1. Introduction
With today’s extensive use of radiation sources and radioactive materials, it is extremely essential to use radiation sources cautiously and safely. Against gamma radiation, the most utilized shielding materials are lead (Pb) and lead-equivalent compounds. However, Pb’s negative impacts on human health and the environment pose a serious concern. Subsequently, it has some disadvantageous material properties, such as optical non-transparency, low durability, high cost, and material durability in terms of shielding applications [
1]. Another material used to attenuate gamma radiation is concrete. Its most serious shortcomings, however, are that it is exceedingly heavy, pricey, opaque, and cracks when overused [
2]. In recent years, researchers have been attempting to investigate the features of eco-friendly, very dense, and chemically homogeneous materials that could be utilized as a replacement for concrete and lead. Corrosion-resistant, biocompatible radiation shielding systems must be created that can be modelled into narrow, compact forms with outstanding structural integrity and endurance. Glass has been proven to be an efficient shielding material due to its transparency to visible light, ease of production, and ease of property change through composition and preparation techniques. Glasses are one of a kind in that they can handle a wide variety of elements. They can act as a shield against hazardous ionizing radiation because of this characteristic. Impurities in the form of metals were incorporated into regular glass to transform it into a radiation shield glass. This doping, especially with heavy metal oxides (Ba, Bi, Pb), enhances the glass’ attenuation properties, making it ideal for shielding applications. Glass formers are oxides that serve as the structural backbone of the glass network and are needed for optimal operation. As potential substitutes, borate glasses and lead-free compounds with adequate chemical resistance, transparency, and radiation protection are being investigated [
3]. Borate-based glasses have a higher melting point and resistance to temperature changes than other types of glasses. Because of their high solubility of rare earth ions, ease of mass production, and low cost, bore-based glasses are the greatest choice for developing new optical devices. Borate-based glass systems have good broad-band properties and demonstrate significant increases in luminescence intensity. Doping transition metal and rare earth ions into borate glasses improves optical transmittances, electric conductivities, thermal, and even magnetic characteristics [
4,
5,
6]. Pb-based glasses are particularly fascinating due to their strong electrical conductivity, stability, and wide glass-forming range. Strong UV transmittances, low melting and glass transition temperatures, and great thermal stability are all advantages of Pb-based glasses [
7,
8]. According to a study conducted by Tekin et al. [
9], phosphate-based glasses are ideal for the fabrication of optical fibres and shielding material for radiation detection, among many other applications. Agar et al. [
10] conducted another significant study which revealed that doping glasses with erbium (Er) leads to an increase in the mass attenuation coefficient and a decrease in build-up factors and half-value layer. Subsequently, glasses doped with Er possess significant radiation-shielding properties. The goal of this novel study is to determine the nuclear-radiation-shielding properties of glass samples from the 10La2O3–50HMO–(40–x) B
2O
3–xEu
2O
3 (x = 0, 0.5, 1 and 2 mol percent and HMO = PbO, Bi
2O
3) system in a wide range of energies between 0.015 and 15 MeV using the MCNPX (version 2.7.0) general-purpose Monte Carlo code [
11] and Phy-X/PSD [
12] software. It also aims to establish the materials’ mechanical qualities, as well as their suitability as shielding materials. The results of this study will be useful in the field of glass literature, notably in the field of radiation shielding. Researchers will gain a better understanding of the utility of HMO-doped glasses as nuclear-radiation-shielding materials as a result of the findings of this study.
3. Results and Discussions
In this study, a comprehensive investigation on high-amount heavy metal oxide (HMO)-added and Eu
3+-activated borate glasses based on 10La
2O
3–50HMO–(40–x)B
2O
3–xEu
2O
3 (x = 0, 0.5, 1 and 2 mol% and HMO = PbO, Bi
2O
3) system was carried out in terms of their individual and comprehensive gamma-ray and charged particle attenuation competencies. In total, eight different glass samples, encoded LPb50B, LPb50Eu0.5, LPb50BEu, LPb50BEu2, LBi50B, LBi50Eu0.5, LBi50Eu1, and LBi50Eu2, were classified considering HMO type in their structure. Material densities and chemical properties of the aforementioned glasses can be obtained from
Table 1. It is clearly seen that material densities of PbO-reinforced borate glasses varied from 5.043 g/cm
3 to 5.393 g/cm
3, whereas material densities of Bi
2O
3-reinforced borate glasses varied from 5.940 g/cm
3 to 6.812 g/cm
3. In the glass structure, (40–x)B
2O
3–xEu
2O
3 indicates that, in both glass groups, B
2O
3 has been replaced with Eu
2O
3 from 0 to 2 mole%. Therefore, one can say that Bi
2O
3 contribution (as 50% mole) has increased the material density more than PbO contribution in terms of their HMO structures. To begin, we calculated the mass attenuation coefficients (MAC) of the aforementioned glass samples using the MCNPX code, and then compared them to theoretical findings obtained using the Phy-X/PSD program. In
Table 2, the findings of both techniques are listed, together with their respective relative variances. Additionally,
Figure 2 illustrates the variation in the MAC values of the investigated glasses throughout the energy range 0.015–15 MeV. From
Table 2, it is seen that the MAC values of LPb50B and LPb50BEu2 glasses vary between 78.429 cm
2/g–0.045 cm
2/g and 79.045 cm
2/g–0.045 cm
2/g, while the MAC values for LBi50B and LBi50Eu2 glasses are between 89.281 cm
2/g–0.048 cm
2/g and 89.442 cm
2/g–0.048 cm
2/g. It is noticed from
Figure 2 that the MAC values decrease rapidly at 0.015–0.1 MeV photon energies, and increase suddenly before reaching 0.1 MeV. This rapid drop is due to the impact of photoelectric absorption (PEA) in the low energy region and the changing in cross-section of interaction with 1/E
3.5 in that zone. Besides, a sudden increase occurred around 88.00 keV and 90.52 keV, which are the absorption edges of Pb and Bi heavy elements in two glass systems, since the cross-section of PEA is proportional to Z
4−5. It is regarded that the reduction in MAC values is slower at medium energies where the Compton scattering (CS) process (Z/E) is powerful. It is remarkable that after 1.022 MeV, where pair production (PP) occurs, the MAC values increased slowly with increasing energy. At high energy levels, most photons are annihilated, and MAC values vary depending on Z
2. Therefore, the MAC values of glasses containing Bi and Pb elements with high Z at high energies increased. With the addition of Eu
2O
3 (0, 0.5, 1, 2 mol%), the MAC values are obtained at 0.015 MeV as 78.429 cm
2/g, 78.586 cm
2/g, 78.742 cm
2/g, and 79.045 cm
2/g and 89.281 cm
2/g, 89.322 cm
2/g, 89.362 cm
2/g, and 89.442 cm
2/g for LPb50B and LBi50B glass systems, respectively. From this, it can be deduced that the insertion of Eu
2O
3 increases MAC values in both glass systems, and the higher MAC values are obtained in glasses prepared with Bi
2O
3. The material thickness of LPb50BEu and LBi50BEu glasses for 0.015–15 MeV photon energies, which halves the incoming radiation intensity, is presented in
Figure 3.
Half-value layers (T
1/2) of the LPb50BEu and LBi50BEu glasses are almost zero in the 0.015–0.1 MeV range. After 0.1 MeV, secondary scattering enhances with the effect of CS, while the T
1/2 values increase quickly. Beyond 3 MeV, the T
1/2 values reduce with the annihilation of photons in the PP process. The densities of LPb50BEu and LBi50BEu glasses are reduced in the range of 5.39–5.04 g/cm
3 and 6.81–5.94 g/cm
3 with the addition of Eu
2O
3. Therefore, it is seen that the T
1/2 values increase with the insertion of Eu
2O
3. The maximum T
1/2 values for LPb50BEu and LBi50BEu glasses were obtained as 3.60 cm and 2.95 cm, respectively. These results are quite satisfactory for a good shield material for gamma rays. Moreover, the mean free path values (λ) of proposed glasses in comparison with some commercial SCHOTT [
17] glasses, RS-253-G18, RS-360, RS-520, and concrete types, barite, ferrite, chromite [
18], are given in
Figure 4.
The λ values of LPb50BEu and LBi50BEu glasses are thinner than other shielding materials. The LBi50BEu2 glass had the smallest λ values, while the RS-213-G18 glass presented the largest MFP values, as seen in
Figure 5. In order to express a composite material with a single atomic number, an effective atomic number (
Zeff) is needed, which shows the shielding capacity of the shielding material well [
19].
Figure 6 presents the change of
Zeff values of L (Bi/Pb)50BEu2 glasses versus photon energy. For LPb50BEu and LBi50BEu glasses, the
Zeff takes values in the range of 76.72–23.15, 75.73–23.84, and 79.64–27.71, 79.38–28.18, respectively. The largest values of
Zeff are at low energies below 0.1 MeV. A few sudden peaks occur on the absorption edge of K and L shells of Pb (L:15.86 keV, K:88.00 keV) and Bi (L:16.38 keV, K: 90.52 keV), and K shell of La (38.92 keV) by the effect of PEA. Between 0.1–1 MeV, the
Zeff values rapidly decrease and, beyond 1 MeV, the
Zeff values increased due to the Z
2-dependent change of the PP cross section. While the addition of Eu
2O
3 in the high energy region increased the
Zeff values of the glasses, the
Zeff values declined at medium and low energy levels. It is noted from
Figure 6 that the
Zeff values of LBi50BEu glasses prepared with Bi
2O
3 are higher than LPb50BEu glasses. Perfect geometry is not possible in real radiation applications. For this reason, the correction factor B (build-up factor) is needed to account for scattering in the material and in the air in the Lambert–Beer law [
20]. Energy absorption and exposure build-up factors (EABF and EBF) for L(Pb/Bi)50BEu glasses were generated using Phy-X/PSD software in photon energies of 0.015–15 MeV for several λ values.
Figure 7 and
Figure 8 visualise the trend of change of the EBF and EABF values of the glasses versus the photon energy and
Table 3,
Table 4,
Table 5,
Table 6,
Table 7,
Table 8,
Table 9 and
Table 10 presented G–P fitting coefficients, respectively. In the low energy range (0.015–0.1 MeV), it is seen that there are very sharp peaks around 0.02 MeV, 0.04 MeV, and 0.1 MeV, which are the L and K absorption edges of the Pb and Bi elements and the K shell absorption edge of La. The high Z values of the relevant elements increase the possibility of PEA interaction and cause the photons to become built up. The EBF and EABF values of LBi50BEu glasses are considerably lower than those of LPb50BEu glasses at lower energies. Since the
Zeff values of the glasses are very large, the EBF and EABF values for all glasses possess the smallest values (nearly zero) in the CS process proportional to Z. In the range of 1–15 MeV, since the PP interaction cross-section is dependent on Z
2, especially when the depth of penetration increases, photon build-up enhances with secondary scatterings. As a result, the EBF and EABF values for all glasses start to boost again at high energies. It is clear from
Figure 7 and
Figure 8 that the EBFs of the glasses are higher than the EABFs.
When all gamma-shielding parameters are evaluated together, the LBi50BEu glasses show a superior performance compared to LPb50BEu glasses in reducing photons. Besides, the protection capability of L(Pb/Bi)50BEu glasses against uncharged (fast neutrons) and charged particles (alpha and protons) was also evaluated. For this purpose, the macroscopic removal cross-section (ΣR) of glasses for fast neutrons was calculated firstly.
In
Figure 9,
ΣR values of both groups of glasses are established. In both glass systems, the
ΣR values decreased as the density decreased with the addition of Eu
2O
3. The
ΣR values of LPb50BEu glasses were 0.10106 cm
−1, 0.09999 cm
−1, 0.09478 cm
−1, and 0.09286 cm
−1, respectively, while, for LBi50BEu glasses, they were found to be 0.11484 cm
−1, 0.11428 cm
−1, 0.09745 cm
−1, and 0.09921 cm
−1. It appears that the LBi50BEu glass system is more effective at capturing neutrons than others. It is clear that selected glass systems are also successful at reducing neutrons when compared to water and paraffin (
ΣR = 0.101 cm
−1), which are traditional neutron moderators. As the charged particle moves through the material, it interacts with the atomic electrons in the material and its energy decreases. However, during this time, the stopping power increases because the kinetic energy of the particle is inversely proportional to the stopping power. The change of the mass stopping power (AMSP and PMSP) of L(Pb/Bi)50BEu glasses versus the photon energy for alpha and proton particles is given in
Figure 10. While the charged particles move in the glass in the form of a Bragg curve, and the curve increases proportionally with 1/E, there is a sharp decrease in the curve at the end of the path where the particle travels through the matter. Since alpha particles are heavier than protons, they have reached the maximum MSP at higher energies. Since the stopping power of the material is proportional to the square of the atomic number, LBi50BEu glasses with larger
Zeff values have higher MSP values. The furthest distance that the charged particles can travel through the material is expressed as the projected range (PR).
Figure 11 presents the change of APR and PPR values of L(Pb/Bi)50BEu glasses in response to kinetic energy. Since the addition of Eu
2O
3 reduces the
Zeff values, PR is larger in glasses with 2 mol% Eu
2O
3 added. Since protons are smaller in mass, they move faster and have a longer range inside the glass (PPR > APR). The PRs of alpha and proton particles are shorter in LBi50BEu glasses.
Finally, it is worth noting that the linear attenuation coefficients determined using Phy-X/PSD and MCNPX (2.7.0) were very consistent.
Figure 12 depicts a comparison of obtained linear attenuation coefficients from MCNPX Monte Carlo code and Phy-X/PSD for the LBi50B sample. A relative difference of 2% was reported at 0.02 MeV photon energy. Overall, our findings showed that relative differences were varied from 1.15% to 2.6% at all photon energies. Both outcomes were reported in comparable linear attenuation coefficient values, based on our results. However, minor variations in certain energy areas were discovered. This is closely linked to the tools employed, since MCNPX is a Monte-Carlo-based technique for radiation transport that needs user specification at different stages of the process described before. By contrast, Phy-X/PSD is a web-based tool that requires just the material composition, density, and energy quantities. As a result, some differences are almost certainly due to a variety of variables, including the number of dispersed gamma rays entering the detecting field, the narrow beam shape, the cross-section libraries and physics lists, the hardware performance, and the CPU characteristics of the computers used.