-
The average neutron energy
$ {\stackrel{-}{E}}_{n} $ at a particular angle is calculated from the average D-beam energy$ {\stackrel{-}{E}}_{d} $ incident on the D-Ti target with a specific thickness according to nuclear reaction kinetics under non-relativistic conditions. Taking into account the effect of the finite geometrical tensor angle on the neutron energy distribution at the sample, the average neutron energy$ {\stackrel{-}{E}}_{n} $ in the 0° direction is calculated by the following equations:$ {\bar E_n} = \frac{{2{d^2}}}{{{R^2}}}\int_0^\theta {{E_n}} (\theta ,{\bar E_d})\frac{{\tan \theta }}{{{{\cos }^2}\theta }}{\rm d}\theta , $
(1) with
$ {\bar E_d} = \frac{{\displaystyle\int_{{E_e}}^{{E_0}} {\dfrac{{{\sigma _T}({E_d})}}{{\dfrac{{{\rm d}E}}{{{\rm d}X}}({E_d})}}{E_d}{\rm d}{E_d}} }}{{\displaystyle\int_{{E_e}}^{{E_0}} {\dfrac{{{\sigma _T}({E_d})}}{{\dfrac{{{\rm d}E}}{{{\rm d}X}}({E_d})}}{\rm d}{E_d}} }}, $
(2) $ \Delta X = \int_{{E_e}}^{{E_0}} {\frac{1}{{\dfrac{{{\rm d}E}}{{{\rm d}X}}({E_d})}}{\rm d}{E_d}}, $
(3) where
$ {\bar{E}}_{d} $ is the average D-beam energy due to the energy deposited by the D-beam onto the D-Ti target, d is the distance of the sample from the target, and R is the sample radius. σT (Ed) is the cross-section of the D (d, n)3He reaction. E0 is the initial energy of the D-beam, and the final energy Ee is obtained by numerical integration based on the energy loss rate${\rm d}E/{\rm d}X$ (the unit is keV/mg$ \cdot $ cm-2) of D inthe D-Ti target and the target thickness $ \Delta X $ (the unit is mg/cm2) as given in Equation (3). Similarly, the average neutron energy in the 60° direction is obtained by taking into account the effects of the target thickness and geometrical tensor angle. Neutron energy dispersion depends on the extent of the spreading of the neutron energy distribution. The neutron energy dispersion caused by the target thickness is derived from half of the difference between the neutron energy corresponding to the initial energy E0 and the final energy Ee of the incident D nucleus. The total neutron energy dispersion$ \Delta {\bar{E}}_{n} $ is the squared sum of the energy dispersion due to the target thickness and the energy dispersion induced by the finite tensor angle. Therefore, neutron energies of 6.117 ± 0.119 MeV, 4.626 ± 0.086 MeV, and 3.622 ± 0.348 MeV were calculated for this experiment. -
The decay schematic of the radionuclide 239U generated by the U3O8 sample after neutron irradiation is shown below:
$ {}_{92}^{238}{\rm U}(n,\gamma ){}_{92}^{239}{\rm U}\xrightarrow{{{\beta ^ - }(100\% ),23.45\min }}{}_{93}^{239}{\rm Np}\xrightarrow{{{\beta ^ - }(100\% ),2.36d}}{}_{94}^{239}{\rm Pu}. $
The decay parameters of the generated radionuclides 239U and 239Np are all from NuDat3.0 [31] and are listed in Table 1. It can be found that the radioisotope 239U has a relatively short half-life of only 23.45 min, and that the characteristic γ-ray intensity greater than 50% has an energy of only 74.66 keV. The characteristic γ-rays with 74.66 keV produced by 239U are of low energy, and the measurement of the full-energy peak by this characteristic γ-ray with the HPGe detector has a large uncertainty. In addition, owing to the γ-ray self-absorption effect of the sample, it is hardly possible to accurately determine the amount of 239U by net counts of the full-energy peak of the characteristic γ-rays generated by 239U. Therefore, the characteristic γ-rays with 277.6 keV originating from the primary
$ {\beta }^{-} $ decay product 239Np with a longer half-life are more appropriate. However, the method of calculating the cross-sections by the characteristic γ-ray spectrum of 239Np causes certain errors. Mainly, it neglects the effect of the decay of 239U on the number growth of 239Np within 1.5 h after the end of irradiation and considers it as the decay of 239Np according to the exponential decay law during this time [32]. According to the work of Qiu et al. [32], the indirect measurement of cross-sections using decay products is meaningful when the difference between the half-lives of the parent and daughter nuclei is large (the ratios of the decay constants > 10). It is clear that the decay chain of 239U satisfies this requirement (decay constant ratio is 144.7); thus, it is not necessary to measure the characteristic γ-rays of the direct product 239U in the process of measuring the neutron capture cross-sections of 238U, and the error introduced by this treatment is negligible at 0.2%. Moreover, after cooling for at least 3 h (more than five half-lives of 239U), more than 99.9% of 239U will have decayed to generate 239Np. Considering the above, the 238U neutron capture cross-sections are determined from the net counts of the characteristic γ-ray full-energy peak of 239Np. The 239Np radionuclide is recognizable by the characteristic γ-rays of 106.1 keV, 228.2 keV, and 277.6 keV, whose intensities all surpass 10%. Nevertheless, the γ-rays at 277.6 keV were preferred over others in the calculations because the γ-rays at 106.1 keV and 228.2 keV are subjected to interference by the γ-rays at 103.2 keV and 228.2 keV originating from the fission products 153Sm (T1/2 = 46.284 h) and 132Te (T1/2 = 3.204 d), respectively [4–6]. In this experiment, the 197Au (n, γ)198Au reaction was applied to measure the neutron fluence at the U3O8 sample with the following equations:Table 1. Relevant decay data of the radionuclides 198Au, 239U, and 239Np.
$ \varphi = \frac{{{\lambda _{\rm Au}}{A_{\rm Au}}(\frac{{{t_c}}}{{{t_l}}})}}{{{\varepsilon _{\rm Au}}{I_{\rm Au}}{\sigma _{\rm Au}}{N_{\rm Au}}\left( {1 - {{\rm e}^{ - {\lambda _{\rm Au}}{t_0}}}} \right){{\rm e}^{ - {\lambda _{\rm Au}}{t_1}}}\left( {1 - {{\rm e}^{ - {\lambda _{\rm Au}}{t_c}}}} \right)}} $
(4) with
$ {N_{\rm Au}} = \frac{W}{M}{N_A}f ,$
(5) where εAu is the full-energy peak efficiency of the characteristic γ-ray produced by the Au sample, IAu is the γ-ray intensity, σAu is the standard reference cross-section originating from ENDF/B-VIII.0, and NAu is the number of atoms of 197Au (the calculation formula of NAu is shown in Equation (4); W is the sample weight, M is the relative atomic mass, NA is the Avogadro constant, and f is the natural abundance of the sample). λAu is the decay constant of the radionuclide 198Au, and AAu refers to the net counts of the characteristic γ-ray full-energy peak. t0, t1, tc, and tl are the total neutron irradiation time, chilling time, measuring time according to the clock, and measurement of the living time, respectively. Having determined the neutron flux at the U3O8 sample, the neutron capture cross-section of 238U is inferred with the following equations:
$ {\sigma _u} = \frac{{{{(\varepsilon INT)}_{\rm Au}}}}{{{{(\varepsilon INT)}_u}}} \cdot \frac{{{{(A\lambda \frac{{{t_c}}}{{{t_l}}})}_u}}}{{{{(A\lambda \frac{{{t_c}}}{{{t_l}}})}_{\rm Au}}}} \cdot {\sigma _{\rm Au}} $
(6) with
$ T = (1 - {{\rm e}^{ - \lambda {t_0}}}){{\rm e}^{ - \lambda {t_1}}}(1 - {{\rm e}^{^{ - \lambda {t_c}}}}). $
(7) -
During the experimental determination of the reaction cross-section of 238U (n, γ)239U, many factors inevitably affect the ultimate values of the experiment. Therefore, the experimental correction of the 238U neutron capture cross-section is particularly important. The primary revision elements concern five components: neutron fluence fluctuation effect Ff, sample self-absorption effect Fγ and the counting geometric correction Fg when measuring γ-rays, the neutron scattering effect FS induced by the layer of cooled water and the tube wall materials of the target head, and the neutron self-shielding effect Fa due to the thickness of the sample itself. Among them, the neutron scattering effect FS, the counting geometric correction Fg, and the neutron self-shielding effect Fa are simulated by the Monte Carlo program, while the neutron fluence fluctuation effect Ff and the γ-rays self-absorption effect Fγ are calculated by theoretical formulas.
Due to the instability of the intensity of the D-beam generated by the ion source in the 3 MV tandem accelerator as well as the divergence of the beam point striking the target, it is inevitable that the neutron fluence will fluctuate during the neutron irradiation process. Therefore, based on the neutron fluence real-time detection system of the BF3 neutron counter meter (the real-time monitoring result of the stability of the neutron fluence in the laboratory lobby is presented in Fig. 6), Ff is determined according to the following equation:
$ {F_f} = \frac{{\displaystyle\sum\limits_{i = 1}^{i = n} {{\varphi _i}(1 - {{\rm e}^{ - \lambda {t_i}}}){{\rm e}^{ - \lambda {T_i}}}} }}{{\displaystyle\sum\limits_{i = 1}^{i = n} {{\varphi _i}{t_i}/T(1 - {{\rm e}^{ - \lambda T}})} }}, $
(8) where T is the total neutron irradiation time, which is divided equally into n parts, and ti represents the irradiation time of the i-th interval taken arbitrarily. Ti is the time interval ranging from the starting moment of ti+1 to the termination of the neutron irradiation. λ is the decay constant of radionuclides 198Au or 239Np.
The interactions of γ-rays with the substance when the characteristic γ-rays generated after irradiation pass through the sample with a limited thickness contribute to the γ-ray self-absorption effect. Fγ is obtained by the equation below:
$ {F_\gamma } = \frac{{{\mu _m}{t_m}}}{{1 - {{\rm e}^{ - {\mu _m}{t_m}}}}}, $
(9) where the parameters tm and µm originate from the NIST-XCOM [35] data and indicate the mass thickness in g/cm2 and the mass attenuation coefficient in cm2/g, respectively. The mass attenuation coefficient of the 411.8 keV γ-ray is 0.1919 cm2/g in the Au sample, and that of the 277.6 keV γ-ray is 0.5018 cm2/g in the U3O8 sample.
In the experiment, the scattered neutrons and the scattering effect interfere with the experimental results to a certain extent when the neutrons emitted from the accelerator cross the layers of cooled water and the tube wall material of the target head. Therefore, the Monte Carlo program GEANT4 is used to simulate and calculate this [6, 30, 36]. The number of target radionuclides Nr was calculated firstly under the actual conditions (the presence of the surrounding materials). Afterwards, Nl was calculated for under ideal experimental circumstances, for which the layers of cooled water and the tube wall material of the target head were neglected. The radionuclide decay effect caused by time is not considered. Consequently, FS = Nr /Nl is derived as the correction factor for low-energy scattered neutrons.
The standard sources used in the calibration of the detection efficiency of the high-purity germanium γ-spectrometer system are point sources, but in practice, it is impossible to neglect the influence on the measured counts of the γ-spectrometer due to the large geometry of the samples (ϕ = 20 mm). Therefore, the counting geometric correction factor Fg = Nd /Nm, where Nd, Nm are the γ-ray counts of the simulated point source and the real sample size in the Monte Carlo program, respectively.
Indeed, the partial neutrons are progressively attracted by the sample itself via nuclear reactions when neutrons cross a sample with finite thickness, resulting in an attenuation of the neutron fluence. The sample is separated into n equal parts in order to work out the neutron self-shielding effect Fa. Suppose that the numbers of radionuclides generated in each part are N1, N2, ..., Ni, ..., Nn [6]; accordingly, the neutron fluence attenuation coefficient is given by the following equation:
$ {F_a} = \frac{{n{N_1}}}{{\displaystyle\sum\limits_{i = 1}^{i = n} {{N_i}} }}. $
(10) Ultimately, Fall is formulated according to the following equation, and the results are presented inTable 2.
En/MeV $ \dfrac{{{F_{\gamma U}}}}{{{F_{\gamma\rm Au}}}} $ $ \dfrac{{{F_{sU}}}}{{{F_{s \rm Au}}}} $ $\dfrac{ { {F_{aU} } } }{ { {F_{a\rm Au} } } }$ $\dfrac{ { {F_{fU} } } }{ { {F_{f\rm Au} } } }$ $\dfrac{ { {F_{gU} } } }{ { {F_{g\rm Au} } } }$ Fall 6.117 ± 0.119 1.2181 1.0535 0.9351 0.9657 0.9892 1.1463 4.626 ± 0.086 1.2184 0.9867 0.9628 1.0245 0.9814 1.1638 3.622 ± 0.348 1.2170 0.8879 1.0205 1.0245 0.9833 1.1109 Table 2. Summary of a variety of experimental correction results.
$ {F_{\rm all}} = \frac{{{{({F_f} \cdot {F_\gamma } \cdot {F_s} \cdot {F_a} \cdot {F_g})}_U}}}{{{{({F_f} \cdot {F_\gamma } \cdot {F_s} \cdot {F_a} \cdot {F_g})}_{\rm Au}}}}. $
(11) -
The uncertainty analysis of the nuclear reaction cross-sections is one of the essential indexes to evaluate the cross-section data in cross-section measurement work. With an increasing demand for accuracy in various experimental cross-section data and the improvement of experimental instruments, the uncertainty of cross-sectional data should be urgently mitigated [37]. The main sources of error in this experiment are systematic and statistical uncertainties. According to formula (6), the uncertainties of the cross-section results consist primarily of the statistical errors of the full-energy peak net counts (AAu, Au) of the characteristic γ-rays, calibration errors of the detector (ξ = εAu/εu), errors in the value of σAu as the standard cross-section, errors in the intensities of the γ-ray (Iu), and errors in the radionuclide half-lifes (T1/2). Due to mutual independence between these parameters, the overall uncertainties of the experimental measurements in terms of the following equations are available.
$\begin{aligned}[b]\\[-5pt] \frac{{\Delta {\sigma _u}}}{{{\sigma _u}}} = \sqrt {{{\left(\frac{{\Delta {\sigma _{\rm Au}}}}{{{\sigma _{\rm Au}}}}\right)}^2} + {{\left(\frac{{\Delta \xi }}{\xi }\right)}^2} + {{\left(\frac{{\Delta {I_u}}}{{{I_u}}}\right)}^2} + {{\left(\frac{{\Delta {A_{\rm Au}}}}{{{A_{\rm Au}}}}\right)}^2} + {{\left(\frac{{\Delta {A_u}}}{{{A_u}}}\right)}^2} + {{\left(\frac{{\Delta {T_u}}}{{{T_u}}}\right)}^2} + {{\left(\frac{{\Delta {T_{\rm Au}}}}{{{T_{\rm Au}}}}\right)}^2}} .\end{aligned}$ (12) The uncertainties in the half-life ∆T1/2 of the radionuclides 198Au and 239Np arise from the ENSDF Library [38]. The relative standard uncertainties of σAu are derived from ENDF/B-VIII.0. The total uncertainties are determined in the region from 3.478% to 7.450% and summarized in Table 3.
${E_n}/\rm MeV$ Relative uncertainty ∆x/x (%) $\dfrac{ {\Delta {\sigma _{\rm Au} } } }{ { {\sigma _{\rm Au} } } }$ $ \dfrac{{\Delta \xi }}{\xi } $ $ \dfrac{{\Delta {I_u}}}{{{I_u}}} $ $\dfrac{ {\Delta {A_{\rm Au} } } }{ { {A_{\rm Au} } } }$ $ \dfrac{{\Delta {A_u}}}{{{A_u}}} $ $\dfrac{ {\Delta {T_u} } }{ { {T_u} } }$ $\dfrac{ {\Delta {T_{\rm Au} } } }{ { {T_{\rm Au} } } }$ $ \dfrac{{\Delta {\sigma _u}}}{{{\sigma _u}}} $ 6.117 ± 0.119 7.094 0.612 0.551 1.950 0.835 0.004 0.007 7.450 4.626 ± 0.086 4.450 0.612 0.551 0.912 1.392 0.004 0.007 4.822 3.622 ± 0.348 2.469 0.612 0.551 1.456 1.790 0.004 0.007 3.478 Table 3. Summarized relative uncertainty for each parameter as well as experimentally measured cross-sectional values ∆x/x (%).
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In the current study, the reaction cross-sections of 238U (n, γ)239U have been determined employing the relative activation approach at neutron energies of 6.117 ± 0.119 MeV, 4.626 ± 0.086 MeV, and 3.622 ± 0.348 MeV. A summary of the experimentally measured cross-section values and the corresponding uncertainties at the corresponding energies is presented in Table 4. The reaction cross-sectional values of 238U (n, γ)239U derived from the ROSFOND-2010, CENDL-3.2, and ENDF/B-VIII.0 evaluation databases in the 0.8–12 MeV energy region are plotted in Fig. 7 together with the experimental measurements.
En/MeV $ {\sigma _u}/\rm mb $ $ \Delta {\sigma _u}/\rm mb $ 6.117 ± 0.119 1.051 0.078 4.626 ± 0.086 4.437 0.214 3.622 ± 0.348 11.960 0.416 Table 4. Summary of experimental cross-sectional measurements and their uncertainties.
Figure 7. (color online) Graphical representation of experimental, evaluated, and theoretically calculated cross-sectional values for 238U (n, γ)239U reaction.
Theoretical calculations of nuclear data are an essential part of the nuclear data measurement and assessment process. TALYS-1.9 is the computational code used to simulate and analyze various nuclear reactions by means of established physical models and optimized parameter settings. The model structure and parameters are taken from the RIPL library [39]. It can calculate the nuclear reactions of a variety of incident particles (n, p, t, 3He, γ, α) with an energy between 0–200 MeV for a target nucleus mass number from 12 to 339. Moreover, it is available with a variety of required information including all cross-sections and each reaction channel cross-section as well as angular distributions and double differential cross-sections of the emitted particles. Therefore, the TALYS-1.9 program is used to perform theoretical simulation calculations of the reaction cross-section of 238U (n, γ)239U in the present work. The theoretical calculation results of the 238U (n, γ)239U reaction cross-section with neutron energies ranging from 0.8 to 12 MeV are illustrated in Fig. 7.
It can be clearly demonstrated that there are significant differences between the evaluation databases for the neutron energies in the range of 3.0–7.0 MeV. Within this energy region, the experimental values of Panitkin et al. [24] are more compatible with the cross-sectional values of the database CENDL-3.2 and superior to those of ROSFOND-2010 and ENDF/B-VIII.0. In addition, the results of this experiment at neutron energies of 3.622 ± 0.348 MeV, 4.626 ± 0.086 MeV, and 6.117 ± 0.119 MeV are in accordance with the evaluation data of ENDF/B-VIII.0 but marginally higher and in general agreement with the theoretical calculation results of TALYS-1.9. Moreover, the trend shown differs from those of the
evaluation databases of CENDL-3.2 and ROSFOND-2010, which clarified the variances between the evaluation databases. In addition, the experimentally measured value is in agreement with the experimental result of H.Naik et al. [20] at 3.622 MeV. From the evaluation data, the neutron capture cross-section of 238U declines sharply from 0.8 to 7.5 MeV before rising progressively. The valleys generated are primarily ascribed to the 238U (n, 2n) 237U reaction [4, 6, 7, 10, 17]. In the range of the neutron energy 0.8–6 MeV and 8–12 MeV, the theoretical calculation data obtained by the initially parameterized TALYS-1.9 are marginally superior to those obtained using the ENDF/B-VIII.0 and ROSFOND-2010 evaluation databases; however, they are inferior to the evaluation data in the 6–8 MeV energy region.
Cross-sections of the 238U (n, γ) 239U reaction in the 3.0–7.0 MeV energy region measured by relative activation method
- Received Date: 2022-09-06
- Available Online: 2023-02-15
Abstract: The reaction cross-sections of 238U (n, γ)239U have been experimentally determined at neutron energies of 6.117 ± 0.119 MeV, 4.626 ± 0.086 MeV, and 3.622 ± 0.348 MeV employing the relative activation approach along with the off-line γ-ray spectroscopy method. The D (d, n)3He reaction was utilized to obtain monoenergetic neutrons of the required energy, and the 197Au (n, γ)198Au reaction cross-sections were adopted as the referential standard to ascertain the neutron capture cross-sections of 238U. Furthermore, the effects of low-energy scattered neutrons, neutron fluence fluctuations, counting of geometric corrections when measuring γ-rays, and neutron and γ-ray self-absorption caused by the sample thickness have been considered and revised in the present work. For a comparison with experimental results, the cross-sections of the 238U (n, γ)239U reaction were calculated theoretically with the original parametric TALYS-1.9 program. The experimental measurements were in contrast to previous experimental results and the evaluation data available for ROSFOND-2010, CENDL-3.2 and ENDF/B-VIII.0.