Results in Physics 9 (2018) 1371–1376

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Results in Physics
journal homepage: www.elsevier.com/locate/rinp

Optical properties of zinc lead tellurite glasses T

a,e,⁎ a,b,⁎ c d
Salah Hassan Alazoumi , Sidek Abdul Aziz , R. El-Mallawany , Umar Sa'ad Aliyu ,
Halimah Mohamed Kamaria,b, Mohd Hafiz Mohd Mohd Zaida,b, Khamirul Amin Matoria,b,
Abdulbaset Ushaha
a
Department of Physics, Faculty of Science, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor, Malaysia
b
Materials Synthesis and Characterization Laboratory, Institute of Advanced Technology, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor, Malaysia
c
Physics Department, Faculty of Science, Menoufia University, Egypt
d
Department of Physics, Faculty of Science, Federal University Lafia, Nigeria
e
Physics Department, Faculty of Science, Gharyan University, Libya

A R T I C LE I N FO A B S T R A C T

Keywords: Tellurite glass systems in the form of [ZnO]x [(TeO2)0.7-(PbO)0.3]1-x with x = 0.15, 0.17, 0.20, 0.22 and 0.25 mol
Tellurite % were prepared using the melt quenching technique. XRD of the prepared samples have been measured for all
Glass samples. Both FTIR (280–4000 cm−1) and UV-Vis (200–800 nm) spectra have been measured. Optical band gap
Optical band gap and refractive index were calculated for every glass sample. Density of glass, molar volume and oxygen packing
Refractive index
density (OPD) were obtained. Values of the direct, indirect band gap ranged were found in the range
3.41–3.94 eV and 2.40–2.63 eV with increasing of ZnO concentration. Refractive index 2.58 and dielectric
constant 6.66 were heigh at 17 ZnO mol% concentration. Molar polarizability, metallization criterion, polaron
radius have been calculated for every glass composition.

Introduction Experimental work

Glasses based on tellurium dioxide and modified by heavy metal [ZnO]x [(TeO2)0.7-(PbO)0.3]1-x glass system was prepared by mixing
oxides have properties promising for various optical applications. Many specific weights of high purity oxides, tellurium oxide, TeO2 (Alfa
different works have been carried out in the study of the physical Aesar, 99.99%), lead oxide, PbO (Alfa Aesar, 99.99%) and zinc oxide,
properties of different composition of tellurite glasses [1–5]. Due to ZnO (Alfa Aesar, 99.99%). The homogenization of the 15 g of chemicals
their versatility in terms applications, tellurite glasses have received mixtures was effected by repeated grinding using a mortar for 30 min.
some scientific and technological attentions in the recent years [6,7,8]. The mixtures were preheated in a crucible (alumina) at 280 °C for one
The glasses have shown great promise in optical fiber technology, la- hour in the electric furnace; the crucible was then transferred to the
sers, sensors, optical fibers, solar cells [9], memory switching devices, another electrical furnace for one hour at a temperature 850–900 °C.
optoelectronic, gas sensors, and optical waveguides applications The mixture melt then turned into a stainless steel cylindrical shaped
[10,11]. The glasses have been so important in the photonic technology split stainless steel mould that has been preheated. After the process of
and other applications because of their excellence in terms of high quenching, the solid sample of glass was annealed at 280 °C for an hour
index of refraction, dielectric constant, wide spectral region transpar- to avoid the mechanical strain developed during the process of
ency, resistance to corrosion, chemical and thermal stability and low quenching and then left to cool down to ambient temperature. The glass
melting point [8,9]. samples were cut into about 2 mm thickness using the low-speed dia-
The present work presents a study on the effect of ZnO on density, mond blade to make great parallel surfaces for UV-Vis charaterization.
the oxygen parking density (O.P.D), FTIR spectra, optical band gap, Both surfaces of the samples were polished using a polishing machine
Urbach energy, reflection loss, molar refractive index, optical trans- with sandpaper to achieve a plane parallelism, and a part of the sample
mission coefficient, molar polarizability and dielectric constant for cut was grinded into a powdered from for XRD and FTIR character-
tellurite glass systems in the form of [ZnO]x [(TeO2)0.7-(PbO)0.3]1-x with izations.
x = 0.15, 0.17, 0.20, 0.22 and 0.25 mol%. Density measurement of the glass samples was carried out at room
temperature using a densitometer model (MD-300SDensimeter)

⁎
Corresponding authors at: Department of Physics, Faculty of Science, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor, Malaysia.
E-mail addresses: selazomi@gmail.com (S.H. Alazoumi), sidek@upm.edu.my (S.A. Aziz).

https://doi.org/10.1016/j.rinp.2018.04.041
Received 10 March 2018; Received in revised form 12 April 2018; Accepted 13 April 2018
Available online 27 April 2018
2211-3797/ © 2018 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/).
S.H. Alazoumi et al. Results in Physics 9 (2018) 1371–1376

employing the principle of Archimedes with distilled water used as the Table 1
fluid of immersion. The density resolution was estimated around ± Experimental values of Density (ρ), Molar volume (Vm), Molar refractivity Rm,
0.001 g/cm3. The glass samples were weighed in air, (Wair), and water index and Oxygen packing density (O.P.C) of ternary [ZnO]x [(TeO2)0.7-
(Wwater), with (ρwater = 1 g/cm3). Density measurement of each glass (PbO)0.3]1-x glass system.
samples done using the following relationship: x (mol%) ρ ( ± 32 kg·m−3) Vm ( ± 0.15 cm3·mol−1) Rm (O.P.D)

Wair 15 6257 26.22 16.76881143 60.822

ρ=
(Wair −Wwater ) (1) 17 6230 26.03 17.00987893 60.748
20 6191 25.72 16.39175565 60.568
where (Wair) and (Wwater) each representing the weights of the glass 22 6144 25.60 16.54759886 60.395
sample in air and distilled water, respectively. Ideally, the glass molar 25 6078 25.40 16.22142697 60.050
volume is used in describing the network structure and the building
units arrangement since it directly deals with the oxygen network
6.4 30
spatial structure. Moreover, molar volume (Vm) is considered to be the

Molar Volume (cm3/mol)

better tool for studying the changes in glass structure since it eliminates Density
29
mass from the density and uses an equal number of particles for com- 6.3

Density (g/cm3)
Molar Volume
parison purposes. It is calculated from density using the equation,
28
(Vm = Mglass/ρglass), where (ρglass) is the density of the glass sample and
6.2
(Mglass) is the molecular weight of the glass. The calculation of molar
27
volume for each glass sample was done using the formula:
6.1
∑i x i Mi 26
Vm =
ρglass (2)
6 25
where (Mi) is the oxide component’s (i) molecular weight and (xi) is its 14 16 18 20 22 24 26
mole fraction. ZnO (mol %)
X-ray diffraction (XRD) system PANalytical (Philips) PW3050/60
Fig. 2. Density (ρ) and molar volume(Vm) of the [ZnO]x [(TeO2)0.7-(PbO)0.3]1-
was used in amorphous nature confirmation in the range of (2θ) value
xglasses.
from 4° to 90°. The FTIR spectra were obtained by using the FTIR
spectrometer (400–4000 cm−1 and resolution of 0.85 cm−1 by KBr
pellet technique). UV-Vis data was collected using UV-Visible spectro- ZnO molar composition is an indication of the preceding structural
meter (Shimadzu UV-3600-VIS-NIR spectrometer) in the wavelength changes via a modification or formation process in the network of the
200 nm–800 nm. glass [14]. Molar volume decreased for the glass system from 26.22 to
25.40 (cm3/mol) may be due to a bond length reduction or inter-atomic
Results and discussion spacing decrease between the constituting atoms in the glasses [15].
Thus, it can be noted that the variation of the densities and molar vo-
Fig. 1 is the glass system’s X-ray diffraction pattern. This pattern lume is due to the low change in concentration of ZnO.
revealed a broadly diffused scattering around 2θ = 20°–30°. This ex- The glasses’ FTIR spectra in the range 280–4000 cm−1are presented
hibits the amorphous glass nature and shows the absence of long-range in Fig. 3. The Fig. 3 shows absorption bands with highest intensities
atomic arrangements [12]. Density and calculated values of the molar around 419 cm−1, and between 596 and 612 cm−1. The vibrations
volume are presented in Table 1 and Fig. 2. Both values were observed around 419 cm−1 is ascribed the stretching vibrations Zn-O in ZnO4 or
to have decreased with increasing amount of ZnO in glass system. The of Te-O-Te vibrations or O-Te-O linkages. The absorptions with centers
density can be observed to decreased gradually with ZnO percentage. between 596 and 619 maybe attributed to the stretching vibrations of
The replacement of ZnO (with lower molecular weight 81.38 g/mol) at Te-O bonds in the TeO4 structural units [16]. The shift in the absorption
the expense of TeO2 and PbO (with higher molecular weights 159.598 center toward higher wave numbers with increase in the proportion of
and 223.1994 g/mol, respectively), led to the decrease in density from ZnO might be attributed to the conversion of TeO4 units to TeO3
6.257 to (6.078 g cm−3) with ZnO content increase from 15 to 25 mol% structural units. The TeO4 to TeO3 unit conversion indicates the for-
[13]. Molar volume decreased from 26.22 to 25.40 cm3/mol with the mation of non-bridging oxygens [17]. Between 664 and 677 cm−1, the
increasing of ZnO concentration. The glass structure is more explained IR absorption maybe either due to Te-O vibrations in TeO3 structural
using molar volume than density, as the former has to do with ions
spatial distribution in structure. The molar volume changes with the
Transmisstion (a.u)
Intensity (a.u)

x=25%
15% ZnO
x=22% 17% ZnO
20 % ZnO
x=20%
22% ZnO
x=17% 25% ZnO

x=15%
200 700 1200 1700
4 24 44 64 84 104 Wavenumber (cm-1)
2 Thetha (degree)
Fig. 3. FTIR spectra of [ZnO]x [(TeO2)0.7-(PbO)0.3]1-xglasses with x = 0.15,
Fig. 1. XRD patterns of [ZnO]x [(TeO2)0.7-(PbO)0.3]1-xglasses. 0.17, 0.20, 0.22, 0.25 mol%.

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S.H. Alazoumi et al. Results in Physics 9 (2018) 1371–1376

5
Direct band gap Indirect band gap
4.5

Optical band gap (ev)

4

3.5

2.5

1.5

1
12 14 16 18 20 22 24 26 28
ZnO (mol %)

Fig. 4. UV absorption spectra of [ZnO]x [(TeO2)0.7-(PbO)0.3]1-x glasses with Fig. 6. Energy gap values for [ZnO]x [(TeO2)0.7-(PbO)0.3]1-xglasses with
x = 0.15, 0.17, 0.20, 0.22, 0.25 mol%. x = 0.15, 0.17, 0.20, 0.22, 0.25 mol%.

units or the vibrations of Pb-O in PbO3 or PbO4 structural units [17]. as the photon energy (hυ) exponential function and B as a constant
The determination of both optical band gaps (Direct and Indirect) value [22];
was carried out using the expression of Davis and Mott [18] for the hυ
coefficient of absorption α (υ) as; α (υ) = B exp
ΔE (5)
(hυ−Eopt )n The values of the Urbach energy as observed in Table 2 varies with
α (υ) = B
hυ (3) the concentration of Zn2+ ions in the network from 0.15 to 0.17, 0.20,
0.22 and 0.25 mol%. The Urbach energy decrease shows an increase in
where Eopt representing the optical band gap, n is a number, with in-
the glass fragility due to increase in the TeO3 concentration that
direct and direct allowed transitions are denoting n = 2 and n = 1/2
changes the structural networking in the glass. This indicates defects
and B = constant. This absorption coefficient value α(υ) is the de-
formation and hence causes the band gap value increase, whereas the
termined by the expression, with A obtained from the UV-Vis spectra in
increase is an indication of defects deformation and results from an
Fig. 4;
increase in the BOs number.
A Figs. 7 and 8 present the index of refraction (n) and the oxygen
α (υ) = 2.303
t (4) packing density respectively. The refractive index (n) of the prepared
glass system was calculated values of the optical energy band gap (In-
where t = sample thickness, A = optical absorbance value. By drawing
direct, Eindir) using the equation in [22].
the Tauc’s plots between (αℏ ω)1/n and the photon energy (ℏ ω) and
extrapolating the linear part of the plots, optical band gap values where n2−1 Eopt
obtained at(αℏ ω)1/2 = 0 and (αℏ ω)2 = 0 respectively for the indirect = 1−
n2 + 2 20 (6)
and direct transitions [19,20]. The optical band gap values both direct
and indirect were presented in as shown in Figs. 5, 6 and Table 2. The The refractive index as presented in Fig. 7 varies with ZnO concentra-
direct and indirect varied between 3.41 and 3.89 eV and 2.40 and tion from 0.15 to 0.25 in the glass system. The increase may be asso-
2.63 eV due to the ZnO content is increased from 0.15 to 0.17, 0.20, ciated with the substitution of TeO4+ and Pb2+with Zn2+ ions with
0.22 and 0.25 mol% respectively. In both cases, the values increase with lower polarizability [23]. Whereas the decrease in the refractive index
the increasing concentration of Zn2+ ions may be to the bridging of the may be associated with the decrease in the NBOs concentration in the
free space in the glass. This results to an increase in the structural glass network [24]. The oxygen packing density in Fig. 8 and Table 1
compactness in the network of the glass [21]. The decrease in the values decreased with ZnO concentration increased. This showed a same re-
of both band gaps (indirect and direct) may be attributed to the electron lation with the molar volume as presented in Fig. 1 and Table 1. The
localization degree that is caused by the glass network’s structural decrease indicates a more spatial distribution of oxygen in the glass
changes. The coefficient of absorption, α (υ) of the glasses is expressed network. This can be associated with a Te4+ substitution and Pb2+ with
higher field intensity than Zn2+ hence, having a lower attraction to the
3500 oxygen atoms [25].
17% ZnO For any material, the metallization criterion gives information about
3000
the metallic or insulating nature of such material on its band gap energy
2500 basis and is expressed as a function of molar refraction (Rm) and molar
(ĮhȞ)2(cm-1ev)2

volume (Vm) as reported by [26] as;

2000
Rm
M = 1−
1500 Vm (7)

1000 The molar polarizability, transmission coefficient, reflection loss, di-

electric constant, optical dielectric constant and oxide ion polarizability
500
3.41 ev were calculated using Eqs. (8)–(13) respectively.
0 3
2 2.5 3 3.5 4 4.5 5 αm = ⎛ ⎞ Rm
⎝ 4πN ⎠ (8)
hȞ (ev)
Fig. 5. The optical band gap of [ZnO]x [(TeO2)0.7-(PbO)0.3]1-x glasses, n−1 ⎤2
RL = ⎡
x = 0.17 mol%. ⎣n + 1⎦ (9)

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S.H. Alazoumi et al. Results in Physics 9 (2018) 1371–1376

2.59
Reflection Loss, RL
2.58

2.57

Refractive Index (n)

2.56
0.185
0.194
0.184
0.190
0.185
2.55

2.54

2.53
Molar refraction, Rm ( ± 0.14) cm3)

2.52

2.51

2.5
14 16 18 20 22 24 26
ZnO (mol %)
Fig. 7. Refractive index of [ZnO]x [(TeO2)0.7-(PbO)0.3]1-xglasses with x = 0.15,
0.17, 0.20, 0.22, 0.25 mol%.
16.76
17.00
16.39
16.54
16.22

61

Oxygen Packing Density (g atm/l)

Refractive index, n ( ± 0.146)

60.5

60
2.51
2.58
2.50
2.54
2.51

59.5
Urbach energy ( ± 0.018 eV)

14 16 18 20 22 24 26
ZnO (mol %)
Fig. 8. Oxygen packing density of[ZnO]x [(TeO2)0.7-(PbO)0.3]1-x, x = 0.15,
0.17, 0.20, 0.22,0.25 mol%.
Direct and Indirect band gap, Urbach energy, Refractive index, Molar refraction and Reflection loss.

2n
0.2764
0.3323
0.2624
0.2724

T=
0.354

n2 + 1 (10)
The dielectric constant is inversely proportional to the square of the
speed of light in the material [27],
Indirect band gap ( ± 0.043 eV)

ε = n2 (11)

dt
ε opt = p = ε−1 = n2−1
dp (12)
The oxide ion polarizability based on refractive index was calculated as
reported by Meena and Bhatia [9].
R
α O(n2)− = ⎡ m − ∑ αi⎤ NO2 − ( )−1
2.40
2.63
2.50
2.61
2.6

⎣ 2.52 ⎦ (13)
where Σαi = molar cation polarizability and NO2 − is the oxide ions
number in the chemical formula. The values of the molar cation po-
Direct band gap ( ± 0.092 eV)

larizability (α) was obtained as reported in [28]. In Table 3, the me-

tallization criterion, molar polarizability, transmission coefficient, di-
electric constant and oxide ion polarizability were presented. Decrease

Table 3
Metallization Criterion, Molar Polarizability, Optical Transmission Coefficient,
Dielectric Constant and Oxide Ion Polarizability.
3.72
3.41
3.94
3.77
3.89

x (mol%) M αm αe T ε εopt −
αO2 (n)

15 0.360 6.65 0.2535 0.686 6.32 5.3205 1.579

17 0.346 6.74 0.2591 0.673 6.66 5.6602 1.624
x (mol%)

20 0.362 6.50 0.2526 0.688 6.27 5.2729 1.561

Table 2

22 0.353 6.56 0.2562 0.680 6.48 5.4853 1.595

15
17
20
22
25

25 0.361 6.43 0.2532 0.687 6.30 5.3045 1.571

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S.H. Alazoumi et al. Results in Physics 9 (2018) 1371–1376

0.692 Table 4
Transmission Coefficient (T)

Number of bond per unit volume (nb), polaron radius (Rp), Inter-nuclear dis-
0.688 tance of Zn2+ (Ri), Field Strength of Zn2+ yield, molar volume of tellurium
atoms (VTe) and average Te to Te separation (〈dTe-Te〉).

0.684 x (mol%) nb Rp (Å) Ri (Å) F (cm−2) VTe 〈dTe-Te〉

15 9.185E+22 2.6689 6.6222 11.512 32.375 3.775E−08

0.68 17 9.255E+22 2.5533 6.3355 12.578 31.056 3.723E−08
20 9.366E+22 2.4091 5.9777 14.129 29.225 3.648E−08
22 9.410E+22 2.3302 5.7818 15.102 28.191 3.605E−08
0.676 25 9.485E+22 2.2270 5.5260 16.533 26.732 3.541E−08

0.672
0.14 0.16 0.18 0.2 0.22 0.24 0.26
in the molar volume increased in the glass network. Whereas the de-
crease in the values may be connected to the substitution of higher
ZnO molar fraction
polarizability Te4+ and Pb2+ ions with lower polarizability Zn2+ ions
Fig. 9. Optical Transmission Coefficient of [ZnO]x [(TeO2)0.7-(PbO)0.3]1-x, in the glass network and also decrease in the inter-ionic distances
x = 0.15, 0.17, 0.20, 0.22,0.25 mol%. [30–32].
The parameters presented in Table 4 were obtained as reported by
0.196 [33] as follows; Average Tellurium-Tellurium separation, 〈dTe-Te〉;
Te 1/3
V
〈dTe − Te 〉 = ⎡ m ⎤
Reflection Loss (RL)

0.192 ⎢ NA ⎥ (14)
⎣ ⎦
Vm
Where VmTe =
0.188 2(1−XTe ) (15)
2+
Zn ion concentration, N is expressed as;

0.184 XZnxρ xNA

N (Zn2) =
mw (16)
where NA, VmTe ,
XTe and XZn are the Avogadro’s number, molar volume of
0.18
0.14 0.16 0.18 0.2 0.22 0.24 0.26
tellurium atoms, molar fraction of tellurium and molar fraction of zinc
respectively. The average Te-Te separation helps in explaining the
ZnO molar fraction
changes in glass material compactness and rigidity and thus, can be
Fig. 10. Reflection Loss of [ZnO]x [(TeO2)0.7-(PbO)0.3]1-x, x = 0.15, 0.17, 0.20, used to explain the changes in optical band gap [34].
0.22,0.25 mol%. Polaron radius (Rp), inter-ionic distance of Zn2+ ions (Ri) and field
strength of Zn2+ yield (F) for the glasses was obtained using the
7 equation as reported [33,35] as;
1 π 1/3
6.5 Rp = ⎛ ⎞
2 ⎝ 6N ⎠ (17)
6 1 1/3
Ri = ⎛ ⎞
(18)
‫ܭܭ‬opt

⎝N ⎠
5.5
Z
F=
5 rp2 (19)
Dielectric Optical dielectric
In Fig. 12 and Table 4 below, the polaron radius value of the ZnO-
4.5
PbO-TeO2 glass system studied decreased from 2.6689 to 2.2270 Å
when the concentration of Zn2+ was increased from 15% to 25%. This
4
0.14 0.16 0.18 0.2 0.22 0.24 0.26
2.8
ZnO molar fraction
Polaron Radius, RP (A°)

Fig. 11. Dielectric and Optical Dielectric Constants of [ZnO]x [(TeO2)0.7-

(PbO)0.3]1-x, x = 0.15, 0.17, 0.20, 0.22,0.25 mol%. 2.6

in the value of metallization criterion is an indication that the width of 2.4

both the conduction and valence band has increased with the addition
of more ZnO in the network [7]. The dielectric constant values in any
glass system depend on their ionic polarizability, electronic polariz- 2.2
ability, and the contribution of dipole orientation to the polarizability.
The observed behavior of the dielectric constant as shown in Fig. 11 in
the studied glasses may be associated to low frequency in the polar- 2
ization caused by multi-component contributions in the system of the 0.13 0.15 0.17 0.19 0.21 0.23 0.25 0.27
studied glasses [29]. Because of its dependence on the molar volume ZnO molar fraction
and refractive index, the polarizability value increased in the glasses
Fig. 12. Polaron Radius of [ZnO]x [(TeO2)0.7-(PbO)0.3]1-x, x = 0.15, 0.17, 0.20,
with an increase in the ZnO content may be associated with the increase 0.22, 0.25 mol%.

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S.H. Alazoumi et al. Results in Physics 9 (2018) 1371–1376

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