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Results in Physics
journal homepage:www.elsevier.com/locate/rinp
Synergistic e
ffect of La
2
O
3
on mass stopping power (MSP)/projected range
(PR) and nuclear radiation shielding abilities of silicate glasses
O. Kilicoglu
a,f, E.E. Altunsoy
b,f, O. Agar
c, M. Kamislioglu
a, M.I. Sayyed
d, H.O. Tekin
e,f,⁎,
Nevzat Tarhan
g,haUskudar University, Department of Nuclear Technology and Radiation Protection, Istanbul 34672, Turkey bUskudar University, Vocational School of Health Services, Medical Imaging Department, Istanbul 34672, Turkey cKaramanoglu Mehmetbey University, Department of Physics, 70100 Karaman, Turkey
dUniversity of Tabuk, Physics Department, Tabuk, Saudi Arabia
eUskudar University, Vocational School of Health Services, Radiotherapy Department, Istanbul 34672, Turkey fUskudar University, Medical Radiation Research Center (USMERA), Istanbul 34672, Turkey
gNPIstanbul Hospital, Department of Psychiatry, Istanbul, Turkey
hUskudar University, Faculty of Humanities and Social Sciences, Department of Psychology, Istanbul, Turkey
A R T I C L E I N F O Keywords: Radiation shielding La2O3 Silicate glasses MCNPX MSP PR A B S T R A C T
Photon and neutron attenuation properties of La2O3based Li2O-SiO2-La2O3 glass system have been evaluated
through MCNPX (2.6.0) Monte Carlo code at some photon energies of 0.256–1.33 MeV. In order to control the accuracy of the data, the estimated MCNPX of mass attenuation coefficients have been compared to those of WinXCOM software. The half value layer (HVL), tenth value layer (TVL) and mean free path (MFP) values of the selected glass system exhibited that the shielding performance of the gamma photons is related to the density of glass, thus, the inclusion of TeO2to Li2O-SiO2improves the capacity of the glass system to attenuate more
photons. In addition, the effective removal cross-section (ΣR) calculations have been done. Further, Mass sop-ping power (MSP) and Projected range (PR) are calculated for proton particles (H1) and alpha particles (He+2). It
may be deduced that La4 glass among the studied samples may be kept in view as a superior glass in terms of shielding for photon and neutron while La0 glass can be considered as a best shielding material against to alpha and proton particles. The results of this study may be useful for shielding optimization of medical and industrial facilities.
Introduction
Lead (Pb) and other traditional materials as shield against to high energetic ionizing radiation possess some drawbacks namely toxic, expensive, heaviness for storage and transportation [13]. Therefore, there has been growing works on radiation attenuation characteristics for new and alternative material[1,2,4,9,15,25]. However, the trans-parency gives a superior and desired property to a material. Such ma-terial is extremely innovative in terms of radiation shielding. Recently, many researchers have studied experimental, theoretical and compu-tational studies on the radiation absorption properties of glass [3,10,22,28,33,34]. Among the diverse glasses containing oxides (e.g., B2O3, GeO2, P2O5,), silicate (SiO2) is one of significant glass former due to their low attenuation losses and excellent transmission in the visible and the near infrared region and broadly used in optics for tele-communication practices[16]. In addition, the transition temperature
(Tg) can be enhanced and thermal expansion coefficient can be de-creased with the insertion of alkali modifier (e.g., Li2O) to a silicate network[12]. Rare-earth (RE) ion incorporated glass systems are ex-amined in detail by various investigators for their practices in different optoelectronic apparatus [8,20,21]. Lanthanum oxide (La2O3) with high refractive index, enhanced alkali resistance, lower cost among rest of RE oxides and high Abbe number plays an significant modifier in the glass industry[17]. In this context, the Li2O-SiO2-La2O3glass system may be a good choice in order to shield ionizing radiation. Any study on radiation shielding characteristics of Li2O- SiO2- La2O3glass system has not been found in literature. The present paper aims towards evaluating not only photon and neutron but also the alpha and proton attenuation properties for the present glasses. The obtained simulation results for mass attenuation coefficients have been approved with those of theo-retical.
https://doi.org/10.1016/j.rinp.2019.102424
Received 9 May 2019; Received in revised form 5 June 2019; Accepted 5 June 2019
⁎Corresponding author at: Uskudar University, Vocational School of Health Services, Radiotherapy Department, Istanbul 34672, Turkey.
E-mail address:huseyinozan.tekin@uskudar.edu.tr(H.O. Tekin).
Available online 08 June 2019
2211-3797/ © 2019 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/BY-NC-ND/4.0/).
Materials and methods
This study deals with glasses including the different rate of Li2 O-SiO2-La2O3in the composite. The structural features of Li2O-SiO2-La2O3 glass system have previously obtained by Gaddam et al.[17]and the experimental glasses with the general molar composition xLa2O3−(100−x)(26Li2O−74SiO2), with x = 0, 0.9, 2.6 and 4.3 mol %, in their paper have considered. These glasses have been tabulated in Table 1.
Theoretical framework of radiation shielding calculations
Gamma-ray (known as Gamma-radiation) is an electro-magnetic radiation deriving from high energy photons in the electromagnetic spectrum. As a very penetrating occurrence, a shielding material has to be used in the process of interaction occurring between matter and gamma-ray. The three mechanisms that are generally used in the lit-erature are photoelectric effect, Compton scattering and pair produc-tion.
The LAC is a quantity referring absorbed photons by the per unit thickness for the shielding absorber. Thus, this thickness plays an im-portant role in shielding calculation. However, LAC for all types of material comes with two fundamental results. First, the LAC increases as the atomic number of the absorber increases. Secondly, it decreases with the energy of the gamma rays. Therefore, the LAC is related to atomic number along with density, thickness of the material and in-cident photon energy.
The LAC is calculated using the Lambert-Beer rule as given below;
⎜ ⎟ = ⎛ ⎝ ⎞ ⎠ LAC μ ρ ρ (1)
wherewi is the proportion by weight and
( )
μρ ithe MAC of the i
th ele-ment.
The mass attenuation coefficients (MAC), denoted by µ/ρ, are used for calculating the penetration of photons in shielding materials[11]. It means that MAC basically corresponds the count of photons interacted with the shielding materials. Eventually, it is an important parameter for radiation shielding and it shows information on attenuationfirst and foremost depending on the atomic structure of the material.
The µ/ρ values of the compound is given by the following mixture rule[30]:
∑
⎛ ⎝ ⎜ = ⎞ ⎠ ⎟ μ ρ/ w μ ρ( / ) i i i (2) wherewishows the fractional weights of the individual elements, Theµ/ρ value at a certain energy of an element is obtained from WinXCOM software[18].
Adjusting the thickness of the shielding material, a better shielding feature can be provided. Half-value layer (HVL) for any material is known as the shielding material’s thickness at which penetrating ra-diation level is reduced by a factor of one-half. Similarly, tenth value layer (TVL) corresponds to the thickness of a shielding material at which attenuating radiation level is decreased by a factor of one tenth of the initial level. Since the penetration of the gamma-ray through all variants of thicknesses and density of the samples can be easily
determined, HVL and TVL are widely used in the shielding design. Actually, HVL and TVL are both of the appropriate parameters that characterize the effectiveness of shielding properties of a given mate-rial. It is frequently employed in calculations for both the penetrating ability of shielding materials. Similar to the attenuation coefficient, HVL and TVL are related to the amount of photon energy. Therefore, increasing photon energy level results with increasing HVL and TVL.
In order to estimate HVL and TVL, the following equations can be used[5,19]: = HVL μ 0.693 (3) and = TVL μ 2.303 (4) whereμ (cm−1) denotes linear attenuation coefficient.
Mean free path (MFP) is another quantity which determines the ability of shielding material and denotes the average distance that a molecule travels between sequential collisions. The MFP is derived from the following formula[7]:
= MFP
μ 1
(5) Zeff, refers to the number that represents total electron numbers surrounding the nucleus. It also depends on the photon energy likefixed atomic numbers and so, the amount of energy plays a significant role in Zeffcalculation. Zeff can be estimated through the total atomic cross section (σa) and the total electronic cross section (σe)[6]:
=
Z σ
σ
eff a
e (6)
The removal cross-section (ΣR) expresses the possibility that a fis-sion or fast energy neutron passes on a primary collifis-sion, which re-moves it from the group of penetrating, uncollided neutron. This quantity for the investigated glass systems were computed as follows [14]:
∑
=∑
W(∑
/ )ρ R i i R i (7) where Wiand∑R/ρrepresent the partial density (g/cm3) and the re-moval cross-section (cm2/g) of individual element.Stopping power is used to describe the physical nature of the energy transmitted to the sample. In fact, this describes the energy loss of the particle over the length it moves in the example that is simply refers to the speed at which energy is transferred from the beam to the sample [23].
In order to detect the particles and examine their properties, they must interact with the substance. The most important interaction pro-cess is electromagnetic interactions. Heavy charged particles (proton, alpha) behave according to the Bethe-Bloch theory [37]. Nuclear stopping power of the charged particle with the nucleus of the atom is given by Eq.(8).
−dE dx/ =Se+Sn (8)
where the minus sign indicates that the charged particle will lose its kinetic energy. Se: electronic stopping power, Sn refers to nuclear stopping force. Mass stopping power of the medium for a charged particle depends on the mass load and speed of the ion. The electron stopping power is similar to the interaction of charged particles with orbital electrons. Nuclear stopping power is specific to electron radia-tion [35,36]. SRIM is a mathematical program that computed the stopping and ion range of matter (10 eV-2 GeV/amu) into substance using quantum mechanical properties of ion-atom collisions. Mass stopping power is showed that decrease of kinetic energy while passing through the ionized particles.
Table 1
Chemical compositions (mol%) and densities (g/cm3) of the studied glasses.
Li2O SiO2 La2O3 ρ
La0 26 74 0.0 2.327
La1 25.8 73.4 0.9 2.426
La3 25.3 72.1 2.6 2.638
MCNPX (version 2.6.0) Monte Carlo code
Monte Carlo N-Particle Transport Code System-eXtended (MCNPX) [31]simulations have been implemented out to model a 3 × 3 inch NaI (Tl) detector[32]. The studies in literature show that MCNPX general-purpose code has been employed for characterization of various types of glassy systems in different studies[26,29,27,34,24]. The structure of
simulation layout for attenuation calculation including various equip-ments such as a 3 × 3 inch NaI (Tl) detector, a radioactive point iso-tropic source, Pb shielding for detector to intercept the back-scattered photons and an attenuator material against gamma ray photon have been defined. The detailed cross-sectional view and 3-D view of 3 × 3 inch NaI (Tl) acquired from a visualization tool has illustrated inFig. 1. More detail can be found in previous studies.
Fig. 1. 3-D view of modeled 3 × 3 inch NaI(Tl) detector obtained from MCNPX Visual Editor (VE X_22S).
Fig. 2. Mass attenuation coefficients of investigated glasses as a function of photon energy (MeV).
Table 2
The mass attenuation coefficients (μ/ρ) of studied glasses.
La0 La1 La3 La4
Energy XCOM MCNPX XCOM MCNPX XCOM MCNPX XCOM MCNPX
0.256 0.11307 0.11261 0.11970 0.11209 0.13073 0.12672 0.14016 0.13496 0.356 0.09950 0.09822 0.10189 0.09790 0.10586 0.09810 0.10925 0.10077 0.511 0.08574 0.08415 0.08637 0.08049 0.08741 0.08160 0.08830 0.08180 0.662 0.07654 0.07560 0.07666 0.07423 0.07685 0.07280 0.07702 0.06978 1.173 0.05825 0.05668 0.05802 0.05521 0.05763 0.05267 0.05730 0.05092 1.275 0.05583 0.05357 0.05559 0.05210 0.05520 0.04954 0.05486 0.04878 1.333 0.05457 0.05220 0.05434 0.05074 0.05394 0.04745 0.05361 0.04618
Fig. 3. Half-value layer (HVL) of the glasses as a function of photon energy (MeV).
Fig. 4. Tenth-value layer (HVL) of the glasses as a function of photon energy (MeV).
Results and discussion
By utilizing the results derived from the WinXCOM software and the MCNPX code, the MAC values for the selected glasses were obtained in energy range of 0.02 to 20 MeV inFig. 2. And also,Table 2has been tabulated the obtained MAC values. This table reveals that the MAC values of all the chosen glass samples reduces sharply with the rise of the photon energy up to 0.1 MeV. The dominating process in this low energy range is the photoelectric event and the cross section is pro-portional to the atomic number as Z4–5. It means that the interaction of gamma-ray with matter, the interaction with photon energy and the selected glasses happens in the low energy region. In medium energy region starting at the 0.1 MeV, Compton scattering mechanism begins dominating the interaction and this event is a show case for a linear dependence between the cross-section of Compton scattering and atomic number. During these processes, the MAC values are the highest for La3 and La4 as shown inFig. 2.
Figs. 3 and 4illustrates the variations in HVL and TVL versus the photon energy of these glass systems. Even though like MAC, both HVL and TVL are related to the energy and rise as the energy increases contrary to the change in MAC and photon energy. As well-known, there is an inverse relationship between the values of HVL and TVL and the photon energy. However, it is worth to note that HVL and TVL are also dependent inversely on the density of the material. Therefore, La3 and La4 glasses with highest densities correspond to smaller values of HVL and TVL compared to other glasses.
Fig. 5 represents the MFP values for different xLa2O3−(100−x) (26Li2O−74SiO2), with x = 0, 0.9, 2.6 and 4.3 mol% La2O3in the en-ergy range between 0.02 and 20 MeV. From thefigure, it can be seen that MFP values for La0, La1, La3 and La4 are in the range of 0.1910–22.0324 cm, 0.1157–19.7395 cm, 00660–16.3584 cm and 0.0462–13.9967 cm respectively.
The variation in Zeff values also fundamentally depends on the photon energy and Fig. 6 shows this fact for the selected glasses. Shortly, the variation in Zeffis seperated into three energy regions viz. low, intermediate and high where occurs owing to different photon interactions. At the lower energies, photoelectric absorption is the dominating photon interaction mechanism. InFig. 6, this mechanism is dominant below 0.356 MeV and thus, the variation in Zeffis quite high. The Zeffvalues in the low energy region decrease suddenly simply be-cause none of the glasses possess heavy elements in their composition. In the intermediate energy region, the dominant mechanism is Compton scattering. As the Compton scattering begins dominating at the intermediate energy regions, the lowest value of Zeffwas found for
Fig. 5. Variation of mean free path (MFP) values of the glasses as a function of photon energy (MeV).
Fig. 6. Zeffvalues for glasses in the energy range 0.02–20 MeV.
Fig. 7. Variation of photon transmission values of the glasses as a function of glass thickness (cm).
the glasses. La3 and La4 in the selected glasses accompany with the highest Zeffvalues varying between 24.89 and 11.87 and 30.06–13.40. Between 0.511 MeV < E < 1.33 MeV the variation is almost constant
because of the Compton scattering process. Otherwise, pair production is the effective mechanism in the high energy region of 5 and 20 MeV. Hence, all variations are determined by the Z dependence of total atomic cross sections and the high Z elements derives from photo-electric absorption cross-section process. However, the Compton
Table 3
Effective removal cross sections for studied glasses.
La0 (density = 2.327 g/cm3) La1 (density = 2.426 g/cm3)
Element ∑R/ρ (cm2g−1) Fraction by weight (%) Partial Density (g cm−3) ∑R (cm−1) Fraction by weight (%) Partial Density (g cm−3) ∑R (cm−1)
Li 0.084 0.069102 0.160800 0.013507 0.065424 0.158719 0.013332
O 0.0405 0.532991 1.240270 0.050231 0.512333 1.242921 0.050338
Si 0.0285 0.397907 0.925930 0.026389 0.376570 0.913558 0.026036
La 0.0127 0.000000 0.000000 0.000000 0.045673 0.110803 0.001407
TOTAL 0.090127 0.091114
La3 (density = 2.638 g/cm3) La4 (density = 2.843 g/cm3)
Element ∑R/ρ (cm2g−1) Fraction by weight (%) Partial Density (g cm−3) ∑R (cm−1) Fraction by weight (%) Partial Density (g cm−3) ∑R (cm−1)
Li 0.084 0.059175 0.156104 0.013113 0.054018 0.153574 0.012900
O 0.0405 0.477946 1.260820 0.051063 0.448554 1.275238 0.051647
Si 0.0285 0.341180 0.900033 0.025651 0.310745 0.883447 0.025178
La 0.0127 0.121699 0.321043 0.004077 0.186684 0.530741 0.006740
TOTAL 0.093904 0.096466
Fig. 9. Proton mass stopping powers of variation as a function of kinetic energy for the selected (La0, La1, La3 and La4) samples.
Fig. 10. Alpha mass stopping powers of variation as a function of kinetic energy for the selected (La0, La1, La3 and La4) samples.
Fig. 11. Proton projected range as a function of kinetic energy for the selected (La0, La1, La3 and La4) samples.
Fig. 12. Alpha projected range as a function of kinetic energy for the selected (La0, La1, La3 and La4) samples.
scattering cross-section depends on Z, giving less weight to the high Z elements than photoelectric absorption and pair production mechan-isms. On the whole, Zefflies its maximum value at the lower energies (E < 0.356 MeV) where Z4dependence gives a heavy weight for the highest atomic number of the compound. In high energy region, typi-cally above 5 MeV, Zeffis again constant but smaller than those of va-lues in the low-energy range. This is resulting from the dominance of pair production, the cross section of which possesses a weaker Z2 de-pendence.
In order to evaluate the effectiveness of any shielding absorber, the photon transmission (%) values are a remarkable quantity. The trans-mission of the La-incorporated glasses is evaluated depending on glass thickness.Fig. 7 indicates the obtained transmission results. It is ob-vious from thisfigure that the transmission results are reduced with the increasing of thickness. One can be appeared that La4 glass has lowest TF values among the present glass samples, which illustrates that this sample possesses best performance in attenuating photon more com-pared to the rest of glasses (Fig. 8).
By estimating the effective removal cross sections (∑R, cm−1), it has been surveyed the role of La2O3concentration in La-doped glasses for fast neutron shielding.Table 3demonstrates theΣRvalues of La0-La4 glasses. It is clear fromTable 3that∑Rresults are near to each other and changed from 0.090127 (La0) to 0.096466 (La4) cm−1. This dissim-ilarity can be resulted from the density of the glass and thus, La4 glass sample has observed the highestΣRvalue.
The mass stopping power (MSP) of some Li2O-SiO2-La2O3glasses for proton and alpha particles is account by SRIM software program. MSP is a strong feature because it refers to decrease of the kinetic energy when passing through a certain density of lanthanum oxide samples.Figs. 9 and 10offered that the Li2O-SiO2-La2O3glasses (La0, La1, La3 and La4) have the smallest worth of proton and alpha stopping power, respec-tively. For example, the removal of protons and alpha ions having the highest energy with about 10 MeV energy, lanthanum oxide Li2O-SiO2 -La2O3 glasses for La0 to be of about 5.58 × 10−1MeVcm2/g and 1.55 × 100MeVcm2/g, respectively.
For lanthanum oxide Li2O-SiO2-La2O3 glasses the projected range (PR) values were calculated using SRIM encode in the proton particles (H1) and alpha particles (He+2). The PR consequences are plotted in Figs. 11 and 12. For example, the removal of protons and alpha ions having the highest energy with about 10 MeV energy, one canfind out the respective range in lanthanum oxide Li2O-SiO2-La2O3glasses for La0 to be of about 0.139 mm and 0.195 mm, respectively. The results showed that among the investigation lanthanum oxide Li2O-SiO2-La2O3 glasses La0 glasses has a superior value. The computation results has deduced that lanthanum oxide Li2O-SiO2-La2O3glasses is an excellent candidate for photon, neutron, proton and alpha shielding.
Conclusions
The MAC values of four xLa2O3−(100−x)(26Li2O−74SiO2) glass system, with x = 0, 0.9, 2.6 and 4.3 mol% was estimated by WinXCOM software and the results were approved by MCNPX code. The insertion of La2O3is related to increase both MAC and Zeffvalues. La4 glass sample with the highest concentration of La2O3possess superior photon attenuation effectiveness among the rest of glasses. Therefore, the Zeff results revealed that to increase the photon attenuation ability of the silicate glasses, high Z-elements La in a appropriate amount should be inserted. Moreover, this conclusion is supported with results of HVL, TVL and MFP. Therewithal, the estimated results may help in fabri-cating novel glass systems doped by La2O3which can forestall the po-tential radiation harm to the environment. According to the results, Li2O, SiO2and La2O3samples for photon, neutron, proton and alpha protection has proven to be a perfectly strong candidate. MSP calcu-lations are quite important in radioisotope production and integral yield calculations.
Declaration of Competing Interest
None
Acknowledgement
None.
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