Materials and Design 101 (2016) 277–284

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Materials and Design

journal homepage: www.elsevier.com/locate/matdes

Computational intelligence method of determining the energy band gap

of doped ZnO semiconductor
Taoreed.O. Owolabi a,b,⁎, Mohamed Faiz a, Sunday O. Olatunji c, Idris.K.Popoola a,d
a
Physics Department, King Fahd University of Petroleum and Minerals, Dhahran, Saudi Arabia
b
Physics and Electronics Department, Adekunle Ajasin University, Akungba Akoko. Ondo State, Nigeria
c
Computer Science Department, University of Dammam, Dammam, Saudi Arabia
d
Department of Physics, Geology and Geophysics, Federal University Ndufu-Alike Ikwo, Ebonyi State, Nigeria.

a r t i c l e i n f o a b s t r a c t

Article history: Presence of a direct wide band gap and large exciton binding energy in ZnO contributes enormously to its diverse
Received 6 February 2016 practical applications such as transparent electrodes in solar cells and guide electron devices to mention a few.
Received in revised form 21 March 2016 Doping has been recognized as an effective way of improving the intrinsic defects associated with pure ZnO
Accepted 22 March 2016
and further serves as a way of controlling the band gap of ZnO for specific application of interest. Since the direct
Available online 7 April 2016
signature of doping in a crystal structure is the distortion of lattice constants, this present work develops a sup-
Keywords:
port vector regression computational intelligence (SVRCI)-based model for estimating the energy band gap of
Doped ZnO semiconductor doped ZnO using lattice parameters as the inputs to the model. The proposed model further investigates the ef-
computational intelligence technique fect of annealing and sample preparation conditions on the band gap of doped ZnO. The proposed model is char-
support vector regression acterized with mean absolute percentage error of 1%. The band gaps estimated by the developed model agree
lattice parameters and energy band gap well with the experimental values. The precision exhibited by the developed model paves way for its application
for quick estimation of energy band gap of doped ZnO and consequently relieves the experimental stress involved
in band gap measurements.
© 2016 Elsevier Ltd. All rights reserved.

1. Introduction
ZnO is a II-VI semiconductor that is characterized with a direct as
well as wide band gap(difference in energy between the top of the va-
lance band and the bottom of conduction band). Its unique properties
include excellent thermal and chemical stability and large exciton bind-
ing energy which promotes its optoelectronic property. These unique
properties exihibited by ZnO have rendered it indispensable in wide
range of applications such as solar cell, thin film transistors,laser diodes
piezoelectric and optoelectronic application to surface acoustic wave
devices, transparent conductive contacts and ultraviolet lasers among
others [1] [2,3]. Presence of various intrinsic defects such as zinc and
oxygen vacancies (missing atoms at regular lattice positions) as well
as interstitial zinc (extra atoms occupying intestices in the lattice), in-
terstitial oxygen, antisite oxygen and zinc (oxygen atom occupying
zinc lattice site and zinc atom occupying oxygen lattice site) in undoped
ZnO have been reported in literature [1,4]. The optical properties of
undoped ZnO is thereby affected by the presence of these intrinsic de-
fects which form either acceptor or donor level in the band gap [4]. In
an effort to reduce these intrinsic defects, a lot of work has been done
⁎ Corresponding author at: Physics Department, King Fahd University of Petroleum and
Minerals, Dhahran, Kingdom of Saudi Arabia.
E-mail address: owolabitaoreedolakunle@gmail.com (T.O. Owolabi).
by doping ZnO with several compounds and metallic elements [1]. Dop-
ing introduces distortion in crystal structure of ZnO and thereby alters
its energy band gap. This work develops SVRCI-based model that esti-
mates the energy band gap of doped ZnO semiconductor with high de-
gree of precision using the distorted lattice parameters. The developed
model also shows high degree of precision in Sn-doped ZnO semicon-
ductor that suffers little or no lattice distortion upon doping [5]. The
novelties of the proposed model include (i) quick and accurate estima-
tion of the effect of dopants on the band gap of ZnO (ii) estimation of the
effect of annealing on the band gap of ZnO (iii) estimation of the effect of
preparation conditions on the band gap of ZnO and (iv) reduction of the
experimental stress involved in band gap measurements.
Three crystal structures are often associated with ZnO and the
thermodynamically stable phase under ambient condition is wurtzite
structure, although other phases like zinc blende can be stabilized by
growing on cubic substrates. The stable wurtzite structure has two lat-
tice parameters which characterize its hexagonal unit cell. The crystal
structure is described by two interpenetrating hexagonal closed packed
sublattices in which one type of atom is displaced with respect to the
other type along the c-axis. The basal plane lattice constant which rep-
resents the edge length of the basal plane hexagon is represented by a
while the unit cell height that is perpendicular to the basal plane is de-
scribed by c. Each of the two sub-lattices has four atoms per unit cell and
each atom of one type is surrounded by four atoms of other kind.

http://dx.doi.org/10.1016/j.matdes.2016.03.116
0264-1275/© 2016 Elsevier Ltd. All rights reserved.
278 T.O. Owolabi et al. / Materials and Design 101 (2016) 277–284

Presence of zinc interstitial, oxygen vacancy and zinc on oxygen antisite The empirical risk Remp then becomes
makes pure ZnO naturally becomes n-type semiconductor [4]. During
doping, the band gap energy which represents the energy difference be- 1X k

Remp ðωÞ ¼ L Egi ; f ðxi ; ωÞ ð3Þ
tween the top level of the valence band and the lowest level of conduc- k i¼1
tion band is altered. Among the factors that influence the lattice
parameters of ZnO include the concentration of defects and foreign SVR reduces the complexity of the model through minimization of
atoms, difference in ionic radii of the foreign atoms with respect to the Euclidian norm ‖ω‖2 and measures the deviation of training data
matrix ion, external strains and annealing temperature. With the use outside the loss function zone by introducing non-negative variables
of the developed SVRCI-based model, the effect of doping concentration, (ξi and ξ⁎i i = 1, ... , k) called slack variables. The optimization problem
temperature and preparation condition on the energy band gap of is presented in equation (4) and (5) with regularization or penalty fac-
doped ZnO can be accurately estimated. tor C.
Computational intelligence techniques are computationally inspired Minimize
methodologies of solving mathematical and physical problems which
are hardly described by linear models. It accurately estimates the de- Xk

1 
sired target by aqcuiring a relation or parttern between the target and kωk2 þ C ξi þ ξi ð4Þ
2 i¼1
the descriptors (input to the model) [6]. Computational intelligence
tools include support vector machines, fuzzy logic and evolutionary
computation among others [7,8,9]. Among these tools, support vector Subject to
regression (SVR) has enjoyed a wide range of applications due to its 8
 
< E
gi − f Eg ; ω ≤ε þ ξi
ability to model real life problems with high degree of stability and esti- 
f Eg ; ω −Egi ≤ε þ ξi ð5Þ
mation generalization ability, even when developed using few data- : 
ξi ; ξi ≥0; i ¼ 1; ::::; k
points [10]. These characteristics make SVR a choice of computational
tool in this research work.
The essence of the penalty factor as indicated in equation (5) is to
The results of our modeling and simulation indicate that the de-
control the trade-off between the complexity of the model and the de-
veloped SVRCI-based model is capable of estimating the energy
gree to which the deviation larger than ε is allowed. Transformation of
band gap (Eg) of doped ZnO with high degree of accuracy. Evaluation
the optimization problem into dual problem gives solution described
of estimation power of the developed model shows average absolute
by equation (6) with inclusion of kernel function K(x, xi) expressed in
percentage error of 1%, correlation coefficient of 94.3% between the
equation (7).
estimated and experimental energy band gap and low root mean
square error. Xvectors
Nsupport


f ðxi Þ ¼ α i −α i K ðx; xi Þ; 0≤α i bC; 0≤α i ≤C ð6Þ
2. Description of the proposed computational intelligence tool i¼1

Support vector regression computational intelligence technique X

k
K ðx; xi Þ ¼ g i ðxÞg i ðxi Þ ð7Þ
is a special class of algorithm first introduced by Vladimir and uses
i
structural risk minimization inductive principles to attain its excel-
lent generalization on limited number of learning patterns [11]. It Where α i and α⁎i are the Lagrangian multiplier employed in solving
is characterized with absence of local minima and utilization of ker- the optimization problem.
nels. In its motivation to optimize and seek the generalization The estimation accuracy of SVR depends significantly on the optimal
bounds, it defines the loss function ε called intensive loss function selection of penalty factor C, loss function ε, hyper-parameter lambda
which ignores possible errors located within certain distance of the (λ) and kernel option of the chosen kernel function [12]. Epsilon (ε)
true value. The ε intensive loss function ensures the existence of influences the number of support vectors utilized in constructing the
global minimum in addition to its optimization of generalization regression function and controls the width of ε - intensive zone used in
bound. Among the most important characteristic features of SVR is fitting the training dataset. The hyper-parameter λ controls the hyper-
its ability to maintain excellent generalization performance in the plane where minimum error is ensured.
presence of small subset of training points which gives significant
computational advantages [12]. In developing and implementing 2.1. Evaluation of the estimation accuracy of the proposed SVRCI-based
SVR algorithm, the input lattice constants a and c of doped ZnO semi- model
conductor are mapped with the aid of nonlinear mapping function
(Gaussian kernel function) onto k-dimensional feature space where The estimation accuracy of the proposed SVRCI-based model was
linear model F(Eg, ω) presented in Eq. (1) is constructed. evaluated using root mean square error (RMSE), mean absolute
percentage difference (MAPD), coefficient of correlation (CC) and

 Xk mean of the estimated energy band gap (Eg(est)). The estimation accura-
f Eg ; ω ¼ α i g i ðx ¼ a&cÞ þ b ð1Þ cy evaluation parameters are formulated using Eq.8, Eq.9, Eq.10 and
i¼1 Eq.11, respectively.
vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
u n
u1 X 2
Where gi(a, c)represents a set of nonlinear transformations while b RMSE ¼ t e ð8Þ
denotes the bias term which can be dropped by preprocessing the n i¼1 i
data to zero mean and α is a Lagrange multiplier.
Loss function L(Eg, f(Eg, ω))which measures the quality of estimation
of energy band gap of doped ZnO is defined by equation (2). 0 1
Xn
B j ei j C
1 B i¼1 C
 



 MAPD ¼ BB X100C
C ð9Þ


 n @X
 0; If
Eg −f Eg ; ω ≤ε
n
L Eg ; f Eg ; ω ¼ ð2Þ A
Eg − f Eg ; ω −ε; otherwise Egð expÞ
i¼1
 T.O. Owolabi et al. / Materials and Design 101 (2016) 277–284 279

Table 1
Statistical analysis of the dataset.

a (Å) c (Å) Eg (eV)

Mean 3.0587 4.8890 3.24

Maximum 3.6600 5.2530 3.54
Minimum 3.0690 4.9800 2.87
CC −18.5% −8.70%

n 
X  
0 0
Egið expÞ −Eg ð expÞ EgiðestÞ −Eg ðestÞ
i¼1
CC ¼ sffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi ð10Þ
X n  2 X n  2
0 0
Egið expÞ −Eg ð expÞ EgiðestÞ −Eg ðestÞ
i¼1 i¼1
Fig. 2. Correlation crossplot between the energy band gap of doped ZnO and the
vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi corresponding lattice parameter(c).
uX n
u
u Egiðest Þ
t
i¼1
Mean ¼ ð11Þ
n

Where ei and n represent error (difference between the experimen-
tal Eg(exp)and estimated Eg(est)value of energy band gap) and number of
data points, respectively. Eg(exp) and Eg(est) respectively represent the ex-
perimental and the estimated energy band gaps while E'g(exp) and E'g(est)
represent their mean values, respectively.
3. Experimental set up and description
and the degree of correlation is very weak. These weak correlations
show the capacity of linear relationship between the descriptors and
the target and can be directly inferred that the relationship between
them cannot be handled using a linear model. The crossplots presented
in Fig.1 and Fig.2 also give more insight about the non-linear relationship
between the energy band gap and lattice parameters as the disparities be-
tween them is so enormous.

3.1. Dataset description 3.2. Description of the adopted computational methodology

Modeling and simulation of SVRCI-based model was conducted using
sixty-one experimental lattice parameters and their correspounding en-
ergy band gaps drawn from literatures [5,13–25]. Statstical analysis was
carried out on the dataset in order to have some insight about the dataset.
The results of the analysis are presented in Table 1. The values of the
mean, maximum and minimum show the average value of the target (en-
ergy band gaps) and the descriptors (lattice parameters) as well as the
range of the content of the dataset. The coefficient of correlation between
energy band gaps and lattice parameters are also presented. Both basal
plane lattice constant (a) and the unit cell height perpendicular to the
basal plane hexagon (c) are negatively correlated with energy band gap
SVRCI-based model was developed using mathematical description
of SVR within MATLAB computing environment. Efficient computation
was ensured by randomization of the dataset before implementing it
for model development. The randomization refers to the systematic se-
lection of the data points into both training and testing set in the ratio of
eight to two. The training set of data was used to learn the relation be-
tween the experimental values of energy band gap and their corre-
sponding lattice parameters with the aid of developed SVR source
code using best parameters obtained through test-set-cross validation
technique [26]. The efficiency and the estimation capacity of the trained
model was assessed and validated using the testing set of data. The sta-
bility of the developed model was confirmed by repeating the

Fig. 1. Correlation crossplot between the energy band gap of doped ZnO and the
corresponding lattice parameter(a). Fig. 3. Effect of Gaussian kernel option on the performance of the model.
280 T.O. Owolabi et al. / Materials and Design 101 (2016) 277–284
Fig. 4. Effect of hyper-parameter lambda on the performance of the model.
experiment several times with the same values of parameters and the
developed SVRCI-based model showed consistency in its estimate. The
algorithm flow chart of the computational description is shown in Algo-
rithm 1 in appendix of this manuscript.
3.3. Optimization strategy
The significance of optimization techniques cannot be over-
emphasized and a lot of research has been conducted in this regard.
Among the available optimization techniques in the literature include
Cuckoo search algorithm [27,28], immune algorithm and Taguchi's
method [29], Particle swarm based approach [30] and artificial bee
colony-based approach [31] among others [32–35]. However, the opti-
mization strategy employed in this present work for obtaining the
best performance parameters associated with SVR was test-set-cross
validation technique. It involves tuning the user defined parameters
which include penalty factor, ε loss function, kernel option and hyper-
parameter λ. For each run of generated training and testing set, fitness
function (CC) is monitored for a group of penalty factor (bound on the
Lagrange multiplier), kernel option, ε and hyper-parameter λ (condi-
tioning parameter for quadratic programming methods). The experi-
ment is repeated for each of the available kernel function until
optimum performance is attained by the model. The model parameters
and the corresponding optimum values were noted, recorded and used
to train final SVR. The procedures are summarized in the Algorithm 2 in
the appendix.
3.4. Effect of SVR parameters on the performance of the developed SVRCI-
based model
The effects of SVR parameters on the performance of the developed
SVRCI-based model were investigated. The values of SVR parameters
Table 2
Optimum parameters for the developed SVRCI-based model.
Parameters Optimum value
C 100
ε 0.003
λ 0.1
Kernel function Gaussian
Kernel option 0.002
Table 3
Determinant of the estimation accuracy of the developed SVRCI-based model.
Determinant of estimation accuracy Value of estimation accuracy
CC 94.3%
MAPD 1%
Max.APD 6.5%
Min.APD 0.1%
depend on the dataset and vary from one dataset to another [10,26]. It
was observed that the penalty factor as well as ε has no profound effects
on the performance of the developed SVRCI-based model. However,
Gaussian kernel option and hyper-parameter λ have profound effects
on the performance of the developed model and their effects are
discussed as follows:
3.4.1. Effect of Gaussian kernel option on the performance of the developed
SVRCI-based model
The effect of Gaussian kernel option on the performance of the de-
veloped SVRCI-based model is presented in Fig.3. The performance of
SVRCI-based model during the training stage is relatively constant
when the value of the kernel option was set below 0.002 and falls grad-
ually as the value of kernel option increases above 0.002. The perfor-
mance of the model during the testing period increases from about
75% to 82% as the value of kernel option increases from 0.0002 to
0.002. The performance thereafter decreases to less than 40% as the ker-
nel option increases and then rises to around 40% before finally goes
down to less than 10% when the kernel option was set above 0.03. The
value of kernel option that optimizes the developed SVRCI-based
model was found to be 0.002.
3.4.2. Effect of hyper-parameter λ on the performance of the developed
SVRCI-based model
The effect of hyper-parameter λ on the performance of SVRCI-based
model is presented in Fig.4. The model performs well at high values of λ.
The performance of the model during testing stage gradually increases
as the value of λ increases and attained optimum value at 0.1. The per-
formance of the model during the training stage is relatively unchanged
as the value of λ progresses. It should be noted that the model shows
over-fitness at lower value of λ as depicted in Fig.4. The over-fitness
later disappeared at high values of λ. The optimum value of λ was ob-
tained as 0.1. The value of λ could not exceed this value due to high
Fig. 5. Pairwise correlation plot for training dataset.
 T.O. Owolabi et al. / Materials and Design 101 (2016) 277–284
Fig. 6. Pairwise correlation plot for testing dataset.
complexity developed by the model and was running for hours without
a unique solution when the value of λ exceeded 0.1. Since the perfor-
mance obtained is already satisfactory, then the simulation could not
proceed further in order to keep a good compromise between perfor-
mance and computational complexity. The optimum values of SVR pa-
rameters for the developed SVRCI-based model are listed in Table 2.
4. Results and discussion
The predictive and generalization ability of the developed SVRCI-
based model was evaluated and presented in Table 3. The model is char-
acterized with high correlation coeffients and low MAPD. MAPD for all
the data set including training and testing was obtained as 1% while
the correlation coefficient was obtained as 94.3%. The maximum abso-
lute percentage difference (max. APD) as well as the minimum absolute
percentage difference (min. APD) are 6.5% and 0.1%, respectively. The
pairwise correlation crossplots between the estimated and experimen-
tal energy band gaps for the training and testing stage of the developed
SVRCI-based model are presented in Fig.5 and Fig.6, respectively. The
correlation coefficient of 98.6% was obtained for the training dataset
while 82.7% was obtained for testing dataset. The cross plots show
Fig. 7. Doping effect of Sm on energy band gap of ZnO using the developed SVRCI-based
model.
281
Fig. 8. Effect of Ag on energy band gap of ZnO using the developed SVRCI-based model.
good alignment as the points are close to each other and this alignment
can be attributed to the effectiveness of the proposed model. Similarly,
RMSE of 0.03 and 0.1 were respectively obtained for the training and
testing set of data.
4.1. Investigating the effect of dopant on the energy band gap of ZnO using
the developed SVRCI-based model
The effect of doping on the energy band gap of ZnO was investigated
using the developed SVRCI-based model and the estimated band gap
was compared with experimental results. Fig.7 shows the doping effect
of samarium (Sm) in ZnO as estimated using the developed SVRCI-
based model through lattice parameters as the input to the model. The
model uses the lattice parameters of the prepared samples for its esti-
mation. The estimated results agree well with the experimental values
[13]. The figure depicts that the energy band gap of ZnO increases
with increase in the percentage concentration of Sm. This trend of in-
crease is also replicated by the developed SVRCI-based model. Similarly,
the effect of silver (Ag) particles on the energy band gap of ZnO is pre-
sented in Fig.8. The developed SVRCI-based model shows that the ener-
gy band gap of ZnO decreases with increase in the concentration of Ag.
The same trend is reported in the experiment [23]. It should be noted
Fig. 9. Effect of Al on energy band gap of ZnO using the developed SVRCI-based model.
282 T.O. Owolabi et al. / Materials and Design 101 (2016) 277–284
Fig. 10. Effect of annealing temperature on energy band gap terbium doped ZnO using the
developed SVRCI-based model.
that the developed SVRCI-based model uses the values of experimental
lattice parameters reported for Sm-doped ZnO [13] and Ag-doped ZnO
[23] to make its estimation.
The effect of aluminum (Al) doping on energy band gap of ZnO is
also presented in Fig.9. Comparison of the results of the developed
SVRCI-based model with experimental values shows excellent agree-
ment. The precision displayed by the developed model shows its excel-
lent predictive ability and can therefore be implemented for estimating
the effect of other dopants on the energy band gap of ZnO.
4.2. Investigating the effect of annealing temperature on the energy band
gap of Tb-doped ZnO using the developed SVRCI-based model
Annealing temperature is one of the factors that distort the crystal
lattice structure of materials and consequently alters the energy differ-
ence between the highest energy level of valence band and lowest ener-
gy level of conduction band in ZnO semiconductor. The effect of
temperature on the energy band gap of Tb-doped ZnO is presented in
Fig.10. The results of the developed model agree well with the experi-
mental values [18]. The developed model can also be used to investigate
the effect of annealing temperature on ZnO semiconductor doped with
other materials.
Fig. 11. Effect of deposition substrate on energy band gap of ZnO using the developed
SVRCI-based model.
Fig. 12. Effect of Sn on energy band gap of ZnO using the developed SVRCI-based model.
4.3. Investigating the effect of the nature of deposition substrates on the en-
ergy band gap of ZnO using the developed SVRCI-based model
The effect of the deposition substrates on the energy band gap of
ZnO is also investigated and presented in Fig.11. The figure shows that
ZnO deposited on glass substrate has lower energy band gap as com-
pared to ZnO deposited on Al/glass substrate. The results of the model
agree well for the ZnO deposited on glass substrate and Al/glass sub-
strate. The result of the developed SVRCI-based model deviates slightly
for ITO/glass substrate. (See Fig. 12.)
4.4. Investigating the effect of tin on the band gap of ZnO using the
developed SVRCI-based model
The experimental report shows that the incorporation of tin dopant
into crystal structure of ZnO has little or no effect on the crystal lattice
structure [5]. The lattice parameters of ZnO changed slightly at high con-
centration of tin. In order to explore the universality of the developed
SVRCI-based model and further show that it accounts for change in
the band gaps of ZnO due to the introduction of dopants that has no
or little distortion on the lattice parameters, the effect of Sn on the
band gap of ZnO was investigated and the results are presented in
Fig.12. The estimated band gaps agree well with the reported experi-
mental values [5]. Although, incorporation of tin does not change lattice
parameters, it changes the energy band gap slightly.
5. Conclusion and recommendation
SVRCI-based model was developed for estimating the energy band
gaps of doped ZnO semiconductor using experimental lattice parame-
ters as the input to the model. The developed model estimates the effect
of several dopants on ZnO with high degree of accuracy. The developed
model also estimates the variation in energy band gaps of doped ZnO
due to annealing temperature as well as the nature of the deposition
substrate. The universality of the developed model was confirmed by
using the model to estimate the band gap of Sn-doped ZnO that shows
little or no lattice distortion upon varying the concentration of dopant.
Comparison of the estimated energy band gaps with experimental
values shows excellent agreement. The precision of the developed
model suggests its extra-ordinary ability to relieve the experimental
stress entailed in energy band gap measurements. Incorporation of the
developed model into microchips is recommended in order to facilitate
its real life applications.
 T.O. Owolabi et al. / Materials and Design 101 (2016) 277–284 283

Appendix A. Appendix

Algorithm 1: Computational procedures involved in developing SVRCI-based model.

284 T.O. Owolabi et al. / Materials and Design 101 (2016) 277–284
Algorithm 2: Optimization algorithm.
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