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The effect of doping Cu 2 O on elastic and structural properties of thermoluminescent glass 90RWG – 10Na 2 O – xCu 2 O

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The purpose of this work was to study the elastic and structural properties of recycle window glass thermoluminescent dosimeter using ultrasonic technique and FTIR spectroscopy. The thermoluminescent glass system 90RWG – 10Na 2 O – xCu 2 O (where x =
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    Siam Physics Congress 2015 20-22 May 2015    xxx The effect of doping Cu 2 O on elastic and structural properties of thermoluminescent glass 90RWG  –   10Na 2 O  –   xCu 2 O Y. Jaichueai, C. Bootjomchai 1 , J. Laopaiboon 1  and R. Laopaiboon 1*   1 Department of Physics, Faculty of Science, Ubon Ratchatani University, 34190 Thailand *  Corresponding author. E-mail: Raewatl@yahoo.com Abstract   The purpose of this work was to study the elastic and structural properties of recycle window glass thermoluminescent dosimeter using ultrasonic technique and FTIR spectroscopy. The thermoluminescent glass system 90RWG  –   10Na 2 O  –   xCu 2 O (where x = 0.001, 0.01, 0.1 and 1.0 mol %) were prepared using the melt quenching technique, 1250°C for 5 hr melting and 500°C for 2 hr annealing. Densities of glass sample with varying the Cu 2 O dopant were measured. The longitudinal and shear velocities were measured by using pulse echo technique at 4 MHz frequency at room temperature. Densities and the ultrasonic velocities data of thermoluminescent glass were used for calculated the elastic properties such as longitudinal modulus, shear modulus, bulk modulus, Young’s modulus and Poisson's ratio. FTIR spectroscopy was measured in wave number range 400 - 4000 cm − 1  to study structure of the glass samples. The result shows that the longitudinal and shear velocities of thermoluminescent glass increase with the increasing of Cu 2 O. The density is correlated with Cu 2 O insignificant concentration. The change in elastic properties calculation of the thermoluminescent glass depends on the concentration of Cu 2 O and can be confirmed by using FTIR spectroscopy results.  Keywords :  Recycle window glasses, Thermoluminescent glass, Ultrasonic technique, FTIR spectroscopy Introduction Many types of thermoluminescence materials used as detectors such as medicine, industry, environmental and etc. the most common types of thermoluminescence dosimetry materials (TLD) are calcium fluoride (CaF), lithium fluoride (LiF) and aluminum oxide (Al 2 O 3 ) for radiation dosimetry. Moreover, lithium fluoride are widely used for medical science due to its effective atomic number of 8.2 ( Human tissue ~ 7.42 )  [1-2]   in the market under trade names like TLD-100 (LiF:Mg,Ti) and high sensitivity for TLD-100H (LiF:Mg,Cu,P). However, many types of materials are interesting such as glass and etc. Glass is interesting material for TL material   such as easy handling, corrosion resistance to chemicals, rigidity and transparency [3]. The structural properties are important to thermoluminescence material and related to thermoluminescence properties. Especially, Soda-lime glass consist 60-70% of silica (SiO 2 ), 12-15 % of soda (Na 2 O) and 5-12 % lime (CaO) lead to lower melting point and higher coefficient of expansion. If added transition metal oxides in glass system such as TiO 2  , ZnO 2  , MnO 2  , NiO, Cu 2 O, V 2 O 5  and etc lead to the change of structural properties, physical properties such as melting point of glass, optical properties, density, thermal expansion and chemical properties [4-7].   In addition, the effect of doped with transition metal oxides in glass system are affect to thermoluminescence properties   due to defect structure of glass and maybe effect to the solidity of glass structure. Also, Soda-lime glasses have been used radiation dosimeter [8-9]. In this work, elastic properties of recycle window glasses doped with Cu 2 O will be discussed. The elastic moduli can be calculated by longitudinal and shear velocities such as Longitudinal modulus, shear modulus, Poisson's ratio, Bulk modulus and Young’s modulus . Network bonds will be examined by FTIR spectroscopy. Experimental and theoretical techniques Sample preparation Glass samples were prepared in the 90RWG  –   10Na 2 O  –   xCu 2 O system, where RWG = Recycle window glass and x = 0.001, 0.01, 0.1 and 1.0 mol % . The chemical composition analyses of the recycled window glass were carried out by using the WDXRF technique as show in Table 1.  The glasses were prepared using the melt quenching technique. The homogeneous mixtures were placed in alumina    Siam Physics Congress 2015 20-22 May 2015    xxx crucible and melted in an electric furnace until homogeneity of the glass melt was ensured. The homogenized molten glass was cast into stainless steel mould and annealed for 2 h. Density and molar volume measurements The densities of the glass samples were determined  by Archimedes’ principle, using n -hexane as an immersion liquid and applying the relationship [10]. =    W  W  − W    (1) where    is density of n-hexane (0.661 g/cm 3 ),    and    are the sample weights in air and in n-hexane, respectively. The molar volume (   ) of the glass was calculated using the relation   =   (2) where   is the density of the glass and   is the molecular weight of the glass [11]. Ultrasonic measurement and elastic moduli The glass samples were cut and polished using different grade of silicon carbide. The thickness measurement was carried out by a micrometer. The ultrasonic wave was generated from a ceramic transducer with a resonant frequency at 4 MHz and acting as a transmitter-receiver at the same time. Ultrasonic flaw detector, SONATEST Sitescan 230. Elastic moduli were calculated using the following standard relations [11]. Longitudinal modulus:  =    (3) Shear modulus: =    (4) Bulk modulus: =    (5) Young’s modulus: =  (6) Poisson’s ratio : = −−  (7) Micro-hardness: = −6+  (8) Infrared absorption measurements The glass samples were measured at room temperature in the wavelength range 400  –  2000 cm -1  by a Fourier Transform infrared spectrometer. The powdered glass samples were mixed with KBr in the ratio 1:100 glass powder : KBr. Table.1.  Quantitative analysis of chemical composition of RWG by using WDXRF technique.   Chemical composition Concentration ( % ) Na 2 O 15.1700 MgO 3.4080 SiO 2  73.3900 Al 2 O 3  0.5866 CaO 7.3390 Fe 2 O 3  0.0635 TiO 2  0.0263 K 2 O 0.0238 Results and Discussion Density and Molar volume The glass composition, density and molar volume are given in Table 1.  The density increase from 2.55 to 2.6 g . cm -3  when the content of doping Cu 2 O increases as shown in Figure 1 . Because the doping of Cu 2 O into the glass which molecular weights of Cu 2 O have more than silica (SiO 2 ). Molecular weights have 143.08 g.mol -1  of Cu 2 O   and 60.09 g.mol -1  of silica. The results of molar volume as shown in Figure 1 . The molar volume of glass samples increase with the increase of content of Cu 2 O. The molar volume increase depends on the ionic radius of the modifier. The ionic radius of the Cu 2+  (0.73   Å ) is larger than the ionic radius of Si 4+  (0.40   Å ) and Na +  (1.02 Å ) which lead to an increase in the size of the interstices and increase in the molar volume [12]. Figure 1. Variation of density and molar volume as a function of mol %  of Cu 2 O   in the glass system. Ultrasonic velocity and elastic moduli The longitudinal and shear ultrasonic velocity in the glass sample with the mol % of the dope are shown in Figure 2.  The velocities (V l  and V s ) show increase with the increase of Cu 2 O mol %. The increase of ultrasonic velocities is related to the decrease in the number of non-bridging oxygen and consequently the increase in connectivity of the glass network [13]. Therefore, Ultrasonic velocity is a tool in revealing the 23.223.223.323.323.423.423.523.523.623.62.502.522.542.562.582.602.622.64 0 0.001 0.01 0.1 1    M  o   l  a  r  v  o   l  u  m  e   (  c  m    3  .  m  o   l   -   1    )   D  e  n  s   i   t  y   (  g .  c  m   -   3    ) Cu 2 O (mol % ) DensityMolar volume    Siam Physics Congress 2015 20-22 May 2015    xxx degree of change in structure with composition of glasses. The Young’s modulus(E) and B ulk modulus(K) as shown in Figure 3 . The moduli increase with the concentration of Cu 2 O modifier such as longitudinal modulus, shear modulus, young’s modulus and bulk modulus shown of change in the number of non-bridging oxygen (NBO) in the glass network [14]. Figure 2. Variation of longitudinal and shear velocity as a function of mol %  of Cu 2 O   in the glass system. Figure 3. Variation of Young’s modulus and B ulk modulus as a function of mol %  of Cu 2 O   in the glass system. In general, the increase of ultrasonic velocity is related to the decrease in the number of non-bridging oxygen (NBO) and consequently the increase in connectivity of the glass network with the concentration of Cu 2 O modifier [15]. The Young’s modulus increase from 73.5 to 80.55 GPa are effect to glass structure with concentration of Cu 2 O in glass system. The Y oung’s modulus increase leads to the rigidity of glass network structure with the increase concentration of Cu 2 O in glass system. The decrease in bulk modulus are effect to the resistance to the force in every direction the decrease at concentration of Cu 2 O 0.001 mol% and increase at 0.01 to 1.0 mol% of Cu 2 O in glass system. The value of Poisson’s  ratio show in Figure 4.   Poisson’s ratio is the measure of the cross -link density of the structure.   Poisson’s ratio reveals a cross -link density in glass structure. The range of Poisson’s ratio 0.1 to 0.2 is shown a high cross-link density while 0.3 to 0.5 is a low cross-link density.   The decreases of Poisson’s  ratio indicate increase the crosslink density in the glass network. Therefore, decreases of Poisson’s ratio shows that the increasing of cross-link density due to decrease of number of non-bridging oxygen [16]. The value of micro-hardness show in Figure 5.  The micro-hardness indicates the rigidity of glass network structure and micro-hardness relate to Poisson’s  ratio and young’s modulus.  The increase in micro-hardness from 5.27 to 6.39 GPa are lead to the increase of resistance to downforce. Figure. 4. Variation of Poisson’s  ratio as a function of mol %  of Cu 2 O   in the glass system. Figure 5. Variation of micro-hardness as a function of mol %  of Cu 2 O   in the glass system. Fourier transform infrared absorption (FTIR) The FTIR spectra for the glass with Cu 2 O doped at the concentrations 0.001, 0.01, 0.1 and 1.0 mol% are shown in Figure 6.  The glass samples were measured at room temperature in the wavelength range 400  –  2000 cm -1 . The frequency bands from the glasses network vibrations appear in the range 400  –  1500 cm -1 . The first vibration signals at around 470 cm -1  are assigned to the Si  –  O  –  Si bending modes of bridging oxygen. The peaks near 775-800 cm -1  are assigned to the vibrations of O-Si-O bonds. The peaks at 960 cm -1  is assigned vibrations of non-bridging oxygen (NBOs). The peak in the region range of 1050-1120 cm -1  is assigned to Si  –  O  –  Si anti symmetric stretching of Si-O-Si. The signal at approximately 1600 cm -1  is assigned molecular water [17]. The networks structure of soda 325033003350340034503500355036003650576057805800582058405860588059005920 0 0.001 0.01 0.1 1    S   h  e  a  r  v  e   l  o  c   i   t  y   (  m .  s   -   1    )    L  o  n  g   i   t  u   d   i  n  a   l  v  e   l  o  c   i   t  y   (  m .  s   -   1    ) Cu 2 O (mol % ) LongitudinalShear 44.5045.0045.5046.0046.5047.0068.0070.0072.0074.0076.0078.0080.0082.0084.00 0 0.001 0.01 0.1 1    B  u   l   k  m  o   d  u   l  u  s   (   G   P  a   )   Y  o  u  n  g   '  s  m  o   d  u   l  u  s   (   G   P  a   ) Cu 2 O (mol % ) E K 0.1900.2000.2100.2200.2300.2400.250 0 0.001 0.01 0.1 1    P  o   i  s  s  o  n   '  s  r  a   t   i  o Cu 2 O (mol % ) 4.004.505.005.506.006.507.00 0 0.001 0.01 0.1 1    M   i  c  r  o  -   h  a  r   d  n  e  s  s   (   G   P  a   ) Cu 2 O (mol % )    Siam Physics Congress 2015 20-22 May 2015    xxx lime glass doped with Cu 2 O are related to network bonds in glass structure. Increasing concentration of Cu 2 O reveal slight the increase of the absorption bands in FTIR spectra. Figure 6.  The IR spectra of the glass samples with vary concentration of Cu 2 O   in the glass system. Table 2. Depicts the detailed assignments of IR bands in sodium silicate glasses [17] . Peak position (cm -1 ) Assignment 460-480 Bending vibration of Si-O-Si linkages 640-680 Si-O-Si and O-Si-O bending 775-800 Symmetric stretching vibrations of O-Si-O bonds 960 Vibrations of non-bridging oxygen(NBO) 1050  –  1120 Anti symmetric stretching of Si-O-Si linkages 1400  –  1460 Carbonate group 1630  –  1645 Molecular water Conclusions Results of ultrasonic velocity in glass system indicate the formation of bridging oxygens with the increase of Cu 2 O concentration in glass system. The elastic moduli are related to change in the structure of the glass. The glass structures are rigid at the higher values of Cu 2 O concentration in glass system. The FTIR spectra also support the structural changes of glass system. References 1. A.Ab Rasid, H.Wagiran, Dosimetric properties of dysprosium doped lithium borate glass irradiated by 6 MV photons, Radiation Physics and Chemistry,112(2015)29  –  33 2. Schulman, J.H.,Kirk,R.D.,West,E.J.,1965.Use of lithium borate for thermoluminescence dosimetry.In:Proceedingsof the International ConferenceonLuminescenceDosimetry.CONF650637.Stanford,CA,USA,p.113. 3. C. Bootjomchai, R. Laopaiboon, Thermoluminescence dosimetric properties and effective atomic numbers of window glass, Nuclear Instruments and Methods in Physics Research B 323 (2014) 42  –  48 4. N. Srisittipokakuna, K. Kirdsiri, Absorption and Coloration of MnO2 Doped in Soda-lime-silicate and Soda-lime-borate Glasses, Procedia Engineering, 8(2011) 261  –  265. 5. M.M.Khalil, Appl.Phys. A86(2007)505. 6. A.B.Jadlika, A.G.Clare, J.Non-Cryst.Solids, Chemical durability of commercial silicate glasses. I. 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Laopaiboon, C. Bootjomchai, Glass structure responses to gamma irradiation using infrared absorption spectroscopy and ultrasonic techniques: A comparative study between Co 2 O 3  and Fe 2 O 3 , Applied Radiation and Isotopes 89 (2014) 42  –  46. 15. Prado, M.O., Messi, N.B., Plivelic, T.S., Torriani, I.L., Bevilacqua, A.M., Arribére, M.A., The effects of radiation on the density of an aluminoborosilicate glass. J. Non-Cryst. Solids, 289(2001)175  –  184. 400 900 1400 1900 % TWavenumber (cm -1 ) 0 0.001 0.010.1 1    Siam Physics Congress 2015 20-22 May 2015    xxx 16. K.J. Singh, SandeepKaur, R.S.Kaundal, Comparative study of gamma ray shielding and some properties of PbO  –  SiO 2  –  Al 2 O 3  and Bi 2 O 3  –  SiO 2  –  Al 2 O 3  glass systems, Radiation Physics and Chemistry, 96(2014)153  –  157. 17. R. Laopaiboon, C. Bootjomchai,M. Chanphet, J. 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