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The 95Nb nucleus in the metastable and ground states can be formed in photonuclear reactions natMo
$ (\gamma,x{{{{np}}}}) $ . Natural molybdenum consists of 7 stable isotopes, but only four isotopes contribute to the formation of the 95Nb nucleus; there are four reactions with the following thresholds:96Mo
$(\gamma,{{p}})^{95{{g}}} {\rm{Nb}}$ –$ E_{\rm{thr}} $ = 9.30 MeV;97Mo
$(\gamma,{{{np}}})^{95{{g}}} {\rm{Nb}}$ –$ E_{\rm{thr}} $ = 16.12 MeV;98Mo
$(\gamma,{{2np}})^{95{{g}}} {\rm{Nb}}$ –$ E_{\rm{thr}} $ = 24.76 MeV;100Mo
$(\gamma,{{4np}})^{95{{g}}} {\rm{Nb}}$ –$ E_{\rm{thr}} $ = 38.98 MeV.The thresholds for the formation of the
$ ^{95{{m}}} {\rm{Nb}} $ nucleus in the metastable state are higher than in the ground state, with an excess excitation energy of 235.7 keV.The calculation of theoretical cross-sections
$ \sigma(E) $ of studied reactions for monochromatic photons was performed using the TALYS1.95 code [32], which is installed on Linux Ubuntu-20.04, for different level density models LD 1-6. There are three phenomenological level density models and three options for microscopic level densities:$ LD 1 $ : Constant temperature + Fermi gas model, introduced by Gilbert and Cameron [35].$ LD 2 $ : Back-shifted Fermi gas model [36].$ LD 3 $ : Generalized superfluid model (GSM) [37, 38].$ LD 4 $ : Microscopic level densities (Skyrme force) from Goriely’s tables [39].$ LD 5 $ : Microscopic level densities (Skyrme force) from Hilaire’s combinatorial tables [40].$ LD 6 $ : Microscopic level densities based on temperature-dependent Hartree-Fock-Bogoliubov calculations using the Gogny force from Hilaire’s combinatorial tables [41].Figure 3 lists the total (metastable + ground) cross-sections
$ \sigma(E) $ for the formation of the 95Nb nucleus on 4 stable isotopes of molybdenum calculated in the TALYS1.95 code, LD1. The cross-sections for the 96,97,98,100Mo nuclei are given considering the abundance of isotopes. The cross-section of the natMo$ (\gamma,x{{{np}}})^{95} {\rm{Nb}} $ reaction is their algebraic sum. As can be seen, in the energy range above 35 MeV, the cross-section of the 98Mo$ (\gamma,{{2np}})^{95} {\rm{Nb}} $ reaction has the highest values. This is due to both the 98Mo isotopic abundance of 24.13% and insignificant differences in the cross-sections for the formation of the 95Nb nucleus on different molybdenum isotopes.Figure 3. (color online) Theoretical total (metastable + ground) cross-sections
$ \sigma(E) $ for the formation of the 95Nb nucleus on stable isotopes of molybdenum 96,97,98,100Mo, considering isotopic abundance (color curves), and on natMo (black curve). The calculations were performed for the level density model LD1.Figure 4 shows the cross-sections
$ \sigma(E) $ for the formation of the 95Nb nucleus in the metastable and ground states in the natMo$ (\gamma,x{{{np}}}) $ reactions and the total cross-section calculated using the TALYS1.95 code, LD1. The cross-section for natMo$ (\gamma,x{{{np}}})^{95{{g}}} {\rm{Nb}} $ is the algebraic sum of the cross-sections of the formation of$ ^{95{{g}}} {\rm{Nb}} $ on each of the 4 isotopes multiplied by the isotopic abundance. Similarly, it needs to take sum in the case of the cross-section for the natMo(γ, xnp)$^{95{m}}{\rm{Nb}} $ reaction. The total cross-section is calculated as the sum of cross-sections for the ground and metastable states. As can be seen from the figure, the contribution of the metastable state to the total cross-section does not exceed 20% at energies above 30 MeV.Figure 4. (color online) Theoretical cross-sections
$ \sigma(E) $ of the natMo$(\gamma,x{{{np}}})^{95{{m,g}}}{\rm{Nb}}$ reactions. The calculations were performed for the level density model LD1.Using the theoretical cross-section
$ \sigma(E) $ , one can obtain the reaction yield, which is determined by the formula$ Y(E_{\rm{\gamma max}}) = N_n \int\nolimits_{E_{{\rm{thr}}}}^{E_{\rm{\gamma max}}}\sigma(E)\cdot W(E,E_{\rm{\gamma max}}){\rm d}E, $
(1) where
$ N_n $ is the number of atoms of the element under study,$ W(E,E_{\rm{\gamma max}}) $ is the bremsstrahlung γ-flux,$ E_{\rm{thr}} $ is an energy of the reaction threshold, and$ E_{\rm{\gamma max}} $ is the bremsstrahlung end-point energy.To estimate the i-th reaction contribution in the total production of a studied nuclide (for example, the 96Mo
$ (\gamma,p) $ reaction in the production of the 95Nb nucleus on natMo), the relative reaction yield$ Y_{\rm{i}}(E_{\rm{\gamma max}}) $ was used. To calculate$ Y_{\rm{i}}(E_{\rm{\gamma max}}) $ , we used the cross-sections from the TALYS1.95 code and the following expression:$ Y_{\rm{i}}(E_{\rm{\gamma max}}) = \frac {A_i \displaystyle\int\nolimits_{E^i_{{\rm{thr}}}}^{E_{\rm{\gamma max}}}\sigma_i(E)\cdot W(E,E_{\rm{\gamma max}}){\rm d}E} {\sum^4_{k=1} A_k \displaystyle\int\nolimits_{E^k_{{\rm{thr}}}}^{E_{\rm{\gamma max}}}\sigma_k(E)\cdot W(E,E_{\rm{\gamma max}}){\rm d}E}, $
(2) where
$ \sigma_k(E) $ is the cross-section for the formation of the 95Nb nucleus on the k-th isotope with isotopic abundance$ A_k $ . Summation over k was performed for 4 stable molybdenum isotopes 96,97,98,100Mo. The relative reaction yield on a given isotope is affected by the cross-section, reaction threshold, and isotope abundance.As a rule, in the presence of several isotopes, there is one whose contribution to the reaction yield dominates (> 90%); see Refs. [42, 43] for examples. In the case of the reaction under study at energies up to 20 MeV, the contribution from the reaction on 96Mo is 100%. However, at the bremsstrahlung end-point energy above 30 MeV, it is difficult to determine the dominant reaction (see Fig. 5). Thus, for natural molybdenum, it is necessary to consider the contribution of all stable isotopes to the yield of the natMo
$ (\gamma,x{{{np}}})^{95} {\rm{Nb}} $ reaction.Figure 5. (color online) Theoretical reaction yields of the 95Nb formation on various molybdenum isotopes relative to the total yield on natMo according to Eq. (2). The sum of the relative yield is equal to 1.0. The calculations were performed for the level density model LD1.
In this study, the values of the IR are calculated as the ratio of the yield
$ Y_{\rm{H}}(E_{\rm{\gamma max}}) $ of the formation of the nucleus in the high-spin state to the yield$ Y_{\rm{L}}(E_{\rm{\gamma max}}) $ of the formation of the nucleus in the low-spin state:$ IR = Y_{\rm{H}}(E_{\rm{\gamma max}}) / Y_{\rm{L}}(E_{\rm{\gamma max}}). $
(3) Figure 6 shows the theoretical prediction of the IR calculated using the cross-sections from the TALYS1.95 code with the LD1 model. As can be seen, the calculated IR values differ for different isotopes (96,97,98,100Mo). The IR value calculated for natural Mo is within the range of these varying values.
Figure 6. (color online) Theoretical IR values for the reaction products
$^{95{{m,g}}}{\rm{Nb}} $ on different molybdenum isotopes and natMo. The calculations were performed for the level density model LD1.The theoretical estimations of the IR values were calculated using the cross-sections from the TALYS1.95 code for six level density models LD and are shown in Fig. 7. As can be seen, the theoretical IR values differ by 17%–36% in the range of
$ E_{\rm{\gamma max}} $ = 35–95 MeV. The IR calculated for the LD3 model has the lowest value in this energy range. -
A simplified diagram of the decay of the niobium nucleus from the ground
$^{95{{g}}} {\rm{Nb}}$ and metastable$^{95{{m}}} {\rm{Nb}}$ states is shown in Fig. 8, according to Ref. [1].Figure 8. (color online) Simplified representation of the formation and decay scheme of the isomeric pair 95m,gNb. The nuclear level energies are in keV. The red color shows the emission γ-lines that were used in this study for the analysis.
The metastable state
$^{95{{m}}} {\rm{Nb}}$ ($ J^\pi = 1/2^{-} $ ) with a half-life$ T_{1/2} $ of$ 86.6 \pm 0.08 $ h decays to the unstable ground state$^{95{{g}}} {\rm{Nb}}$ ($ J^\pi = 9/2^{+} $ ) by emitting γ-quanta with an energy of 235.7 keV ($ I_\gamma = 24.9 \pm 0.8 $ %) through an internal transition with a branching ratio p of$ 94.4 \pm 0.6 $ %. Meanwhile, 5.6% of the metastable state decays to the various energy levels of stable 95Mo via a$ \beta^- $ -process. The unstable ground state$^{95{{g}}} {\rm{Nb}}$ with a half-life$ T_{1/2} $ of$ 34.975 \pm 0.007 $ d decays to the 765.8 keV ($ I_\gamma$ = 100%) energy level of 95Mo via a$ \beta^- $ -process (99.97%).This decay pattern leads to the ground state radionuclide
$^{95{{g}}} {\rm{Nb}}$ , which can be formed in two ways: directly from the target nuclide and/or indirectly through the decay of the metastable radionuclide.As a result, to find the experimental values of the IR, it is necessary to solve the system of equations describing the radioactive decay of the metastable state and decay with accumulation for the ground state. The solution of such a system of equations is described in several works [4, 44, 45], with different analytical representations.
In this study, to determine the experimental values of the IR, the following expression is used according to Ref. [44]:
$ \begin{aligned}[b] IR =& Y_{{H}}(E_{\rm{\gamma max}}) / Y_{{L}}(E_{\rm{\gamma max}}) = \\& \left[ \frac{\lambda_{{g}} F_{{m}}(t)}{\lambda_{{m}} F_{{g}}(t)} \left(\frac{\Delta A_{{g}} I_{{m}} \varepsilon_{{m}}}{\Delta A_{{m}} I_{{g}} \varepsilon_{{g}}} - p\frac{\lambda_{{g}}}{\lambda_{{g}} - \lambda_{{m}}}\right) + p\frac{\lambda_{{m}}}{\lambda_{{g}} - \lambda_{{m}}} \right], \end{aligned} $
(4) $ F_{{m}}(t) = (1-{\rm e}^{-\lambda_{{m}} t_{\rm{irr}}}){\rm e}^{-\lambda_{{m}} t_{\rm{cool}}}(1-{\rm e}^{-\lambda_{{m}} t_{\rm{meas}}}), $
(5) $ F_{{g}}(t) = (1-{\rm e}^{-\lambda_{{g}} t_{\rm{irr}}}){\rm e}^{-\lambda_{{g}} t_{\rm{cool}}}(1-{\rm e}^{-\lambda_{{g}} t_{\rm{meas}}}), $
(6) where
$\lambda_{{g}}$ and$\lambda_{{m}}$ are the decay constants for the ground and metastable states, respectively;$\Delta A_{{g}}$ and$\Delta A_{{m}}$ are the number of counts under the peaks at the energies of γ-quanta corresponding to the decays of the ground and metastable states, respectively;$\varepsilon_{{g}}$ and$I_{{g}}$ ($\varepsilon_{{m}}$ and$I_{{m}}$ ) are the detector efficiency and absolute intensity of a γ-quantum with an energy corresponding to the decay of the ground state (metastable state); p is the branching ratio for the decay of the metastable to the ground state (94.4%); and$ t_{\rm{irr}} $ ,$ t_{\rm{cool}} $ , and$ t_{\rm{meas}} $ are the irradiation time, cooling time, and measurement time, respectively.In natural molybdenum targets, as a result of the natMo
$ (\gamma,x{{n2p}}) $ reaction, the 95Zr nucleus can also be formed. In the decay scheme of 95Zr ($ T_{1/2} = 65.02 \pm 0.05 $ d), there is a γ-transition with an energy$ E_\gamma $ = 235.7 keV and intensity$ I_\gamma = 0.294 \pm 0.016 $ %. The decay of the 95Zr nucleus can contribute to the observed value of$\Delta A_{{m}}$ . Considering this contribution, calculations were performed in the TALYS1.95 code with level density model LD1. It was found that the activity of 95Zr estimated using the γ-linewith 235.7 keV is negligible. The contribution of 95Zr was also experimentally verified by the γ-lines corresponding to the decay of the 95Zr nucleus, namely,$ E_\gamma $ = 724.2 keV ($ I_\gamma = 44.17 \pm 0.13 $ %) and$ E_\gamma $ = 756.7 keV ($ I_\gamma $ = 54%). No such peaks were found in the measured spectra of the induced γ-activity of the targets.For the γ-quanta with an energy of 235.7 keV and the thicknesses of the molybdenum targets used, the self-absorption coefficients were calculated using the GEANT4.9.2 code. It was found that the value of the self-absorption coefficient did not exceed 0.8%, which was considered when processing the experimental results.
The experimental values of the IR of the nuclei products from the natMo
$ (\gamma,x{{{np}}})^{95{{m,g}}}{\rm{Nb}} $ reaction were determined at the bremsstrahlung end-point energy of 38–93 MeV (see Fig. 9 and Table 1).Figure 9. (color online) IR for the reaction products from the natMo
$(\gamma,x{{{np}}})^{95{{m,g}}}{\rm{Nb}}$ reaction. Experimental results of this study are indicated using blue circles. The data of other studies are indicated as follows: square – [23], red empty circles – [21], and black circles – [22]. The curve indicates the calculation using the code TALYS1.95, LD3, divided by a factor of 3.85.$ E_{\rm{\gamma max}} $ /MeV$IR \pm \Delta IR $ 37.50 0.75 ± 0.10 41.10 0.79 ± 0.10 44.20 0.91 ± 0.07 49.00 0.80 ± 0.06 53.70 0.97 ± 0.10 53.70* 1.03 ± 0.10 59.60 0.95 ± 0.07 59.60* 0.81 ± 0.07 63.30 1.05 ± 0.12 63.30* 0.98 ± 0.13 65.50 1.16 ± 0.12 65.50* 1.13 ± 0.13 68.25 1.05 ± 0.13 68.25* 1.00 ± 0.13 73.10 0.83 ± 0.11 77.50 1.10 ± 0.09 82.50 1.28 ± 0.13 86.90 1.03 ± 0.11 92.50 1.07 ± 0.12 92.90 1.11 ± 0.13 Table 1. IR for the nuclei products
$^{95{{m,g}}}{\rm{Nb}}$ from the$ {^{\rm{nat}}{\rm{Mo}}}(\gamma,x{{{np}}}) $ reaction.The calculation of the experimental error of the IR values was performed considering statistical and systematic errors, the description of which can be found, for example, in [24, 25]. The uncertainties related to IR were calculated from Eq. (4) using the error propagation principle, which indicates the maximum uncertainty of the measured values in Fig. 9 and Table 1.
Isomeric pair 95m,g Nb in the photonuclear reactions on natMo at the bremsstrahlung end-point energy of 38–93 MeV
- Received Date: 2023-07-09
- Available Online: 2023-12-15
Abstract: The