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Activation cross sections of deuteron induced reactions on natHf in the 12–50 MeV energy range
Nuclear Inst. and Methods in Physics Research B 441 (2019) 93–101
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Activation cross sections of deuteron induced reactions on 12–50 MeV energy range
nat
Hf in the
T
F. Tárkányia, A. Hermanneb, F. Ditróia, , S. Takácsa, A.V. Ignatyukc ⁎
a
Institute for Nuclear Research, Hungarian Academy of Sciences (ATOMKI), Debrecen, Hungary Cyclotron Laboratory, Vrije Universiteit Brussel (VUB), Brussels, Belgium c Institute of Physics and Power Engineering (IPPE), Obninsk 249020, Russia b
ARTICLE INFO
ABSTRACT
Keywords: Deuteron irradiation Stacked foil technique Ta, Hf, Lu and Yb radioisotopes Cross section Thick target yield Theoretical model codes
As a part of our systematical study of activation cross sections of deuteron induced nuclear reactions, cross sections on hafnium were investigated up to 50 MeV. Excitation functions were measured for the natHf (d,xn)178g,177,176,175,173Ta, natHf(d,x)181,180m,179m2,175,173,172Hf, natHf(d,x)173,172,171,170Lu and natHf(d,x)169Yb reactions by using the activation method, stacked foil irradiation technique and off-line gamma-ray spectrometry for quantification of the produced radionuclides. The experimental results are compared with the earlier results in the overlapping energy range, and with the theoretical predictions of the ALICE IPPE-D and EMPIRE II-D theoretical codes and with values reported in the TENDL-2017 on-line library obtained with the TALYS code.
1. Introduction Systematic measurements of activation cross sections of deuteron induced nuclear reactions are in progress up to 50 MeV deuteron energy for practical applications and to test nuclear reaction models. The status of the database for deuteron induced reactions was relatively poor compared to what is available for proton induced reactions, and the quality of the theoretical descriptions, even after several attempts for improvement, does not allow reliable estimation of the cross sections in many cases. In the present work we report our new data on deuteron induced reaction on natHf up to 50 MeV incident particle energy. Hafnium is essential in different aspects of aerospace, nuclear energy (control rods) and opto-electronics industry [1,2]. In most of these applications reliable activation cross section data are useful. They are also of interest for production of the medically relevant radionuclides 169 Yb, 177Lu, 179Lu 177Ta, 178gTa and for 172Hf/172Lu, 173Lu, 179Ta radioisotopes used in industrial measurement instruments. We investigated the production of the above listed isotopes by using proton and deuteron induced reactions on tungsten [3–5], tantalum [6], hafnium [7] lutetium [6,8], ytterbium [9–11], thulium [12–14] and alpha particle induced reactions on erbium [15,16] and ytterbium [16–18]. For deuteron induced reactions on hafnium only three sets of experimental activation cross section or production yields are available in
⁎
the literature, all of them below 22 MeV. Our cross section data measured earlier up to 20 MeV were reported by Takacs et al. 2010 [19] (corrected in Takacs et al. 2012 [20]) for production of 174,175,176,177,178m,180gTa, 173,175,179m2,180m,181Hf and 177g,179 Lu radioisotopes; Cross sections up to 16 MeV for production of 177Ta were measured by Simonelli et al. 2012 [21]; Thick target yield data for formation of 176,178Ta and 175Hf radionuclides at 22-MeV deuteron energy were reported by Dmitriev et al. 1982 [22]. 2. Experiment and data evaluation The experimental cross sections were determined by using the activation method, stacked foil irradiation technique and off-line gamma ray spectrometry for quantification of the produced radionuclides. Cross-section data were deduced relative to the recommended excitation functions of the 27Al(d,x)22,24Na monitor reactions [23] re-measured over the whole covered energy range. The irradiation was made at an external beam line of the Cyclone 90 cyclotron of the Université Catholique in Louvain la Neuve (LLN). The irradiation time was 60 min with a 50 MeV extracted deuteron beam of 100 nA nominal intensity. The targets were irradiated in a short Faraday cup. The irradiated stack contained a sequence of 7 sections consisting of
Corresponding author. E-mail address: [email protected] (F. Ditrói).
https://doi.org/10.1016/j.nimb.2019.01.005 Received 6 November 2018; Received in revised form 20 December 2018; Accepted 7 January 2019 0168-583X/ © 2019 Elsevier B.V. All rights reserved.
Nuclear Inst. and Methods in Physics Research B 441 (2019) 93–101
F. Tárkányi et al.
Table 1 (continued)
Table 1 Decay characteristics of the investigated reaction products and Q-values of reactions for their productions. Nuclide (Level) Decay
Half-life
178g
2.36 h
Ta ε: 100%
177
Ta ε: 100%
176
56.56 h
Iγ (%)
Contributing reaction
Q-value (keV)
213.440 325.562 331.613 426.383
81.4 94.1 31.19 97.0
177
Hf(d,n) Hf(d,2n) 179 Hf(d,3n) 180 Hf(d,4n)
2782.4 −4844.1 −10943.1 −18330.9
112.9 208.4
7.2 0.94
176
Hf(d,n) Hf(d,2n) 178 Hf(d,3n) 179 Hf(d,4n) 180 Hf(d,5n)
2202.69 −4172.91 −11798.84 −17897.84 −25285.59
178
177
5.7 2.4 5.4 24.7 5.7
176
Hf(d,2n) Hf(d,3n) Hf(d,4n) 179 Hf(d,5n) 180 Hf(d,6n)
−6217.9 −12593.5 −20219.4 −26318.4 −33706.2
207.4 266.9 348.5 998.3
14.0 11.24 12.0 2.6
174
Hf(d,n) Hf(d,3n) Hf(d,4n) 178 Hf(d,5n) 179 Hf(d,6n) 180 Hf(d,7n)
1628.6 −13245.9 −19621.5 −27247.5 −33346.4 −40734.2
3.14 h
160.4 172.2 180.6 1030.0 1208.2
4.9 17.5 2.22 1.42 2.7
174
Hf(d,3n) Hf(d,5n) 177 Hf(d,6n) 178 Hf(d,7n) 179 Hf(d,8n)
−14526.2 −29400.6 −35776.3 −43402.2 −49501.2
42.39 d
133.021 136.260 345.93 482.18
43.3 5.85 15.12 80.5
180
3470.234
−2224.566
5401.374 −2224.566 −9612.32
8.09 h
175
Ta ε: 100%
10.5 h
173
Ta ε: 100%
181
β-: 100%
177 178
176 177
176
Hf(d, p)
180m
Hf 1141.729 keV IT: 100%
5.53 h
215.426 332.274 443.162 500.697
81.6 94 81.7 14.2
180
179m2
Hf 1105.74 keV IT: 100%
25.05 d
122.70 146.15 169.78 192.66 217.04 236.48 268.85 315.93 362.55 409.72 453.59
27.7 27.1 19.4 21.5 9.0 18.8 11.3 20.3 39.6 21.5 68
177
175
Hf ε: 100%
70 d
343.40 433.0
84 1.44
174
Hf(d,p) Hf(d,p2n) 177 Hf(d,p3n) 178 Hf(d,p4n) 179 Hf(d,p5n) 180 Hf(d,p6n) 175 Ta decay
4483.934 −10390.54 −16766.16 −24392.1 −30491.09 −37878.85 1628.6
173
Hf ε: 100%
23.6 h
123.675 139.635 296.974 311.239
83 12.7 33.9 10.7
174
Hf(d,p2n) Hf(d,p4n) 177 Hf(d,p5n) 178 Hf(d,p6n) 179 Hf(d,p7n) 173 Ta decay
−10728.6 −25603.1 −31978.7 −39604.6 −45703.6 −14526.2
172
Hf ε: 100%
1.87 y
114.061 122.916 125.812 127.91
2.6 1.14 11.3 1.46
174
Hf(d,p3n) Hf(d,p5n) 177 Hf(d,p6n) 178 Hf(d,p7n) 172 Ta decay
−17809.5 −32683.9 −39059.6 −46685.5 −23664.1
173
1.37 y
171.393 272.105
2.90 21.2
174
−8477.1 −23351.58 −29727.2 −37353.13 −43452.12
Lu ε: 100%
Hf(d,pn)
Hf(d,p) Hf(d,pn) Hf(d,p2n)
179 180
176
176
176
Hf(d,2pn) Hf(d,2p3n) 177 Hf(d,2p4n) 178 Hf(d,2p5n) 179 Hf(d,2p6n) 176
Half-life
Eγ (keV)
Iγ (%)
Contributing reaction
Q-value (keV)
180
Hf(d,2p7n) Hf decay
−50839.88 −14526.2
173
201.84 521.6 710.50 1159.30 201.84
Ta ε: 100%
Hf
Eγ (keV)
Nuclide (Level) Decay
172g
181.525 810.064 900.724 912.079 1093.63
20.6 16.6 29.8 15.3 63
174
Hf(d,2p2n) Hf(d,2p4n) Hf(d,2p5n) 178 Hf(d,2p6n) 172 Hf decay
−16693.35 −31567.83 −37943.45 −45569.39 −17809.5
8.24 d
667.422 739.793 780.711 839.961
11.1 47.9 4.37 3.05
174
Hf(d,2p3n) Hf(d,2p5n) 177 Hf(d,2p6n) 171 Hf decay
−23672.25 −38546.74 −44922.36 −26851.7
Lu ε: 100%
2.012 d
938.75 985.10 987.25 1003.20 1225.65
1.57 5.4 1.65 3.44 4.83
174
Hf(d,2p4n) Hf(d,2p6n) 170 Hf decay
−32265.7 −47140.2 −34100.5
169
32.018 d
109.77924 130.52293 177.21307 197.95675 307.73586
17.39 11.38 22.28 35.93 10.35
174
−36483.38 −43708.7
Lu ε: 100%
6.70 d
171
Lu ε: 100%
170
Yb ε: 100%
176 177
176
176
169
Hf(d,3p4n) Lu decay
Abundance of isotopes in natural Hf -%: 174Hf-0.162, 176Hf-5.206, 177Hf-18.60, 178 Hf-27.30, 179Hf-13.63, 180Hf-35.10. The Q-values shown in Table 1 refer to formation of the ground state. Decrease Q-values for isomeric states with level energy of the isomer. Increase the Q-values if compound particles are emitted by: pn → d + 2.2 MeV, p2n → t + 8.5 MeV, 2pn → 3He + 7.7 MeV, 2p2n → α + 28.3 MeV.
Hf (10.54 μm), Al (49.54 μm), Al (49.54 μm), Pt (19.29 μm), Al (49.54 μm), Al (49.54 μm), CuMnNi alloy (24.73 μm), Al (49.54 μm), Al (49.54 μm) followed by 13 sections of Hf (10.54 μm) Al (10.85 μm), Al (49.54 μm), CuMnNi alloy (24.73 μm) and Al (10.85 μm). The 20 Hf targets covered the 50–12 MeV energy range. Gamma-ray spectra were measured at HpGe detectors in the cyclotron laboratory of VUB (Brussels). Four series of gamma-ray spectra were measured to follow the decay. These four series started between 7.9 and 10.3 h, 32.9 and 69.4 h, 126.8 and 194.5 h as well as 2166.3 and 2736.7 h after end of bombardment, respectively. Gamma spectra were evaluated by the automatic fitting algorithm included in the Genie 2000 package or in an iterative process using the Forgamma [24,25] code. For data evaluation NUDAT2.7 [26] and in case of 178Ta the Lund/ LBNL Nuclear Data [27] libraries were used (Table 1). As natural Hf consists of 6 stable isotopes, only the so called elemental cross-sections were determined over the entire energy range except for one reaction where only a single target isotope is contributing. The Q values of the contributing reactions (Q value calculator [28]) are also shown in Table 1 to indicate the reaction thresholds. Uncertainty of the measured cross-sections, estimated to be between 10 and 22%, was determined according to the recommendations in [29] by taking the sum in quadrature of all individual linear contributions: beam current (7%), target thickness or homogeneity (5%), detector efficiency (5%), photo peak area determination and counting statistics (1–20%). For preparation of the stack composition and of the irradiation parameters, the median energy in each of the target foils was obtained by a degradation calculation based on the calibrated primary beam energy and the stopping powers based on Anderson and Ziegler formula [30]. Final energy correction was applied based on the results of the fitted monitor reactions over the whole energy range (Tarkanyi et al. 1991 [31]), shown in Fig. 1. Only small correction was needed on the beam intensity and the energy degradation. Uncertainty of energy was estimated by taking into account cumulative effects on the energy 94
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Table 2 Experimental cross sections for the 178g
Fig. 1. Agreement of simultaneously measured experimental data of 27Al (d,x)22,24Na monitor reactions in comparison with the recommended values to monitor of the deuteron beam parameters through the irradiated stacks.
degradation (primary energy, target thickness, energy straggling) and the applied correction to monitor reaction. Due to the experimental circumstances (stacked foil technique, high dose to personnel at EOB, limited detector capacity, long cooling time before the first series of gamma spectra measurements) no cross section data were obtained for short lived (T1/2 < 2 h) activation products.
nat
177
Ta
Hf(d,xn)178g,177g,176,175g,173Ta reactions. 176
Ta
175
Ta
173
Ta
Ta
E
ΔE
σ
Δσ
σ
Δσ
σ
Δσ
σ
Δσ
σ
Δσ
MeV 49.2 47.1 45.0 42.8 40.5 38.1 35.6 33.2 31.8 30.4 28.9 27.4 25.8 24.2 22.4 20.6 18.6 16.5 14.2 11.5
0.3 0.3 0.4 0.4 0.4 0.5 0.5 0.6 0.6 0.7 0.8 0.9 0.9 1.0 1.1 1.3 1.4 1.5 1.7 1.8
mb 44.5 48.9 64.9 85.6 83.5 87.3 116.3 190.5 203.2 226.8 155.5 193.0 130.8 132.8 91.2 64.6 78.2 61.6 32.3 13.3
5.4 5.9 7.8 10.2 10.0 10.4 13.9 22.7 24.3 27.1 18.6 23.0 15.6 15.9 10.9 7.7 9.4 7.4 3.9 1.7
190.3 245.5 336.3 431.1 372.2 286.8 264.5 260.3 276.6 276.7 224.3 350.4 269.6 350.2 292.3 217.2 249.3 175.2 90.5 40.9
22.8 29.3 40.1 51.4 44.4 34.2 31.6 31.0 33.0 33.0 26.8 41.8 32.2 41.8 34.9 25.9 29.7 20.9 10.8 4.9
267.2 262.7 308.7 316.9 261.7 219.5 234.4 253.2 319.8 332.6 242.8 313.2 207.6 213.4 185.5 125.5 126.4 59.3 33.7 14.2
32.5 32.4 38.1 39.4 32.7 28.1 29.6 34.6 38.7 40.3 29.5 38.3 25.2 26.0 22.6 15.7 15.6 7.8 4.1 1.7
271.5 308.0 377.4 426.7 325.5 240.6 214.1 215.5 227.1 225.6 148.0 181.8 96.9 81.5 55.1 36.1 24.6 8.9 2.2 1.8
32.4 36.8 45.1 51.0 38.9 28.8 25.6 26.0 27.1 27.0 17.7 21.8 11.6 9.8 6.7 4.4 3.0 1.2 0.3 0.2
72.8 50.8 52.5 32.3 14.9 7.5
8.9 6.6 6.5 4.2 3.0 1.0
Simonelli et al. [21] (Fig. 3). According to the new unpublished evaluated value for gamma-intensity of 208 keV by Kondev (private communication in [38]), all experimental data should be divided by a factor of 1.49 in the case if the new intensities are confirmed.
3. Comparison with nuclear model calculations
4.1.3. natHf(d,x)176Ta reaction The new experimental data for production of 176Ta (2.36 h) are in good agreement with the earlier low energy data [19]. The results of the reaction codes show different shapes and only TENDL-2017 describes approximately well the experimental excitation curve (Fig. 4).
The cross-sections of the investigated reactions were compared with the data given in the on-line TENDL-2017 library [32]. This library is based on both default and adjusted TALYS (1.9) calculations (Koning and Rochman, 2012 [33]). The cross sections of the investigated reactions were also compared with results of our calculations using ALICE-IPPE (Dityuk et al., 1998 [34]) and EMPIRE-II (Herman et al., 2008 [35]) codes modified for deuterons (D versions) by Ignatyuk, 2010–2011 [36,37]. To achieve a better description of available data for (d,p) reactions in these codes a phenomenological energy dependent enhancement factor was introduced on the basis of the observed (d,p) cross sections for medium and heavy nuclei. By this improvement, the direct (d,p) channel is increased strongly and this is reflected in changes for all other reaction channels. As ALICE-IPPE calculates only the total cross section, for estimation of isomeric state cross sections with the ALICE code the isomeric ratios obtained from EMPIRE-D were used.
4.1.4. natHf(p,x)175Ta reaction The new data are, similarly to the previous reactions, a little lower when compared to our earlier data [19] measured up to 20 MeV (Fig. 5). The shapes and the values of the experimental and theoretical excitation functions are different above 30 MeV, with TENDL-2017 giving a reasonable agreement. 4.1.5. natHf(d,x)173Ta reaction No earlier experimental data exist for production of 173Ta (3.14 h). The theoretical cross sections TENDL, ALICE and EMPIRE give higher estimations than our new experimental results (Fig. 6). 4.1.6. 180Hf(d,p)181Hf The 181Hf (42.39 d) is produced only via (d,p) reaction on 180Hf and the reaction cross sections are shown in Fig. 7. There was an extra hafnium foil placed out of the range of the bombarding beam into the stack (at least below the threshold of the natHf(d,x)181Hf) and no 181Hf contribution was found in this foil, indicating negligible contribution of the secondary neutron reactions. The agreement with the earlier low energy data [19] is acceptable. Significant underestimation for all model codes can be observed (Fig. 6).
4. Results and discussion 4.1. Excitation functions The measured cross sections for the natHf(d,xn)178g,177,176,175,173Ta, 173,172,171,170 nat Hf(d,x)181,180m,179m2,175,173,172Hf, Lu and Hf 169 (d,x) Yb reactions are shown in Tables 2–4 and in Figs. 2–17. The figures also show the earlier reported data and the theoretical results.
nat
4.1.1. natHf(p,x)178gTa reaction The 9.31 min meta- and 2.36 h ground-states of 178Ta are decaying independently. Our new data for 178gTa formation are in agreement with the low energy data [19] in the overlapping energy range (Fig. 2). All model codes overestimate significantly the experimental data.
4.1.7. natHf(d,x)180mHf The isotope 180Hf has a stable ground state and a 180mHf (5.53 h) isomeric state, which is produced directly by deuteron bombardment of Hf. The neighboring isobars 180Ta (EC) and the 180Lu (β−) are decaying only to the 180gHf ground state. The agreement with our earlier reported low energy data [19] is good. The results of the theoretical codes are disagreeing, probably because of different estimations of isomeric ratios: TENDL-2017 presents some overestimation, while ALICE-D and
4.1.2. natHf(d,x)177Ta reaction Our data for production of 177Ta (56.56 h) are in good agreement with the earlier experimental data of Takacs et al. [19,20] and of 95
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Table 3 Experimental cross sections for the 181
nat
Hf(d,x)181,180m,179m2,175,173,172Hf reactions. 180m
Hf
179m2
Hf
175
Hf
173
Hf
172
Hf
Hf
E
ΔE
σ
Δσ
σ
Δσ
σ
Δσ
σ
Δσ
σ
Δσ
σ
Δσ
MeV 49.2 47.1 45.0 42.8 40.5 38.1 35.6 33.2 31.8 30.4 28.9 27.4 25.8 24.2 22.4 20.6 18.6 16.5 14.2 11.5
0.3 0.3 0.4 0.4 0.4 0.5 0.5 0.6 0.6 0.7 0.8 0.9 0.9 1.0 1.1 1.3 1.4 1.5 1.7 1.8
mb 20.7 23.5 31.3 40.7 37.5 32.0 38.8 54.2 58.9 72.9 53.5 87.3 70.4 101.6 103.9 95.4 143.4 159.4 163.8 196.6
2.5 2.8 3.7 4.9 4.5 3.8 4.6 6.5 7.0 8.7 6.4 10.4 8.4 12.1 12.4 11.4 17.1 19.0 19.5 23.4
2.6 2.2 4.6 3.8 5.3 4.3
0.8 0.7 0.7 1.0 1.0 0.9
413.0 440.0 532.6 605.3 454.9 314.8 289.0 306.6 284.1 292.6 177.9 216.2 115.5 96.3 61.9 41.4 26.9 5.8 1.4 1.3
49.2 52.4 63.5 72.1 54.2 37.5 34.4 36.5 33.9 34.9 21.2 25.8 13.8 11.5 7.4 4.9 3.2 0.7 0.2 0.2
13.4 10.7 9.0 7.5 3.8 1.1
13.8 9.8 9.7 6.0
1.8 1.9 1.3 1.2
7.1
1.2
1.0 0.7 0.9 0.9 1.2 0.6 1.1 0.7 0.5 0.7 0.5 0.3 0.2
0.4 0.4 0.5 0.6 0.6 0.4 0.4 0.5 0.4 0.4 0.3 0.3 0.2 0.2 0.2 0.1 0.1 0.1
112.4 89.6 75.2 61.9 30.5 6.9
5.0 4.6 6.7 4.1 7.0 3.7 6.6 4.7 3.1 3.8 2.2 1.4 1.4
3.1 3.1 4.1 4.7 4.5 2.9 3.0 3.6 3.2 3.3 2.0 2.2 1.5 1.8 1.2 0.8 0.6 0.2
1.6 3.2
0.7 0.7
1.9
0.7
2.5 3.8 5.5
0.5 0.7 0.9
4.6 2.6
1.1 0.7
3.6
0.6
1.2
0.4
1.5
0.5
Table 4 Experimental cross sections for the 173
172
Lu
E
ΔE
MeV 49.2 47.1 45.0 42.8 40.5 38.1 35.6 33.2 31.8 30.4 28.9 27.4 25.8 24.2 22.4 20.6 18.6 16.5 14.2 11.5
0.3 0.3 0.4 0.4 0.4 0.5 0.5 0.6 0.6 0.7 0.8 0.9 0.9 1.0 1.1 1.3 1.4 1.5 1.7 1.8
173,172,171
Lu and
nat
Hf(d,x)169Yb reactions.
171
Lu
169
Lu
Yb
σ
Δσ
σ
Δσ
σ
Δσ
σ
Δσ
mb 106.4 88.0 83.9 74.7 43.8 22.8 16.6 17.3 15.6 18.5 12.5 17.6 12.1 13.7 11.1 7.4 8.9 7.3
12.7 10.5 10.0 8.9 5.2 2.8 2.0 2.1 1.9 2.2 1.5 2.1 1.5 1.7 1.4 0.9 1.1 0.9
5.9 5.5 5.7 5.2 3.4 1.9
0.7 0.7 0.7 0.6 0.4 0.2
5.1 4.3 3.8 3.4 0.5
0.6 0.5 0.5 0.4 0.1
33.4 26.4 24.7 18.5 8.9
4.1 3.2 3.0 2.3 1.2
1.3 0.9 0.9 0.4 0.4
0.2 0.1 0.1 0.1 0.1
0.1
0.0
Fig. 2. Experimental and theoretical cross sections for the formation of by deuteron bombardment of hafnium.
178g
Ta
EMPIRE-D are nearly equal and underestimate by a factor of 3 (Fig. 8). 4.1.8. natHf(d,x)179m2Hf reaction The isotope 179Hf has a stable ground-state and two isomeric states: a short-lived 179m1Hf (18.67 s) lower lying state and the longer-lived 179m2 Hf (25.05 d) higher energy isomeric state. We can deduce cross sections for this second isomeric state, which is produced only directly. There is no contribution from the neighboring isobars 179Lu (4.59 h) and 179Ta (1.82 y) in production of 179m2Hf. The agreement with our earlier reported low energy data [19] is good. There is large disagreement with the TENDL-2017 data (a factor of 2), the agreement with the ALICE-D and EMPIRE-D calculations is acceptable up to 40 MeV (Fig. 9).
Fig. 3. Experimental and theoretical cross sections for the formation of 177Ta by deuteron bombardment of hafnium.
4.1.9. natHf(d,x)175Hf(cum) reaction The measured cross section of 175Hf (70 d) is cumulative, measured 96
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Fig. 7. Experimental and theoretical cross sections for the clear reaction.
Fig. 4. Experimental and theoretical cross sections for the formation of 176Ta by deuteron bombardment of hafnium.
180
Hf(d,p)181Hf nu-
Fig. 8. Experimental and theoretical cross sections for the formation of by deuteron bombardment of hafnium.
Fig. 5. Experimental and theoretical cross sections for the formation of 175Ta by deuteron bombardment of hafnium.
180m
Hf
Fig. 9. Experimental and theoretical cross sections for the formation of 179m2Hf by deuteron bombardment of hafnium.
Fig. 6. Experimental and theoretical cross sections for the formation of 173Ta by deuteron bombardment of hafnium.
4.1.10. natHf(d,x)173Hf(cum) reaction The measured cumulative cross sections of 173Hf (23.6 h) include the decay of parent 173Ta (3.14 h, ε: 100%). The new results are in good agreement with the earlier measured low energy data [19] and also with results of TENDL and EMPIRE theoretical codes (Fig. 11).
after the “complete” decay of 175Ta (10.5 h, ε: 100%) (Fig. 10). The agreement with the low energy data [19] and with the theoretical predictions is acceptable. The contribution of secondary neutrons was neglected as described by the 181Hf case. 97
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Fig. 10. Experimental and theoretical cross sections for the formation of by deuteron bombardment of hafnium.
175
Fig. 13. Experimental and theoretical cross sections for the formation of by deuteron bombardment of hafnium.
173
Fig. 11. Experimental and theoretical cross sections for the formation of by deuteron bombardment of hafnium.
173
Fig. 14. Experimental and theoretical cross sections for the formation of by deuteron bombardment of hafnium.
172
Fig. 12. Experimental and theoretical cross sections for the formation of by deuteron bombardment of hafnium.
172
Fig. 15. Experimental and theoretical cross sections for the formation of by deuteron bombardment of hafnium.
171
Hf
Hf
Hf
Lu
Lu
Lu
4.1.12. natHf(d,x)173Lu(cum) reaction The measured cross sections of 173Lu (1.37 y) are cumulative, including the contributions from the 173Ta (3.14 h) → 173Hf (23.6 h) parent decay chain (Fig. 13). The experimental data are lower than the model predictions above 35 MeV. No earlier results are known for
4.1.11. natHf(d,x)172Hf(cum) reaction The 172Hf (1.87 y) is produced directly and through the decay of short-lived parent 172Ta (36.8 min). The comparison of the measured cumulative cross sections with the theory are shown in Fig. 12 (no earlier experimental results). 98
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Fig. 16. Experimental and theoretical cross sections for the formation of by the deuteron bombardment of hafnium.
170
Fig. 18. Integral thick target yields for the formation of the investigated radioisotopes of tantalum as a function of incident energy.
Lu
energy shifts of 5 MeV between them. 4.1.16. natHf(d,x)169Yb(cum) reaction The cross sections for production of 169Yb (32.018 d) were obtained from the gamma-spectra measured after nearly complete decay of the 169 Ta (4.9 min) → 169Hf (3.24 min) → 169Lu (34.06 h) → 169Yb parent decay chain (Fig. 17). The experimental data are much higher than the predictions of the theoretical codes, for which no proper explanation has been found yet. 5. Integral yields
Fig. 17. Experimental and theoretical cross sections for the formation of by the deuteron bombardment of hafnium.
The so-called physical integral yield ([Bonardi 1988 [39], Otuka 2015 [40]) was calculated from a spline fit to our earlier and recently measured experimental excitation functions and are shown in Figs. 18–20, respectively. For comparison only one experimental data point at 22 MeV was found, measured by Dmitriev et al. (1982), for the natHf(d,x)176,178Ta and 175Hf reactions [22]. As seen from Fig. 18 the earlier data of Dmitriev [22] for the single 22 MeV point are significantly lower in the case of 178gTa and significantly larger in the case of 176Ta than our new calculated yields. The largest thick targets yields can be observed by the 178g,176Ta radioisotopes, where considerable yield is expected even by lower
169
Yb
production of radioisotopes of lutetium. 4.1.13. natHf(d,x)172Lu(cum) reaction The measured cross section of 172Lu (6.70 d) includes the contribution from the decay of the short-lived 172mLu isomeric state (3.7 min, IT 100%) (Fig. 14). The cross section of the ground state was deduced from the measured gamma-spectra, where the contribution of the possible parent 172Hf (1.87 y) could be neglected. The rate of increase for the theoretical codes is different between TENDL-2017 and the two other codes and is clearly sharper than what is experimentally seen. 4.1.14. natHf(d,x)171Lu(cum) reaction The measured cumulative cross sections of 171Lu (8.24 d) include the contribution from the decay of the 171Ta (23.3 min) → 171Hf (12.2 h) → 171Lu decay chain (Fig. 15). The experimental data are significantly lower than the results of the theoretical codes that show different rates of increase above 40 MeV. 4.1.15. natHf(d,x)170Lu(cum) reaction The single cumulative cross section point of 170Lu (2.012 d) (1.62 ± 0.60 mb at 49.2 MeV) (Fig. 16) was deduced from the gammaspectra measured after the complete decay of the 170Ta (6.76 min) → 170 Hf (16 h) parent radioisotopes. Due to low statistics no other reliable data points could be re-produced. The results of the three codes show
Fig. 19. Integral thick target yields for the formation of the investigated radioisotopes of hafnium as a function of the energy. 99
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[2] J.N.A. Matthews, Semiconductor industry switches to hafnium-based transistors, Phys. Today 61 (2008) 25. [3] F. Tárkányi, S. Takács, F. Szelecsényi, F. Ditrói, A. Hermanne, M. Sonck, Excitation functions of deuteron induced nuclear reactions on natural tungsten up to 50 MeV, Nucl. Instrum. Methods Phys. Res., Sect. B 211 (2003) 319–330. [4] F. Tárkányi, S. Takács, F. Szelecsényi, F. Ditrói, A. Hermanne, M. Sonck, Excitation functions of proton induced nuclear reactions on natural tungsten up to 34 MeV, Nucl. Instrum. Methods Phys. Res., Sect. B 252 (2006) 160–174. [5] F. Tárkányi, F. Ditrói, S. Takács, A. Hermanne, New measurements of excitation functions of 186W(p,x) nuclear reactions up to 65 MeV. Production of a 178W/ 178mTa generator, Nucl. Instrum. Methods Phys. Res., Sect. B 391 (2017) 27–37. [6] F. Tarkanyi, S. Takacs, F. Ditroi, A. Hermanne, A.V. Ignatyuk, M.S. Uddin, Activation cross sections of alpha-particle induced nuclear reactions on hafnium and deuteron induced nuclear reaction on tantalum: Production of W-178/Ta-178m generator, Appl. Radiat. Isot. 91 (2014) 114–125. [7] S. Takács, F. Tárkányi, A. Hermanne, R.A. Rebeles, Activation cross sections of proton induced nuclear reactions on natural hafnium, Nucl. Instrum. Methods Phys. Res., Sect. B 269 (2011) 2824–2834. [8] S. Takács, F. Tárkányi, A. Hermanne, A.-R. R., Investigation of cross sections of deuteron induced nuclear reactions on natural lutetium, in: International Conference on Radioanalytical and Nuclear Chemistry. RANC 2016, Springer, Budapest, Hungary, 2016, pp. 95. [9] F. Tárkányi, A. Hermanne, S. Takács, F. Ditrói, B. Király, H. Yamazaki, M. Baba, A. Mohammadi, A.V. Ignatyuk, Activation cross sections of proton induced nuclear reactions on ytterbium up to 70 MeV, Nucl. Instrum. Methods Phys. Res., Sect. B 267 (2009) 2789–2801. [10] F. Tárkányi, F. Ditrói, S. Takács, A. Hermanne, H. Yamazaki, M. Baba, A. Mohammadi, A.V. Ignatyuk, Activation cross-sections of longer lived products of deuteron induced nuclear reactions on ytterbium up to 40 MeV, Nucl. Instrum. Methods Phys. Res., Sect. B 304 (2013) 36–48. [11] F. Tárkányi, F. Ditrói, S. Takács, A. Hermanne, A.V. Ignatyuk, New data on activation cross section for deuteron induced reactions on ytterbium up to 50 MeV, Nucl. Instrum. Methods Phys. Res., Sect. B 336 (2014) 37–44. [12] F. Tárkányi, A. Hermanne, S. Takács, F. Ditrói, I. Spahn, A.V. Ignatyuk, Activation cross-sections of proton induced nuclear reactions on thulium in the 20–45 MeV energy range, Appl. Radiat. Isot. 70 (2012) 309–314. [13] I. Spahn, S. Takács, Y.N. Shubin, F. Tárkányi, H.H. Coenen, S.M. Qaim, Cross-section measurement of the Tm-169(p, n) reaction for the production of the therapeutic radionuclide Yb-169 and comparison with its reactor-based generation, Appl. Radiat. Isot. 63 (2005) 235–239. [14] F. Tárkányi, A. Hermanne, S. Takács, F. Ditrói, I. Spahn, S.F. Kovalev, A.V. Ignatyuk, S.M. Qaim, Activation cross sections of the Tm-169(d,2n) reaction for production of the therapeutic radionuclide Yb-169, Appl. Radiat. Isot. 65 (2007) 663–668. [15] B. Király, F. Tárkányi, S. Takács, A. Hermanne, S.F. Kovalev, A.V. Ignatyuk, Excitation functions of alpha-induced nuclear reactions on natural erbium, Nucl. Instrum. Methods Phys. Res., Sect. B 266 (2008) 549–554. [16] B. Király, F. Tárkányi, S. Takács, A. Hermanne, S.F. Kovalev, A.V. Ignatyuk, Excitation funcions of alpha-induced nuclear reactions on natural erbium and natural ytterbium targets, in: O. Bersillon, F. Gunsing, E. Bange (Eds.), International Conference on Nuclear Data for Science and Technology, EDP Sciences, Nice, France, 2008, pp. 1371–1374. [17] B. Király, F. Tárkányi, S. Takács, A. Hermanne, S.F. Kovalev, A.V. Ignatyuk, Excitation functions of alpha-particle induced nuclear reactions on natural ytterbium, Nucl. Instrum. Methods Phys. Res., Sect. B 266 (2008) 3919–3926. [18] F. Tárkányi, F. Ditrói, S. Takács, A. Hermanne, B. Király, Activation cross-section data for alpha-particle induced nuclear reactions on natural ytterbium for some longer lived radioisotopes, J. Radioanal. Nucl. Chem. 311 (2017) 1825–1829. [19] S. Takács, F. Tárkányi, A. Hermanne, R.A. Rebeles, Activation cross sections of deuteron-induced nuclear reactions on hafnium, Nucl. Instrum. Methods Phys. Res., Sect. B 268 (2010) 3443–3451. [20] S. Takács, F. Tárkányi, A. Hermanne, R.A. Rebeles, Activation cross sections of deuteron-induced nuclear reactions on hafnium (vol 268, pg 3443, 2010), Nucl. Instrum. Methods Phys. Res., Sect. B 281 (2012) 98–99. [21] F. Simonelli, K. Abbas, A. Bulgheroni, S. Pomme, T. Altzitzoglou, G. Suliman, Measurement of the Hf-nat(d, x)Ta-177 cross section and impact of erroneous gamma-ray intensities, Nucl. Instrum. Methods Phys. Res., Sect. B 285 (2012) 162–164. [22] P.P. Dmitriev, N.N. Krasnov, G.A. Molin, Radioactive nuclide yields for thick target at 22 MeV deuterons energy, Yadernie Konstanti 34 (1982) 38. [23] A. Hermanne, A.V. Ignatyuk, R. Capote, B.V. Carlson, J.W. Engle, M.A. Kellett, T. Kibedi, G. Kim, F.G. Kondev, M. Hussain, O. Lebeda, A. Luca, Y. Nagai, H. Naik, A.L. Nichols, F.M. Nortier, S.V. Suryanarayana, S. Takacs, F.T. Tarkanyi, M. Verpelli, Reference cross sections for charged-particle monitor reactions, Nucl. Data Sheets 148 (2018) 338–382. [24] Canberra, http://www.canberra.com/products/radiochemistry_lab/genie-2000software.asp., in, 2000. [25] G. Székely, Fgm – a flexible gamma-spectrum analysis program for a small computer, Comput. Phys. Commun. 34 (1985) 313–324. [26] NuDat, NuDat2 database (2.6), in, National Nuclear Data Center, Brookhaven National Laboratory, 2014. [27] S.Y.F. Chu, L.P. Ekström, R.B. Firestone, WWW Table of Radioactive Isotopes, version 2.1 http://ie.lbl.gov/toi/, in, 2004. [28] B. Pritychenko, A. Sonzogni, Q-value calculator, in: NNDC, Brookhaven National Laboratory, 2003. [29] International-Bureau-of-Weights-and-Measures, Guide to the Expression of
Fig. 20. Integral thick target yields for the formation of the investigated radioisotopes of lutetium and ytterbium as a function of the energy.
bombarding energies. The only earlier literature value for 175Hf in a single energy point is significantly larger than our new result. The yields are significantly lower than by Ta radioisotopes and only the 181,180mHf have reasonable yields under 10 MeV. There are no literature data for production of Lu and Yb radioisotopes. The calculated yields are even lower than in the above two cases and the production thresholds are definitively higher. Comparing the yield results of deuteron induced reactions on natural hafnium we can conclude that for the production of medically relevant radioisotopes there are competitive routes as far as the target element and bombarding particle regarded [41]. 6. Summary and conclusion We report experimental cross sections for the natHf (d,xn)178g,177,176,175,173Ta, natHf(d,x)181,180m,179m2,175,173,172Hf, 173,172, 171,170 Lu and natHf(d,x)169Yb reactions up to 50 MeV incident deuteron energy. The new results successfully complete the earlier experimental data published up to 22 MeV [19,20]. In most cases acceptable agreement was found with the literature values in the overlapping energy range. The experimental data were compared with the results of a priori model calculations performed with the EMPIRE-D, ALICE-IPPE-D and TALYS codes (available in TENDL-2017 on-line database). The descriptions of the shape and the absolute values of the excitation functions by the theoretical calculations is only partly successful, and despite upgrading of the codes still large disagreements were found for many cases. The obtained experimental data provide a basis for improved model calculations and for optimization of various applications connected to charged particle activation. Among the radioisotopes mentioned in the introduction with recently documented practical applications, the magnitude of deuteron induced reactions could be of significance for production of 177 Ta,178gTa,179Ta and 173Lu. Acknowledgement The authors acknowledge the support of the respective institutions and the accelerator staffs for providing the beam time and experimental facilities. References [1] R. Tricot, The metallurgy and functional properties of hafnium, J. Nucl. Mater. 189 (1992) 277–288.
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F. Tárkányi et al.
[30] [31] [32] [33] [34] [35]
Uncertainty in Measurement, 1st ed., International Organization for Standardization, Genève, Switzerland, 1993. H.H. Andersen, J.F. Ziegler, Hydrogen stopping powers and ranges in all elements. The stopping and ranges of ions in matter, Pergamon Press, New York, 1977 vol. 3. F. Tárkányi, F. Szelecsényi, S. Takács, Determination of effective bombarding energies and fluxes using improved stacked-foil technique, Acta Radiol. Suppl. 376 (1991) 72. A.J. Koning, D. Rochman, J.C. Sublet, TENDL-2017 TALYS-based evaluated nuclear data library, in, 2017. A.J. Koning, D. Rochman, Modern nuclear data evaluation with the TALYS code system, Nucl. Data Sheets 113 (2012) 2841. A.I. Dityuk, A.Y. Konobeyev, V.P. Lunev, Y.N. Shubin, New version of the advanced computer code ALICE-IPPE, in: INDC (CCP)-410, IAEA, Vienna, 1998. M. Herman, R. Capote, B.V. Carlson, P. Oblozinsky, M. Sin, A. Trkov, H. Wienke, V. Zerkin, EMPIRE: nuclear reaction model code system for data evaluation, Nucl. Data Sheets 108 (2007) 2655–2715.
[36] A.V. Ignatyuk, 2nd RCM on FENDL-3, in: IAEA, Vienna, Austria, 2010. [37] A.V. Ignatyuk, Phenomenological systematics of the (d,p) cross sections, http:// www-nds.iaea.org/fendl3/000pages/RCM3/slides//Ignatyuk_FENDL-3%20presentation.pdf, in: IAEA (Ed.), Vienna, 2011. [38] F.G. Kondev, Personal communicatiom, in, 2018. [39] M. Bonardi, The contribution to nuclear data for biomedical radioisotope production from the Milan cyclotron facility, in: K. Okamoto (Ed.) Consultants Meeting on Data Requirements for Medical Radioisotope Production, IAEA, INDC(NDS)-195 (1988), Tokyo, Japan, 1987, pp. 98–112. [40] N. Otuka, S. Takacs, Definitions of radioisotope thick target yields, Radiochim. Acta 103 (2015) 1–6. [41] F. Tarkanyi, A. Hermanne, F. Ditroi, S. Takacs, A.V. Ignatyuk, Activation crosssections of proton induced reactions on Hf-nat in the 38–65 MeV energy range: production of Lu-172 and of Yb-169, Nucl. Instrum. Methods Phys. Res., Sect. B 427 (2018) 20–37.
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Nuclear Inst. and Methods in Physics Research B journal homepage: www.elsevier.com/locate/nimb
Activation cross sections of deuteron induced reactions on 12–50 MeV energy range
nat
Hf in the
T
F. Tárkányia, A. Hermanneb, F. Ditróia, , S. Takácsa, A.V. Ignatyukc ⁎
a
Institute for Nuclear Research, Hungarian Academy of Sciences (ATOMKI), Debrecen, Hungary Cyclotron Laboratory, Vrije Universiteit Brussel (VUB), Brussels, Belgium c Institute of Physics and Power Engineering (IPPE), Obninsk 249020, Russia b
ARTICLE INFO
ABSTRACT
Keywords: Deuteron irradiation Stacked foil technique Ta, Hf, Lu and Yb radioisotopes Cross section Thick target yield Theoretical model codes
As a part of our systematical study of activation cross sections of deuteron induced nuclear reactions, cross sections on hafnium were investigated up to 50 MeV. Excitation functions were measured for the natHf (d,xn)178g,177,176,175,173Ta, natHf(d,x)181,180m,179m2,175,173,172Hf, natHf(d,x)173,172,171,170Lu and natHf(d,x)169Yb reactions by using the activation method, stacked foil irradiation technique and off-line gamma-ray spectrometry for quantification of the produced radionuclides. The experimental results are compared with the earlier results in the overlapping energy range, and with the theoretical predictions of the ALICE IPPE-D and EMPIRE II-D theoretical codes and with values reported in the TENDL-2017 on-line library obtained with the TALYS code.
1. Introduction Systematic measurements of activation cross sections of deuteron induced nuclear reactions are in progress up to 50 MeV deuteron energy for practical applications and to test nuclear reaction models. The status of the database for deuteron induced reactions was relatively poor compared to what is available for proton induced reactions, and the quality of the theoretical descriptions, even after several attempts for improvement, does not allow reliable estimation of the cross sections in many cases. In the present work we report our new data on deuteron induced reaction on natHf up to 50 MeV incident particle energy. Hafnium is essential in different aspects of aerospace, nuclear energy (control rods) and opto-electronics industry [1,2]. In most of these applications reliable activation cross section data are useful. They are also of interest for production of the medically relevant radionuclides 169 Yb, 177Lu, 179Lu 177Ta, 178gTa and for 172Hf/172Lu, 173Lu, 179Ta radioisotopes used in industrial measurement instruments. We investigated the production of the above listed isotopes by using proton and deuteron induced reactions on tungsten [3–5], tantalum [6], hafnium [7] lutetium [6,8], ytterbium [9–11], thulium [12–14] and alpha particle induced reactions on erbium [15,16] and ytterbium [16–18]. For deuteron induced reactions on hafnium only three sets of experimental activation cross section or production yields are available in
⁎
the literature, all of them below 22 MeV. Our cross section data measured earlier up to 20 MeV were reported by Takacs et al. 2010 [19] (corrected in Takacs et al. 2012 [20]) for production of 174,175,176,177,178m,180gTa, 173,175,179m2,180m,181Hf and 177g,179 Lu radioisotopes; Cross sections up to 16 MeV for production of 177Ta were measured by Simonelli et al. 2012 [21]; Thick target yield data for formation of 176,178Ta and 175Hf radionuclides at 22-MeV deuteron energy were reported by Dmitriev et al. 1982 [22]. 2. Experiment and data evaluation The experimental cross sections were determined by using the activation method, stacked foil irradiation technique and off-line gamma ray spectrometry for quantification of the produced radionuclides. Cross-section data were deduced relative to the recommended excitation functions of the 27Al(d,x)22,24Na monitor reactions [23] re-measured over the whole covered energy range. The irradiation was made at an external beam line of the Cyclone 90 cyclotron of the Université Catholique in Louvain la Neuve (LLN). The irradiation time was 60 min with a 50 MeV extracted deuteron beam of 100 nA nominal intensity. The targets were irradiated in a short Faraday cup. The irradiated stack contained a sequence of 7 sections consisting of
Corresponding author. E-mail address: [email protected] (F. Ditrói).
https://doi.org/10.1016/j.nimb.2019.01.005 Received 6 November 2018; Received in revised form 20 December 2018; Accepted 7 January 2019 0168-583X/ © 2019 Elsevier B.V. All rights reserved.
Nuclear Inst. and Methods in Physics Research B 441 (2019) 93–101
F. Tárkányi et al.
Table 1 (continued)
Table 1 Decay characteristics of the investigated reaction products and Q-values of reactions for their productions. Nuclide (Level) Decay
Half-life
178g
2.36 h
Ta ε: 100%
177
Ta ε: 100%
176
56.56 h
Iγ (%)
Contributing reaction
Q-value (keV)
213.440 325.562 331.613 426.383
81.4 94.1 31.19 97.0
177
Hf(d,n) Hf(d,2n) 179 Hf(d,3n) 180 Hf(d,4n)
2782.4 −4844.1 −10943.1 −18330.9
112.9 208.4
7.2 0.94
176
Hf(d,n) Hf(d,2n) 178 Hf(d,3n) 179 Hf(d,4n) 180 Hf(d,5n)
2202.69 −4172.91 −11798.84 −17897.84 −25285.59
178
177
5.7 2.4 5.4 24.7 5.7
176
Hf(d,2n) Hf(d,3n) Hf(d,4n) 179 Hf(d,5n) 180 Hf(d,6n)
−6217.9 −12593.5 −20219.4 −26318.4 −33706.2
207.4 266.9 348.5 998.3
14.0 11.24 12.0 2.6
174
Hf(d,n) Hf(d,3n) Hf(d,4n) 178 Hf(d,5n) 179 Hf(d,6n) 180 Hf(d,7n)
1628.6 −13245.9 −19621.5 −27247.5 −33346.4 −40734.2
3.14 h
160.4 172.2 180.6 1030.0 1208.2
4.9 17.5 2.22 1.42 2.7
174
Hf(d,3n) Hf(d,5n) 177 Hf(d,6n) 178 Hf(d,7n) 179 Hf(d,8n)
−14526.2 −29400.6 −35776.3 −43402.2 −49501.2
42.39 d
133.021 136.260 345.93 482.18
43.3 5.85 15.12 80.5
180
3470.234
−2224.566
5401.374 −2224.566 −9612.32
8.09 h
175
Ta ε: 100%
10.5 h
173
Ta ε: 100%
181
β-: 100%
177 178
176 177
176
Hf(d, p)
180m
Hf 1141.729 keV IT: 100%
5.53 h
215.426 332.274 443.162 500.697
81.6 94 81.7 14.2
180
179m2
Hf 1105.74 keV IT: 100%
25.05 d
122.70 146.15 169.78 192.66 217.04 236.48 268.85 315.93 362.55 409.72 453.59
27.7 27.1 19.4 21.5 9.0 18.8 11.3 20.3 39.6 21.5 68
177
175
Hf ε: 100%
70 d
343.40 433.0
84 1.44
174
Hf(d,p) Hf(d,p2n) 177 Hf(d,p3n) 178 Hf(d,p4n) 179 Hf(d,p5n) 180 Hf(d,p6n) 175 Ta decay
4483.934 −10390.54 −16766.16 −24392.1 −30491.09 −37878.85 1628.6
173
Hf ε: 100%
23.6 h
123.675 139.635 296.974 311.239
83 12.7 33.9 10.7
174
Hf(d,p2n) Hf(d,p4n) 177 Hf(d,p5n) 178 Hf(d,p6n) 179 Hf(d,p7n) 173 Ta decay
−10728.6 −25603.1 −31978.7 −39604.6 −45703.6 −14526.2
172
Hf ε: 100%
1.87 y
114.061 122.916 125.812 127.91
2.6 1.14 11.3 1.46
174
Hf(d,p3n) Hf(d,p5n) 177 Hf(d,p6n) 178 Hf(d,p7n) 172 Ta decay
−17809.5 −32683.9 −39059.6 −46685.5 −23664.1
173
1.37 y
171.393 272.105
2.90 21.2
174
−8477.1 −23351.58 −29727.2 −37353.13 −43452.12
Lu ε: 100%
Hf(d,pn)
Hf(d,p) Hf(d,pn) Hf(d,p2n)
179 180
176
176
176
Hf(d,2pn) Hf(d,2p3n) 177 Hf(d,2p4n) 178 Hf(d,2p5n) 179 Hf(d,2p6n) 176
Half-life
Eγ (keV)
Iγ (%)
Contributing reaction
Q-value (keV)
180
Hf(d,2p7n) Hf decay
−50839.88 −14526.2
173
201.84 521.6 710.50 1159.30 201.84
Ta ε: 100%
Hf
Eγ (keV)
Nuclide (Level) Decay
172g
181.525 810.064 900.724 912.079 1093.63
20.6 16.6 29.8 15.3 63
174
Hf(d,2p2n) Hf(d,2p4n) Hf(d,2p5n) 178 Hf(d,2p6n) 172 Hf decay
−16693.35 −31567.83 −37943.45 −45569.39 −17809.5
8.24 d
667.422 739.793 780.711 839.961
11.1 47.9 4.37 3.05
174
Hf(d,2p3n) Hf(d,2p5n) 177 Hf(d,2p6n) 171 Hf decay
−23672.25 −38546.74 −44922.36 −26851.7
Lu ε: 100%
2.012 d
938.75 985.10 987.25 1003.20 1225.65
1.57 5.4 1.65 3.44 4.83
174
Hf(d,2p4n) Hf(d,2p6n) 170 Hf decay
−32265.7 −47140.2 −34100.5
169
32.018 d
109.77924 130.52293 177.21307 197.95675 307.73586
17.39 11.38 22.28 35.93 10.35
174
−36483.38 −43708.7
Lu ε: 100%
6.70 d
171
Lu ε: 100%
170
Yb ε: 100%
176 177
176
176
169
Hf(d,3p4n) Lu decay
Abundance of isotopes in natural Hf -%: 174Hf-0.162, 176Hf-5.206, 177Hf-18.60, 178 Hf-27.30, 179Hf-13.63, 180Hf-35.10. The Q-values shown in Table 1 refer to formation of the ground state. Decrease Q-values for isomeric states with level energy of the isomer. Increase the Q-values if compound particles are emitted by: pn → d + 2.2 MeV, p2n → t + 8.5 MeV, 2pn → 3He + 7.7 MeV, 2p2n → α + 28.3 MeV.
Hf (10.54 μm), Al (49.54 μm), Al (49.54 μm), Pt (19.29 μm), Al (49.54 μm), Al (49.54 μm), CuMnNi alloy (24.73 μm), Al (49.54 μm), Al (49.54 μm) followed by 13 sections of Hf (10.54 μm) Al (10.85 μm), Al (49.54 μm), CuMnNi alloy (24.73 μm) and Al (10.85 μm). The 20 Hf targets covered the 50–12 MeV energy range. Gamma-ray spectra were measured at HpGe detectors in the cyclotron laboratory of VUB (Brussels). Four series of gamma-ray spectra were measured to follow the decay. These four series started between 7.9 and 10.3 h, 32.9 and 69.4 h, 126.8 and 194.5 h as well as 2166.3 and 2736.7 h after end of bombardment, respectively. Gamma spectra were evaluated by the automatic fitting algorithm included in the Genie 2000 package or in an iterative process using the Forgamma [24,25] code. For data evaluation NUDAT2.7 [26] and in case of 178Ta the Lund/ LBNL Nuclear Data [27] libraries were used (Table 1). As natural Hf consists of 6 stable isotopes, only the so called elemental cross-sections were determined over the entire energy range except for one reaction where only a single target isotope is contributing. The Q values of the contributing reactions (Q value calculator [28]) are also shown in Table 1 to indicate the reaction thresholds. Uncertainty of the measured cross-sections, estimated to be between 10 and 22%, was determined according to the recommendations in [29] by taking the sum in quadrature of all individual linear contributions: beam current (7%), target thickness or homogeneity (5%), detector efficiency (5%), photo peak area determination and counting statistics (1–20%). For preparation of the stack composition and of the irradiation parameters, the median energy in each of the target foils was obtained by a degradation calculation based on the calibrated primary beam energy and the stopping powers based on Anderson and Ziegler formula [30]. Final energy correction was applied based on the results of the fitted monitor reactions over the whole energy range (Tarkanyi et al. 1991 [31]), shown in Fig. 1. Only small correction was needed on the beam intensity and the energy degradation. Uncertainty of energy was estimated by taking into account cumulative effects on the energy 94
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Table 2 Experimental cross sections for the 178g
Fig. 1. Agreement of simultaneously measured experimental data of 27Al (d,x)22,24Na monitor reactions in comparison with the recommended values to monitor of the deuteron beam parameters through the irradiated stacks.
degradation (primary energy, target thickness, energy straggling) and the applied correction to monitor reaction. Due to the experimental circumstances (stacked foil technique, high dose to personnel at EOB, limited detector capacity, long cooling time before the first series of gamma spectra measurements) no cross section data were obtained for short lived (T1/2 < 2 h) activation products.
nat
177
Ta
Hf(d,xn)178g,177g,176,175g,173Ta reactions. 176
Ta
175
Ta
173
Ta
Ta
E
ΔE
σ
Δσ
σ
Δσ
σ
Δσ
σ
Δσ
σ
Δσ
MeV 49.2 47.1 45.0 42.8 40.5 38.1 35.6 33.2 31.8 30.4 28.9 27.4 25.8 24.2 22.4 20.6 18.6 16.5 14.2 11.5
0.3 0.3 0.4 0.4 0.4 0.5 0.5 0.6 0.6 0.7 0.8 0.9 0.9 1.0 1.1 1.3 1.4 1.5 1.7 1.8
mb 44.5 48.9 64.9 85.6 83.5 87.3 116.3 190.5 203.2 226.8 155.5 193.0 130.8 132.8 91.2 64.6 78.2 61.6 32.3 13.3
5.4 5.9 7.8 10.2 10.0 10.4 13.9 22.7 24.3 27.1 18.6 23.0 15.6 15.9 10.9 7.7 9.4 7.4 3.9 1.7
190.3 245.5 336.3 431.1 372.2 286.8 264.5 260.3 276.6 276.7 224.3 350.4 269.6 350.2 292.3 217.2 249.3 175.2 90.5 40.9
22.8 29.3 40.1 51.4 44.4 34.2 31.6 31.0 33.0 33.0 26.8 41.8 32.2 41.8 34.9 25.9 29.7 20.9 10.8 4.9
267.2 262.7 308.7 316.9 261.7 219.5 234.4 253.2 319.8 332.6 242.8 313.2 207.6 213.4 185.5 125.5 126.4 59.3 33.7 14.2
32.5 32.4 38.1 39.4 32.7 28.1 29.6 34.6 38.7 40.3 29.5 38.3 25.2 26.0 22.6 15.7 15.6 7.8 4.1 1.7
271.5 308.0 377.4 426.7 325.5 240.6 214.1 215.5 227.1 225.6 148.0 181.8 96.9 81.5 55.1 36.1 24.6 8.9 2.2 1.8
32.4 36.8 45.1 51.0 38.9 28.8 25.6 26.0 27.1 27.0 17.7 21.8 11.6 9.8 6.7 4.4 3.0 1.2 0.3 0.2
72.8 50.8 52.5 32.3 14.9 7.5
8.9 6.6 6.5 4.2 3.0 1.0
Simonelli et al. [21] (Fig. 3). According to the new unpublished evaluated value for gamma-intensity of 208 keV by Kondev (private communication in [38]), all experimental data should be divided by a factor of 1.49 in the case if the new intensities are confirmed.
3. Comparison with nuclear model calculations
4.1.3. natHf(d,x)176Ta reaction The new experimental data for production of 176Ta (2.36 h) are in good agreement with the earlier low energy data [19]. The results of the reaction codes show different shapes and only TENDL-2017 describes approximately well the experimental excitation curve (Fig. 4).
The cross-sections of the investigated reactions were compared with the data given in the on-line TENDL-2017 library [32]. This library is based on both default and adjusted TALYS (1.9) calculations (Koning and Rochman, 2012 [33]). The cross sections of the investigated reactions were also compared with results of our calculations using ALICE-IPPE (Dityuk et al., 1998 [34]) and EMPIRE-II (Herman et al., 2008 [35]) codes modified for deuterons (D versions) by Ignatyuk, 2010–2011 [36,37]. To achieve a better description of available data for (d,p) reactions in these codes a phenomenological energy dependent enhancement factor was introduced on the basis of the observed (d,p) cross sections for medium and heavy nuclei. By this improvement, the direct (d,p) channel is increased strongly and this is reflected in changes for all other reaction channels. As ALICE-IPPE calculates only the total cross section, for estimation of isomeric state cross sections with the ALICE code the isomeric ratios obtained from EMPIRE-D were used.
4.1.4. natHf(p,x)175Ta reaction The new data are, similarly to the previous reactions, a little lower when compared to our earlier data [19] measured up to 20 MeV (Fig. 5). The shapes and the values of the experimental and theoretical excitation functions are different above 30 MeV, with TENDL-2017 giving a reasonable agreement. 4.1.5. natHf(d,x)173Ta reaction No earlier experimental data exist for production of 173Ta (3.14 h). The theoretical cross sections TENDL, ALICE and EMPIRE give higher estimations than our new experimental results (Fig. 6). 4.1.6. 180Hf(d,p)181Hf The 181Hf (42.39 d) is produced only via (d,p) reaction on 180Hf and the reaction cross sections are shown in Fig. 7. There was an extra hafnium foil placed out of the range of the bombarding beam into the stack (at least below the threshold of the natHf(d,x)181Hf) and no 181Hf contribution was found in this foil, indicating negligible contribution of the secondary neutron reactions. The agreement with the earlier low energy data [19] is acceptable. Significant underestimation for all model codes can be observed (Fig. 6).
4. Results and discussion 4.1. Excitation functions The measured cross sections for the natHf(d,xn)178g,177,176,175,173Ta, 173,172,171,170 nat Hf(d,x)181,180m,179m2,175,173,172Hf, Lu and Hf 169 (d,x) Yb reactions are shown in Tables 2–4 and in Figs. 2–17. The figures also show the earlier reported data and the theoretical results.
nat
4.1.1. natHf(p,x)178gTa reaction The 9.31 min meta- and 2.36 h ground-states of 178Ta are decaying independently. Our new data for 178gTa formation are in agreement with the low energy data [19] in the overlapping energy range (Fig. 2). All model codes overestimate significantly the experimental data.
4.1.7. natHf(d,x)180mHf The isotope 180Hf has a stable ground state and a 180mHf (5.53 h) isomeric state, which is produced directly by deuteron bombardment of Hf. The neighboring isobars 180Ta (EC) and the 180Lu (β−) are decaying only to the 180gHf ground state. The agreement with our earlier reported low energy data [19] is good. The results of the theoretical codes are disagreeing, probably because of different estimations of isomeric ratios: TENDL-2017 presents some overestimation, while ALICE-D and
4.1.2. natHf(d,x)177Ta reaction Our data for production of 177Ta (56.56 h) are in good agreement with the earlier experimental data of Takacs et al. [19,20] and of 95
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Table 3 Experimental cross sections for the 181
nat
Hf(d,x)181,180m,179m2,175,173,172Hf reactions. 180m
Hf
179m2
Hf
175
Hf
173
Hf
172
Hf
Hf
E
ΔE
σ
Δσ
σ
Δσ
σ
Δσ
σ
Δσ
σ
Δσ
σ
Δσ
MeV 49.2 47.1 45.0 42.8 40.5 38.1 35.6 33.2 31.8 30.4 28.9 27.4 25.8 24.2 22.4 20.6 18.6 16.5 14.2 11.5
0.3 0.3 0.4 0.4 0.4 0.5 0.5 0.6 0.6 0.7 0.8 0.9 0.9 1.0 1.1 1.3 1.4 1.5 1.7 1.8
mb 20.7 23.5 31.3 40.7 37.5 32.0 38.8 54.2 58.9 72.9 53.5 87.3 70.4 101.6 103.9 95.4 143.4 159.4 163.8 196.6
2.5 2.8 3.7 4.9 4.5 3.8 4.6 6.5 7.0 8.7 6.4 10.4 8.4 12.1 12.4 11.4 17.1 19.0 19.5 23.4
2.6 2.2 4.6 3.8 5.3 4.3
0.8 0.7 0.7 1.0 1.0 0.9
413.0 440.0 532.6 605.3 454.9 314.8 289.0 306.6 284.1 292.6 177.9 216.2 115.5 96.3 61.9 41.4 26.9 5.8 1.4 1.3
49.2 52.4 63.5 72.1 54.2 37.5 34.4 36.5 33.9 34.9 21.2 25.8 13.8 11.5 7.4 4.9 3.2 0.7 0.2 0.2
13.4 10.7 9.0 7.5 3.8 1.1
13.8 9.8 9.7 6.0
1.8 1.9 1.3 1.2
7.1
1.2
1.0 0.7 0.9 0.9 1.2 0.6 1.1 0.7 0.5 0.7 0.5 0.3 0.2
0.4 0.4 0.5 0.6 0.6 0.4 0.4 0.5 0.4 0.4 0.3 0.3 0.2 0.2 0.2 0.1 0.1 0.1
112.4 89.6 75.2 61.9 30.5 6.9
5.0 4.6 6.7 4.1 7.0 3.7 6.6 4.7 3.1 3.8 2.2 1.4 1.4
3.1 3.1 4.1 4.7 4.5 2.9 3.0 3.6 3.2 3.3 2.0 2.2 1.5 1.8 1.2 0.8 0.6 0.2
1.6 3.2
0.7 0.7
1.9
0.7
2.5 3.8 5.5
0.5 0.7 0.9
4.6 2.6
1.1 0.7
3.6
0.6
1.2
0.4
1.5
0.5
Table 4 Experimental cross sections for the 173
172
Lu
E
ΔE
MeV 49.2 47.1 45.0 42.8 40.5 38.1 35.6 33.2 31.8 30.4 28.9 27.4 25.8 24.2 22.4 20.6 18.6 16.5 14.2 11.5
0.3 0.3 0.4 0.4 0.4 0.5 0.5 0.6 0.6 0.7 0.8 0.9 0.9 1.0 1.1 1.3 1.4 1.5 1.7 1.8
173,172,171
Lu and
nat
Hf(d,x)169Yb reactions.
171
Lu
169
Lu
Yb
σ
Δσ
σ
Δσ
σ
Δσ
σ
Δσ
mb 106.4 88.0 83.9 74.7 43.8 22.8 16.6 17.3 15.6 18.5 12.5 17.6 12.1 13.7 11.1 7.4 8.9 7.3
12.7 10.5 10.0 8.9 5.2 2.8 2.0 2.1 1.9 2.2 1.5 2.1 1.5 1.7 1.4 0.9 1.1 0.9
5.9 5.5 5.7 5.2 3.4 1.9
0.7 0.7 0.7 0.6 0.4 0.2
5.1 4.3 3.8 3.4 0.5
0.6 0.5 0.5 0.4 0.1
33.4 26.4 24.7 18.5 8.9
4.1 3.2 3.0 2.3 1.2
1.3 0.9 0.9 0.4 0.4
0.2 0.1 0.1 0.1 0.1
0.1
0.0
Fig. 2. Experimental and theoretical cross sections for the formation of by deuteron bombardment of hafnium.
178g
Ta
EMPIRE-D are nearly equal and underestimate by a factor of 3 (Fig. 8). 4.1.8. natHf(d,x)179m2Hf reaction The isotope 179Hf has a stable ground-state and two isomeric states: a short-lived 179m1Hf (18.67 s) lower lying state and the longer-lived 179m2 Hf (25.05 d) higher energy isomeric state. We can deduce cross sections for this second isomeric state, which is produced only directly. There is no contribution from the neighboring isobars 179Lu (4.59 h) and 179Ta (1.82 y) in production of 179m2Hf. The agreement with our earlier reported low energy data [19] is good. There is large disagreement with the TENDL-2017 data (a factor of 2), the agreement with the ALICE-D and EMPIRE-D calculations is acceptable up to 40 MeV (Fig. 9).
Fig. 3. Experimental and theoretical cross sections for the formation of 177Ta by deuteron bombardment of hafnium.
4.1.9. natHf(d,x)175Hf(cum) reaction The measured cross section of 175Hf (70 d) is cumulative, measured 96
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Fig. 7. Experimental and theoretical cross sections for the clear reaction.
Fig. 4. Experimental and theoretical cross sections for the formation of 176Ta by deuteron bombardment of hafnium.
180
Hf(d,p)181Hf nu-
Fig. 8. Experimental and theoretical cross sections for the formation of by deuteron bombardment of hafnium.
Fig. 5. Experimental and theoretical cross sections for the formation of 175Ta by deuteron bombardment of hafnium.
180m
Hf
Fig. 9. Experimental and theoretical cross sections for the formation of 179m2Hf by deuteron bombardment of hafnium.
Fig. 6. Experimental and theoretical cross sections for the formation of 173Ta by deuteron bombardment of hafnium.
4.1.10. natHf(d,x)173Hf(cum) reaction The measured cumulative cross sections of 173Hf (23.6 h) include the decay of parent 173Ta (3.14 h, ε: 100%). The new results are in good agreement with the earlier measured low energy data [19] and also with results of TENDL and EMPIRE theoretical codes (Fig. 11).
after the “complete” decay of 175Ta (10.5 h, ε: 100%) (Fig. 10). The agreement with the low energy data [19] and with the theoretical predictions is acceptable. The contribution of secondary neutrons was neglected as described by the 181Hf case. 97
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Fig. 10. Experimental and theoretical cross sections for the formation of by deuteron bombardment of hafnium.
175
Fig. 13. Experimental and theoretical cross sections for the formation of by deuteron bombardment of hafnium.
173
Fig. 11. Experimental and theoretical cross sections for the formation of by deuteron bombardment of hafnium.
173
Fig. 14. Experimental and theoretical cross sections for the formation of by deuteron bombardment of hafnium.
172
Fig. 12. Experimental and theoretical cross sections for the formation of by deuteron bombardment of hafnium.
172
Fig. 15. Experimental and theoretical cross sections for the formation of by deuteron bombardment of hafnium.
171
Hf
Hf
Hf
Lu
Lu
Lu
4.1.12. natHf(d,x)173Lu(cum) reaction The measured cross sections of 173Lu (1.37 y) are cumulative, including the contributions from the 173Ta (3.14 h) → 173Hf (23.6 h) parent decay chain (Fig. 13). The experimental data are lower than the model predictions above 35 MeV. No earlier results are known for
4.1.11. natHf(d,x)172Hf(cum) reaction The 172Hf (1.87 y) is produced directly and through the decay of short-lived parent 172Ta (36.8 min). The comparison of the measured cumulative cross sections with the theory are shown in Fig. 12 (no earlier experimental results). 98
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Fig. 16. Experimental and theoretical cross sections for the formation of by the deuteron bombardment of hafnium.
170
Fig. 18. Integral thick target yields for the formation of the investigated radioisotopes of tantalum as a function of incident energy.
Lu
energy shifts of 5 MeV between them. 4.1.16. natHf(d,x)169Yb(cum) reaction The cross sections for production of 169Yb (32.018 d) were obtained from the gamma-spectra measured after nearly complete decay of the 169 Ta (4.9 min) → 169Hf (3.24 min) → 169Lu (34.06 h) → 169Yb parent decay chain (Fig. 17). The experimental data are much higher than the predictions of the theoretical codes, for which no proper explanation has been found yet. 5. Integral yields
Fig. 17. Experimental and theoretical cross sections for the formation of by the deuteron bombardment of hafnium.
The so-called physical integral yield ([Bonardi 1988 [39], Otuka 2015 [40]) was calculated from a spline fit to our earlier and recently measured experimental excitation functions and are shown in Figs. 18–20, respectively. For comparison only one experimental data point at 22 MeV was found, measured by Dmitriev et al. (1982), for the natHf(d,x)176,178Ta and 175Hf reactions [22]. As seen from Fig. 18 the earlier data of Dmitriev [22] for the single 22 MeV point are significantly lower in the case of 178gTa and significantly larger in the case of 176Ta than our new calculated yields. The largest thick targets yields can be observed by the 178g,176Ta radioisotopes, where considerable yield is expected even by lower
169
Yb
production of radioisotopes of lutetium. 4.1.13. natHf(d,x)172Lu(cum) reaction The measured cross section of 172Lu (6.70 d) includes the contribution from the decay of the short-lived 172mLu isomeric state (3.7 min, IT 100%) (Fig. 14). The cross section of the ground state was deduced from the measured gamma-spectra, where the contribution of the possible parent 172Hf (1.87 y) could be neglected. The rate of increase for the theoretical codes is different between TENDL-2017 and the two other codes and is clearly sharper than what is experimentally seen. 4.1.14. natHf(d,x)171Lu(cum) reaction The measured cumulative cross sections of 171Lu (8.24 d) include the contribution from the decay of the 171Ta (23.3 min) → 171Hf (12.2 h) → 171Lu decay chain (Fig. 15). The experimental data are significantly lower than the results of the theoretical codes that show different rates of increase above 40 MeV. 4.1.15. natHf(d,x)170Lu(cum) reaction The single cumulative cross section point of 170Lu (2.012 d) (1.62 ± 0.60 mb at 49.2 MeV) (Fig. 16) was deduced from the gammaspectra measured after the complete decay of the 170Ta (6.76 min) → 170 Hf (16 h) parent radioisotopes. Due to low statistics no other reliable data points could be re-produced. The results of the three codes show
Fig. 19. Integral thick target yields for the formation of the investigated radioisotopes of hafnium as a function of the energy. 99
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[2] J.N.A. Matthews, Semiconductor industry switches to hafnium-based transistors, Phys. Today 61 (2008) 25. [3] F. Tárkányi, S. Takács, F. Szelecsényi, F. Ditrói, A. Hermanne, M. Sonck, Excitation functions of deuteron induced nuclear reactions on natural tungsten up to 50 MeV, Nucl. Instrum. Methods Phys. Res., Sect. B 211 (2003) 319–330. [4] F. Tárkányi, S. Takács, F. Szelecsényi, F. Ditrói, A. Hermanne, M. Sonck, Excitation functions of proton induced nuclear reactions on natural tungsten up to 34 MeV, Nucl. Instrum. Methods Phys. Res., Sect. B 252 (2006) 160–174. [5] F. Tárkányi, F. Ditrói, S. Takács, A. Hermanne, New measurements of excitation functions of 186W(p,x) nuclear reactions up to 65 MeV. Production of a 178W/ 178mTa generator, Nucl. Instrum. Methods Phys. Res., Sect. B 391 (2017) 27–37. [6] F. Tarkanyi, S. Takacs, F. Ditroi, A. Hermanne, A.V. Ignatyuk, M.S. Uddin, Activation cross sections of alpha-particle induced nuclear reactions on hafnium and deuteron induced nuclear reaction on tantalum: Production of W-178/Ta-178m generator, Appl. Radiat. Isot. 91 (2014) 114–125. [7] S. Takács, F. Tárkányi, A. Hermanne, R.A. Rebeles, Activation cross sections of proton induced nuclear reactions on natural hafnium, Nucl. Instrum. Methods Phys. Res., Sect. B 269 (2011) 2824–2834. [8] S. Takács, F. Tárkányi, A. Hermanne, A.-R. R., Investigation of cross sections of deuteron induced nuclear reactions on natural lutetium, in: International Conference on Radioanalytical and Nuclear Chemistry. RANC 2016, Springer, Budapest, Hungary, 2016, pp. 95. [9] F. Tárkányi, A. Hermanne, S. Takács, F. Ditrói, B. Király, H. Yamazaki, M. Baba, A. Mohammadi, A.V. Ignatyuk, Activation cross sections of proton induced nuclear reactions on ytterbium up to 70 MeV, Nucl. Instrum. Methods Phys. Res., Sect. B 267 (2009) 2789–2801. [10] F. Tárkányi, F. Ditrói, S. Takács, A. Hermanne, H. Yamazaki, M. Baba, A. Mohammadi, A.V. Ignatyuk, Activation cross-sections of longer lived products of deuteron induced nuclear reactions on ytterbium up to 40 MeV, Nucl. Instrum. Methods Phys. Res., Sect. B 304 (2013) 36–48. [11] F. Tárkányi, F. Ditrói, S. Takács, A. Hermanne, A.V. Ignatyuk, New data on activation cross section for deuteron induced reactions on ytterbium up to 50 MeV, Nucl. Instrum. Methods Phys. Res., Sect. B 336 (2014) 37–44. [12] F. Tárkányi, A. Hermanne, S. Takács, F. Ditrói, I. Spahn, A.V. Ignatyuk, Activation cross-sections of proton induced nuclear reactions on thulium in the 20–45 MeV energy range, Appl. Radiat. Isot. 70 (2012) 309–314. [13] I. Spahn, S. Takács, Y.N. Shubin, F. Tárkányi, H.H. Coenen, S.M. Qaim, Cross-section measurement of the Tm-169(p, n) reaction for the production of the therapeutic radionuclide Yb-169 and comparison with its reactor-based generation, Appl. Radiat. Isot. 63 (2005) 235–239. [14] F. Tárkányi, A. Hermanne, S. Takács, F. Ditrói, I. Spahn, S.F. Kovalev, A.V. Ignatyuk, S.M. Qaim, Activation cross sections of the Tm-169(d,2n) reaction for production of the therapeutic radionuclide Yb-169, Appl. Radiat. Isot. 65 (2007) 663–668. [15] B. Király, F. Tárkányi, S. Takács, A. Hermanne, S.F. Kovalev, A.V. Ignatyuk, Excitation functions of alpha-induced nuclear reactions on natural erbium, Nucl. Instrum. Methods Phys. Res., Sect. B 266 (2008) 549–554. [16] B. Király, F. Tárkányi, S. Takács, A. Hermanne, S.F. Kovalev, A.V. Ignatyuk, Excitation funcions of alpha-induced nuclear reactions on natural erbium and natural ytterbium targets, in: O. Bersillon, F. Gunsing, E. Bange (Eds.), International Conference on Nuclear Data for Science and Technology, EDP Sciences, Nice, France, 2008, pp. 1371–1374. [17] B. Király, F. Tárkányi, S. Takács, A. Hermanne, S.F. Kovalev, A.V. Ignatyuk, Excitation functions of alpha-particle induced nuclear reactions on natural ytterbium, Nucl. Instrum. Methods Phys. Res., Sect. B 266 (2008) 3919–3926. [18] F. Tárkányi, F. Ditrói, S. Takács, A. Hermanne, B. Király, Activation cross-section data for alpha-particle induced nuclear reactions on natural ytterbium for some longer lived radioisotopes, J. Radioanal. Nucl. Chem. 311 (2017) 1825–1829. [19] S. Takács, F. Tárkányi, A. Hermanne, R.A. Rebeles, Activation cross sections of deuteron-induced nuclear reactions on hafnium, Nucl. Instrum. Methods Phys. Res., Sect. B 268 (2010) 3443–3451. [20] S. Takács, F. Tárkányi, A. Hermanne, R.A. Rebeles, Activation cross sections of deuteron-induced nuclear reactions on hafnium (vol 268, pg 3443, 2010), Nucl. Instrum. Methods Phys. Res., Sect. B 281 (2012) 98–99. [21] F. Simonelli, K. Abbas, A. Bulgheroni, S. Pomme, T. Altzitzoglou, G. Suliman, Measurement of the Hf-nat(d, x)Ta-177 cross section and impact of erroneous gamma-ray intensities, Nucl. Instrum. Methods Phys. Res., Sect. B 285 (2012) 162–164. [22] P.P. Dmitriev, N.N. Krasnov, G.A. Molin, Radioactive nuclide yields for thick target at 22 MeV deuterons energy, Yadernie Konstanti 34 (1982) 38. [23] A. Hermanne, A.V. Ignatyuk, R. Capote, B.V. Carlson, J.W. Engle, M.A. Kellett, T. Kibedi, G. Kim, F.G. Kondev, M. Hussain, O. Lebeda, A. Luca, Y. Nagai, H. Naik, A.L. Nichols, F.M. Nortier, S.V. Suryanarayana, S. Takacs, F.T. Tarkanyi, M. Verpelli, Reference cross sections for charged-particle monitor reactions, Nucl. Data Sheets 148 (2018) 338–382. [24] Canberra, http://www.canberra.com/products/radiochemistry_lab/genie-2000software.asp., in, 2000. [25] G. Székely, Fgm – a flexible gamma-spectrum analysis program for a small computer, Comput. Phys. Commun. 34 (1985) 313–324. [26] NuDat, NuDat2 database (2.6), in, National Nuclear Data Center, Brookhaven National Laboratory, 2014. [27] S.Y.F. Chu, L.P. Ekström, R.B. Firestone, WWW Table of Radioactive Isotopes, version 2.1 http://ie.lbl.gov/toi/, in, 2004. [28] B. Pritychenko, A. Sonzogni, Q-value calculator, in: NNDC, Brookhaven National Laboratory, 2003. [29] International-Bureau-of-Weights-and-Measures, Guide to the Expression of
Fig. 20. Integral thick target yields for the formation of the investigated radioisotopes of lutetium and ytterbium as a function of the energy.
bombarding energies. The only earlier literature value for 175Hf in a single energy point is significantly larger than our new result. The yields are significantly lower than by Ta radioisotopes and only the 181,180mHf have reasonable yields under 10 MeV. There are no literature data for production of Lu and Yb radioisotopes. The calculated yields are even lower than in the above two cases and the production thresholds are definitively higher. Comparing the yield results of deuteron induced reactions on natural hafnium we can conclude that for the production of medically relevant radioisotopes there are competitive routes as far as the target element and bombarding particle regarded [41]. 6. Summary and conclusion We report experimental cross sections for the natHf (d,xn)178g,177,176,175,173Ta, natHf(d,x)181,180m,179m2,175,173,172Hf, 173,172, 171,170 Lu and natHf(d,x)169Yb reactions up to 50 MeV incident deuteron energy. The new results successfully complete the earlier experimental data published up to 22 MeV [19,20]. In most cases acceptable agreement was found with the literature values in the overlapping energy range. The experimental data were compared with the results of a priori model calculations performed with the EMPIRE-D, ALICE-IPPE-D and TALYS codes (available in TENDL-2017 on-line database). The descriptions of the shape and the absolute values of the excitation functions by the theoretical calculations is only partly successful, and despite upgrading of the codes still large disagreements were found for many cases. The obtained experimental data provide a basis for improved model calculations and for optimization of various applications connected to charged particle activation. Among the radioisotopes mentioned in the introduction with recently documented practical applications, the magnitude of deuteron induced reactions could be of significance for production of 177 Ta,178gTa,179Ta and 173Lu. Acknowledgement The authors acknowledge the support of the respective institutions and the accelerator staffs for providing the beam time and experimental facilities. References [1] R. Tricot, The metallurgy and functional properties of hafnium, J. Nucl. Mater. 189 (1992) 277–288.
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Nuclear Inst. and Methods in Physics Research B 441 (2019) 93–101
F. Tárkányi et al.
[30] [31] [32] [33] [34] [35]
Uncertainty in Measurement, 1st ed., International Organization for Standardization, Genève, Switzerland, 1993. H.H. Andersen, J.F. Ziegler, Hydrogen stopping powers and ranges in all elements. The stopping and ranges of ions in matter, Pergamon Press, New York, 1977 vol. 3. F. Tárkányi, F. Szelecsényi, S. Takács, Determination of effective bombarding energies and fluxes using improved stacked-foil technique, Acta Radiol. Suppl. 376 (1991) 72. A.J. Koning, D. Rochman, J.C. Sublet, TENDL-2017 TALYS-based evaluated nuclear data library, in, 2017. A.J. Koning, D. Rochman, Modern nuclear data evaluation with the TALYS code system, Nucl. Data Sheets 113 (2012) 2841. A.I. Dityuk, A.Y. Konobeyev, V.P. Lunev, Y.N. Shubin, New version of the advanced computer code ALICE-IPPE, in: INDC (CCP)-410, IAEA, Vienna, 1998. M. Herman, R. Capote, B.V. Carlson, P. Oblozinsky, M. Sin, A. Trkov, H. Wienke, V. Zerkin, EMPIRE: nuclear reaction model code system for data evaluation, Nucl. Data Sheets 108 (2007) 2655–2715.
[36] A.V. Ignatyuk, 2nd RCM on FENDL-3, in: IAEA, Vienna, Austria, 2010. [37] A.V. Ignatyuk, Phenomenological systematics of the (d,p) cross sections, http:// www-nds.iaea.org/fendl3/000pages/RCM3/slides//Ignatyuk_FENDL-3%20presentation.pdf, in: IAEA (Ed.), Vienna, 2011. [38] F.G. Kondev, Personal communicatiom, in, 2018. [39] M. Bonardi, The contribution to nuclear data for biomedical radioisotope production from the Milan cyclotron facility, in: K. Okamoto (Ed.) Consultants Meeting on Data Requirements for Medical Radioisotope Production, IAEA, INDC(NDS)-195 (1988), Tokyo, Japan, 1987, pp. 98–112. [40] N. Otuka, S. Takacs, Definitions of radioisotope thick target yields, Radiochim. Acta 103 (2015) 1–6. [41] F. Tarkanyi, A. Hermanne, F. Ditroi, S. Takacs, A.V. Ignatyuk, Activation crosssections of proton induced reactions on Hf-nat in the 38–65 MeV energy range: production of Lu-172 and of Yb-169, Nucl. Instrum. Methods Phys. Res., Sect. B 427 (2018) 20–37.
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