying, especially near the maximum of the excitation curve. The available data, in comparison with the TENDL predictions, are shown in Fig. 135, the selected data with the Padé fit in Fig. 136. The calculated integral yields based on the recommended values from the Padé fit can be seen in Fig. 139. Experimental integral yields were measured by Abe [192] and Birattari [202].

¹⁹⁷Au(d,2n)^197gHg

Eight data sets were found: Vandenbosch [183], Chevalier [194], Khrisanfov [195], Long [196], Zhao Wenrong [197], Tárkányi [198], Tárkányi [199] and Lebeda [191] (Fig. 137). The Long [196] and Vandenbosch [183] data sets were deselected. The remaining selected data and the Padé fit are presented in Fig. 138, and the calculated integral yield in Fig. 139. No experimental yield values were found.

Integral yields for ^197mHg and ^197gHg formation

Integral yields of reactions related to the production of ^197mHg and ^197gHg are deduced from the recommended values obtained from Padé fittings and are shown in Fig. 139.

^198gAu production

The radionuclide ^198gAu (T_1/2 = 2.6947 d) is a mixed β¯ (0.96 MeV, abundance 98.6%) and gamma emitter (0.412 MeV, abundance 95.5%). The emission of β¯ particles makes it useful in targeted radiotherapy essentially as permanent seed implant therapy for the prostate gland. The emission of low-energy photons allows for the evaluation of dose distributions by SPECT imaging. The decay schemes are available in [15] and decay data are displayed in Table 2.

Evaluated nuclear reactions for ^198gAu formation

The ¹⁹⁸Pt(p,x)^198gAu and ¹⁹⁸Pt(d,x)^198gAu reactions were evaluated.

¹⁹⁸Pt(p,x)^198gAu

Three data sets are reported by Tárkányi [203], Showaimy [204] and Gantumur [205] (Fig. 140). Seven outlying data points in the 16–22 MeV energy range (at 16.3, 17.4,18.4, 19.4, 20.4, 21.3 and 22.2 MeV) of Tárkányi [203] were deleted and a Padé fit was performed on the remaining selected data (Fig. 141).

The calculated integral yields are shown in Fig. 144. No experimental yield data were found.

¹⁹⁸Pt(d,2n)^198gAu

Five data sets are available, published by Tárkányi [203], Ditrói [206], Khandaker [207], Ditrói [208] and Tárkányi [209] (Fig. 142). All data were selected and fitted (Fig. 143). Calculated yields are seen in Fig. 144. No experimental yield values were found.

Integral yields for ¹⁹⁸Au formation

Integral yields of reactions related to the production of ¹⁹⁸Au are deduced from the recommended values obtained from Padé fittings and are shown in Fig. 144.

²³⁰Pa (²³⁰U) production

The α-emitter ²³⁰U (T_1/2 = 20.8 d) and its short-lived daughter ²²⁶Th (T_1/2 = 30.6 min) are the parents in a generator system of novel therapeutic nuclides for application in targeted radiotherapy. The decay of ²³⁰U/²²⁶Th is followed by a chain of short-lived radionuclides generating numerous additional α-particles.

By using accelerators, ²³⁰U can be obtained through the decay of its ²³⁰Pa (T_1/2 = 17.4 d) parent (β⁻ decay with a probability of 7.8%) with proton or deuteron activation of thorium nuclei (only ²³²Th with a half-life of 1.405 × 10¹⁰ y occurs naturally). The decay schemes are available in [15] and decay data are displayed in Table 2.

Evaluated nuclear reactions for ²³⁰ Pa formation

The ²³²Th(p,3n)²³⁰Pa and ²³²Th(d,4n)²³⁰Pa reactions were evaluated.

²³²Th(p,3n)²³⁰Pa

Twelve sets with experimental cross section data for this reaction were found: Tewes [210], Tewes [211], Meinke [212] (series1 and series2), Lefort [213], Brun [214], Celler [215], Kudo [216], Chu [217], Roshchin [218], Morgenstern [219], Jost [220] and Radchenko [221] (Fig. 145). Out of them Tewes [211] and the two series of Meinke [212] were deselected, for Brun [214] the energy was rescaled and for Lefort [213] the two lowest energy points were deleted. The selected data and the Padé fit with uncertainties can be seen in Fig. 146. The Padé fit based integral yield data is shown in Fig. 149. Experimental yields were reported by Friend [222].

²³²Th(d,4n)²³⁰Pa

Two data sets, measured by Rama Rao [223] and Duchemin [224], are available and both were selected. The experimental data, in comparison to the prediction by TENDL, are shown in Fig. 147, the Padé fit with uncertainties in Fig. 148 while the calculated integral yields are shown in Fig. 149. No experimental yield data were found.

Integral yields for ²³⁰Pa formation

Integral yields of reactions related to the production of ²³⁰Pa are deduced from the recommended values obtained from Padé fittings and are shown in Fig. 149.

Summary and conclusions

Evaluations of production cross sections and their uncertainties were performed on sixty reactions for direct, indirect and generator production of the ⁴⁷Sc,⁴⁷Ca(⁴⁷Sc), ^58mCo, ⁷¹As(⁷¹Ge), ⁷¹Ge, ⁷⁷Br, ^80mBr, ¹⁰³Pd (^103mRh), ¹⁰³Ru(^103mRh), ¹⁰⁵Rh, ^117mSn, ¹¹⁹Sb, ¹³⁴Ce, ¹³⁵La, ¹⁶¹Tb, ¹⁶⁵Er, ¹⁶⁵Tm(¹⁶⁵Er), ¹⁶⁷Tm, ^197mHg, ^197gHg, ^198gAu and ²³⁰Pa(²³⁰U) radioisotopes. The collected experimental data were compared with the theoretical predictions to be found in the TENDL-2017, 2019 and 2021 libraries. While the predictions in TENDL-2017 and 2019 are nearly the same, the description obtained in TENDL-2021 is better but still in some cases significant disagreements in the magnitude and shape of the resulting excitation functions exist (especially when considering isomeric states or deuteron-induced reactions).

A Padé fitting method was applied to the selected datasets, and uncertainties for all recommended cross-section data were deduced. The recommended cross-section data have been used to determine integral yields for practical radionuclide production.

The recommended data may also have a useful role in other fields of non-energy related nuclear studies (e.g., accelerator technology, activation analysis and thin layer activation) and further development of the theory and modelling of nuclear reactions.

References

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Acknowledgements

This work was partly supported by Project No. NKTA-42, which has been implemented with the support provided by the Ministry of Innovation and Technology of Hungary from the National Research, Development and Innovation Fund, financed under the TKP2021 funding scheme.

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Institute for Nuclear Research, Debrecen, Hungary
F. Tárkányi, F. Ditrói & S. Takács
Vrije Universiteit, Brussels, Belgium
A. Hermanne
Institute for Physics and Power Engineering, Obninsk, Russia
A. V. Ignatyuk
IAEA, Vienna, Austria
R. Capote Noy

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F. Tárkányi
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Tárkányi, F., Hermanne, A., Ignatyuk, A.V. et al. Extension of recommended cross section database for production of therapeutic isotopes. J Radioanal Nucl Chem 333, 717–804 (2024). https://doi.org/10.1007/s10967-023-09283-8

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Received: 15 September 2023
Accepted: 15 November 2023
Published: 09 January 2024
Issue Date: February 2024
DOI: https://doi.org/10.1007/s10967-023-09283-8

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Extension of recommended cross section database for production of therapeutic isotopes

Abstract

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TALYS: modeling of nuclear reactions

EANM guidance document: dosimetry for first-in-human studies and early phase clinical trials

Discussion of the evaluated nuclear reactions

Production of 47Sc

Evaluated nuclear reactions for 47Ca and 47Sc formation

natV(p,x)47Ca

natV(p,x)47Sc

natV(d,x)47Ca

natV(d,x)47Sc

natTi(p,x)47Ca

natTi(p,x)47Sc

natTi(d,x)47Sc

48Ti(p,x)47Sc

48Ca(p,2n)47Sc

Integral yields for 47Ca and 47Sc formation

Production of 58mCo

Evaluated nuclear reactions for 58mCo formation

58Fe(p,n)58mCo

55Mn(α,n)58mCo

Integral yields for 58mCo formation

71Ge production

Evaluated nuclear reactions for 71As and 71Ge formation

68Zn(α,n) 71Ge

natGa(α,x)71As

natGe(p,xn)71As

natGe(d,x)71As

70Ge(d,n)71As

72Ge(p,2n)71As

Integral yields for 71As and 71Ge formation

Production of 77Br

Evaluated nuclear reactions for 77Kr and 77Br formation

77Se(p,n)77Br

78Se(p,2n)77Br

79Br(p,3n)77Kr

75As(α,2n)77Br

natKr(p,x)77Br

Integral yields for 77Kr and 77Br formation

80mBr production

Evaluated nuclear reactions for 80mBr formation

80Se(p,n)80mBr

natSe(d,xn)80mBr

natSe(p,x)80mBr

80Se(d,2n)80mBr

natSe(α,x)80mBr

Integral yields for 80mBr formation

103Pd and 103Ru production

Evaluated nuclear reactions for 103Ru and 103Pd formation

natAg(p,x)103Pd

natRu(p,x)103Ru

natRu(d,x)103Ru

100Mo(α,n)103Ru

Integral yields for 103Pd and 103Ru formation

105Rh production

Evaluated nuclear reaction for 105Rh formation

104Ru(d,n)105Rh

Integral yields for 105Rh formation

117mSn production

Evaluated nuclear reactions for 117mSn formation

114Cd(α,n)117mSn

116Cd(α,3n)117mSn

natCd(α,xn)117mSn

115In(α,pn)117mSn

natSb(p,x)117mSn

Integral yields for 117mSn formation

119Sb production

Evaluated nuclear reactions for 119mTe and 119Sb formation

119Sn(p,n)119Sb

natSb(p,xn)119mTe

Integral yields for 119Sb and 139Te formation

134Ce/134La production

Evaluated nuclear reaction for 134Ce formation

139La(p,6n)134Ce

Integral yields for 134Ce formation

135La production

Evaluated nuclear reaction for 135La formation

natBa(p,xn)135La

Production of ⁴⁷Sc

Evaluated nuclear reactions for ⁴⁷Ca and ⁴⁷Sc formation

^natV(p,x)⁴⁷Ca

^natV(p,x)⁴⁷Sc

^natV(d,x)⁴⁷Ca

^natV(d,x)⁴⁷Sc

^natTi(p,x)⁴⁷Ca

^natTi(p,x)⁴⁷Sc

^natTi(d,x)⁴⁷Sc

⁴⁸Ti(p,x)⁴⁷Sc

⁴⁸Ca(p,2n)⁴⁷Sc

Integral yields for ⁴⁷Ca and ⁴⁷Sc formation

Production of ^58mCo

Evaluated nuclear reactions for ^58mCo formation

⁵⁸Fe(p,n)^58mCo

⁵⁵Mn(α,n)^58mCo

Integral yields for ^58mCo formation

⁷¹Ge production

Evaluated nuclear reactions for ⁷¹As and ⁷¹Ge formation

⁶⁸Zn(α,n) ⁷¹Ge

^natGa(α,x)⁷¹As

^natGe(p,xn)⁷¹As

^natGe(d,x)⁷¹As

⁷⁰Ge(d,n)⁷¹As

⁷²Ge(p,2n)⁷¹As

Integral yields for ⁷¹As and ⁷¹Ge formation

Production of ⁷⁷Br

Evaluated nuclear reactions for ⁷⁷Kr and ⁷⁷Br formation

⁷⁷Se(p,n)⁷⁷Br

⁷⁸Se(p,2n)⁷⁷Br

⁷⁹Br(p,3n)⁷⁷Kr

⁷⁵As(α,2n)⁷⁷Br

^natKr(p,x)⁷⁷Br

Integral yields for ⁷⁷Kr and ⁷⁷Br formation

^80mBr production

Evaluated nuclear reactions for ^80mBr formation

⁸⁰Se(p,n)^80mBr

^natSe(d,xn)^80mBr

^natSe(p,x)^80mBr

⁸⁰Se(d,2n)^80mBr

^natSe(α,x)^80mBr

Integral yields for ^80mBr formation

¹⁰³Pd and ¹⁰³Ru production

Evaluated nuclear reactions for ¹⁰³Ru and ¹⁰³Pd formation

^natAg(p,x)¹⁰³Pd

^natRu(p,x)¹⁰³Ru

^natRu(d,x)¹⁰³Ru

¹⁰⁰Mo(α,n)¹⁰³Ru

Integral yields for ¹⁰³Pd and ¹⁰³Ru formation

¹⁰⁵Rh production

Evaluated nuclear reaction for ¹⁰⁵Rh formation

¹⁰⁴Ru(d,n)¹⁰⁵Rh

Integral yields for ¹⁰⁵Rh formation

^117mSn production

Evaluated nuclear reactions for ^117mSn formation

¹¹⁴Cd(α,n)^117mSn

¹¹⁶Cd(α,3n)^117mSn

^natCd(α,xn)^117mSn

¹¹⁵In(α,pn)^117mSn

^natSb(p,x)^117mSn

Integral yields for ^117mSn formation

¹¹⁹Sb production

Evaluated nuclear reactions for ^119mTe and ¹¹⁹Sb formation

¹¹⁹Sn(p,n)¹¹⁹Sb

^natSb(p,xn)^119mTe

Integral yields for ¹¹⁹Sb and ¹³⁹Te formation

¹³⁴Ce/¹³⁴La production

Evaluated nuclear reaction for ¹³⁴Ce formation

¹³⁹La(p,6n)¹³⁴Ce

Integral yields for ¹³⁴Ce formation

¹³⁵La production

Evaluated nuclear reaction for ¹³⁵La formation

^natBa(p,xn)¹³⁵La

Integral yields for ¹³⁵La formation

^149gTb production

Evaluated nuclear reaction for ¹⁴⁹ Tb formation

^natGd(p,xn)¹⁴⁹Tb

Integral yields for ¹⁴⁹Tb formation

¹⁶¹Tb production

Evaluated nuclear reaction for ¹⁶¹ Tb formation