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Synthesis and Reactivity in Inorganic, Metal-Organic,

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Investigation of Structural, Morphological, Optical and

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Electrical Properties of Al Doped Zno Thin Films Via
Spin Coating Technique
ab d b c d
Mehmet Yilmaz , Demet Tatar , Erdal Sonmez , Cagri Cirak , Sakir Aydogan & Rustu
e
Gunturkun
a
Department of Elementary Science, Faculty of Education, Ataturk University, 25240,
Erzurum/Turkey
b
Advanced Materials Research Laboratory, Department of Nanoscience and
Nanoengineering, Graduate School of Natural and Applied Sciences, Ataturk University,
25240, Erzurum/Turkey
c
Department of Physics, Faculty of Science, Erzincan University, 24100, Erzincan/Turkey
d
Department of Physics, Faculty of Science, Ataturk University, 25240, Erzurum/Turkey
e
Department of Electrical and Electronics Engineering, Faculty of Technology, Dumlupinar
University, 43500, Simav, Kütahya/Turkey
Accepted author version posted online: 01 Jun 2015.

To cite this article: Mehmet Yilmaz, Demet Tatar, Erdal Sonmez, Cagri Cirak, Sakir Aydogan & Rustu Gunturkun
(2015): Investigation of Structural, Morphological, Optical and Electrical Properties of Al Doped Zno Thin Films
Via Spin Coating Technique, Synthesis and Reactivity in Inorganic, Metal-Organic, and Nano-Metal Chemistry, DOI:
10.1080/15533174.2014.988795

To link to this article: http://dx.doi.org/10.1080/15533174.2014.988795

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 ACCEPTED MANUSCRIPT

INVESTIGATION OF STRUCTURAL, MORPHOLOGICAL, OPTICAL AND

ELECTRICAL

PROPERTIES OF Al DOPED ZnO THIN FILMS VIA SPIN COATING TECHNIQUE

Mehmet Yilmaz1,2*, Demet Tatar4, Erdal Sonmez2, Cagri Cirak3, Sakir Aydogan4, Rustu

Gunturkun5
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1
Department of Elementary Science, Faculty of Education, Ataturk University, 25240,

Erzurum/Turkey
2
Advanced Materials Research Laboratory, Department of Nanoscience and

Nanoengineering,

Graduate School of Natural and Applied Sciences, Ataturk University, 25240,

Erzurum/Turkey
3
Department of Physics, Faculty of Science, Erzincan University, 24100, Erzincan/Turkey
4
Department of Physics, Faculty of Science, Ataturk University, 25240, Erzurum/Turkey
5
Department of Electrical and Electronics Engineering, Faculty of Technology,

Dumlupinar University, 43500, Simav, Kütahya/Turkey

*Corresponding author

E-mail: mehmetyilmaz@atauni.edu.tr; yilmazmehmet32@gmail.com

Address: Advanced Materials Research Laboratory, Department of Nanoscience and

Nanoengineering, University of Ataturk, Erzurum, 25240, Turkey

ABSTRACT

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In this study, Al doped ZnO thin films were synthesized by sol gel spin coating technique. To

investigate the effect of Al doping on ZnO properties, Al doping concentration was diversified

in the range of 0 mol. % - 5 mol. % The effect of Al doping on structural, morphological, optical

and electrical properties of ZnO thin films was evaluated by XRD, SEM, UV-VIS and four point

probe measurements. All results whether pure or Al doped ZnO thin films were described in
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detail and they indicated that the films prepared in this study can be used in many

nanotechnological applications.

Keywords: ZnO thin films, Sol-gel technique, Al doping.

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INTRODUCTION

Recently, nanostructured semiconductors have been widely used for the nanotechnological

applications. Because of their high chemical flexibility and synthetic tunability, the II-VI groups

of nanostructured semiconductors are very attractive materials [1]. Among them, ZnO has a

commercial potential, due to low cost and excellent properties such as high transparency in the
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visible region and chemical stability [2-3]. Also, ZnO has a direct wide bandgap energy (3.37eV)

and large exciton binding energy (60 meV). These properties make ZnO one of the most

favorable candidates for the optoelectronic applications such as light emitting diodes, optical

sensors, lasers etc. [2-4]. ZnO can be obtained n-type and p-type semiconductor identified by the

dopant properties. While group-III elements such as aluminum (Al), gallium (Ga), indium (In)

and Boron (B) are used to obtain n-type ZnO and group V elements such as Nitrogen (N),

phosphorous (P), arsenic (As) and antimony (Sb) are used for p-type [5-6]. To improve the

performance of ZnO based devices, it is necessary that nanostructured and high quality ZnO thin

films should be grown [7]. Electrical and optical properties of pure ZnO can be developed by

doping Al. ZnO:Al thin films have some advantages such as adjustable band-gap and high c-axis

directed crystalline structure along (0 0 2) plane [4]. ZnO:Al thin films are produced by pulsed

laser deposition [8], RF magnetron sputtering [9], spray pyrolysis [10], sol-gel [11], etc. In this

study, pure and Al doped ZnO (hereafter ZO and AZO) thin films are prepared by sol-gel spin

coating technique. This technique has several advantages such as broad deposition area, low cost

for the technological applications and easy to use [12-13]. We also investigated the effects of Al

dopants on the structural, morphological, optical and electrical properties of ZnO thin films.

EXPERIMENTAL

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ZO and AZO thin films were prepared by sol-gel spin coating technique onto glass substrate.

Zn(CH3COO)2∙2H2O was used for starting precursor and Al(NO3)3∙9H2O was used as Al dopant

sources. To prepare the solution, 2-methoxyethanol and ethanolamine were used respectively as

a solvent and stabilizer. For this purpose, firstly zinc acetate dihydrate was dissolved in a mixture

of 2-methoxyethanol and ethanolamine. Molar ratios of Zn/ethanolamine and zinc acetate

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dihydrate were adjusted respectively at 1.0M, 0.5M. To investigate effects of Al dopant on the

features of ZnO thin films, the molar ratios were altered at 0, 2.0, 3.0, 4.0, 5.0 mole %. Final

solutions were stirred at 60°C about 2h and obtained clear, homogenous solution. The glass

substrates washed before using with detergent and then rinsed in methanol, acetone and

deionized water by an ultrasonic cleaner respectively [14]. Following the process, AZO thin

films were coated onto glass substrates by a spin coating method. This method was carried out at

room temperature and the rate of rotations 3600 rpm for 30s. In order to get rid of organic

residuals, synthesized films were preheated at 200°C for 5 min after each coating. This procedure

was repeated 7 times. Finally the films were annealed in oxygen atmosphere at 450°C for 1 hour

by an electrical tube furnace. Oxygen flow rate was kept fixed for all samples.

Crystal structures of AZO thin films were analyzed by X-ray diffraction (XRD) using Rigaku

D/Max III C diffractometer with CuKα radiation (λ=1. 5418 Å) at 30kV,10mA. Surface

morphology was evaluated by scanning electron microscope (SEM). Besides, optical and

electrical properties of ZO and AZO films were determined by UV-VIS spectroscopy

measurement, four probe point measurement.

Structural properties

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The structural features of pure and Al doped ZnO thin films have been evaluated by XRD

measurement. Typical XRD patterns of the films are shown in Figure 1. Accordingly, all samples

exhibit a poly-crystalline hexagonal wurtzite structure and there is no impurity peak such as Al

in the films. These results are in harmony with JCPDS card no: 99-0111. Additionally, the

intensity of the (002) plane has decreased with the increasing Al concentration from 0 to 5 mole
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%. Due to the fact that Al3+ ions, entering the ZnO structure, have a small radius compare with

the Zn2+ ions, the ZnO crystal structure affected by Al doping [15-16]. Muiva et al. [17] have

also faced with the same situation as in Al doped ZnO thin flms deposited by spray pyrolysis

technique and they said that increasing Al concentration led to random orientation. Because of

this, (002) peak orientation decrease with increasing doping content.The lattice constants a and c

of the hexagonal structure have been determined by the following formula [18]

( )
( ) (1)

where d is the interplanar distance and h,k,l are miller indices. The calculated a and c lattice

constants are shown in Table 1. These values are very close with JCPDS 99-0111 (a=b=3. 25Å,

c=5. 20Å). It indicates that lattice constants are not much affected by the Al doping. Generally,

the average grain size is calculated at the most intense peak. In this study average particle sizes

are calculated at (002) peak by using Scherrer equation [19].

(2)

where λ is the X-ray wavelength of 1.5418Å, ϴ is the Bragg’s angle and β is the full-width half-

maximum (FWHM) in radians. The grain size values about the samples are given in Table 1. For

(002) peak, calculated D values have decreased with increasing Al concentration. The misfit

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stress has a negative impact on the structural parameters. This effect occurs if there is a

geometric mismatch at inter phase boundaries between the crystalline lattice of films and

substrates. Because of this, these stresses can cause microstrains in the films to form [20-21].

The microstrain (ε) values have been identified by following expression [22].

(3)
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where β is the FWHM and ϴ is the Bragg’s angle. Calculated ε values are given in Table 1.

According to the Table 1, it can clearly be said that ε values increase with increasing Al

contribution. As Al contribution leads to structural disorders in the ZnO’s crystal structure, this

is an expected result.

The dislocation density (δ) which is the measure of the amount of the defects in crystal

structure have been described as the length of the dislocation lines per unit volume (lines/m2).

The dislocation density of the films has been estimated using following formula [23].

(4)

For (002) peak, the dislocation density values are given in Table 1. These values have shown a

tendency to rise with the increase of Al concentration.

Morphological properties

Figure 2 has shown surface morphologies in ZO and AZO thin films. It has been obtained from

the SEM images that surface morphology has nanoparticle network structures. Also, these

structures have depended on the Al doping concentration. When the Al doping concentration

increases from 2 to 3 mole %, nanonetwork structures have sharp lines. With the further Al

concentration (4-5 mole %), these structures have begun to deteriorate. In fact, this kind of

surface morphology is expected in ZnO thin films derived from sol-gel spin coating technique.

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According to the Scherer [24] , this has caused by considerable loss of hydroxy or alkoxy groups

from the precursor solution during the sintering process. Finally, the composition of elements

such as Zn, O, Si and Al are confirmed by energy dispersive x-ray (EDX) spectra and results are

presented in Table 2. It is thought that Si peak comes from the glass substrate because the

electron penetration depth is higher than the film thickness. According to the EDX spectra, ZO
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and AZO thin films’ Al/Zn (at.%) atomic ratio distributions have shown similarity with the

starting solution’s distribution.

Optical properties

Optical properties of ZO and AZO thin films have been evaluated by UV-VIS spectrometer at

room temperature. Figure 3a has shown optical transmittance in ZO and AZO thin films. From

the transmittance curves, it is observed that the transmittance of ZO film is slightly affected by

the Al doping concentration. Especially at lower wavelengths, the transmittance has raised with

increasing Al concentration. All films have demonstrated a transmittance higher than %80 in the

visible region. These results have shown that all films have a high transparency and sharp

absorption edge.

The absorption coefficient (α) is calculated using with following formula [25].

(5)

where I/I0 ratio is transmittance and t is the thickness of the films. The optical band-gap of ZO

and AZO thin films are defined as [26].

(6)

where α is the absorption coefficient, B is a constant, hυ is the photon energy and Eg is the band-

gap. The effect of Al doping on Eg have been investigated by plotting (αhυ)2 vs hυ. The point

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which coincided with extrapolated plot and the energy axis have been defined as Eg. It has been

clearly observed in the Figure 3b that ZO thin films’ optical band gap have been quietly effected

by Al doping. The band-gap values of ZO and AZO-2, AZO-3, AZO-4, AZO-5 thin films have

been calculated as 3.279 eV, 3.286 eV, 3.295eV, 3.309eV, 3.314eV, respectively. This result

shows that Eg value has risen with increasing Al doping concentration. Mridra and Basak [27]
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also reported that the optical band gap values of sol-gel spin coated ZO thin films increased from

3.33 eV to 3.70 eV with Al doping concentration.This experience can be explained by Burstein-

Moss effect. ZnO is one of the most degenerate semiconductors. In this case, fermi level , inside

the conduction band and its position depend on the concentration of free electrons. Identified

band gap, not real band gap, related to the excitation of the electrons from the valence band to

fermi level [28-29]. When the Zn2+ substitutes with Al3+, free electron density begins to increase.

Thereby, fermi level which lies on the conduction band leads to an energy band widening effect

called “blue shift”. On the other hand, this case can be expressed with Urbach energy. In the

low energy region the spectral dependence of α is expressed by the Urbach formula [30].

(7)

Where α0 and E0 are the characteristic parameters of the material and E u is related to the energy

width of the Urbach tail. Equation (7) has explained the optical transition between occupied

states in valance band tail to unoccupied states of the conduction band [31]. In this context, the

Urbach tail occurrence is owing to the structural disorder, caused by the defects and doping in

the films. When equation (7) is considered, a plot of ln(α) versus hυ should be linear and Urbach

energy can observed from the slope.[31-32]. Accordingly , The Urbach energy has been

determined from the variation of lnα versus photon energy (Figure 4). The calculated Eu values

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have been presented in Table 2. According to the results, Urbach energies have decreased with

Al corporation. Generally, there is a reverse relationship between optical band gap and Urbach

energy. This can clearly be observed in Figure 5. To identify steepness parameter (ζ) which

characterizes width of the straight line near the absorption edge eq.(7) can be rewritten

( ) (8)
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where ζ is the steepness parameter, T is the room temperature and kB is the Boltzmann constant.

Eu is associated with the slope absorption edge and ζ is calculated;

(9)

The steepness parameter is calculated from eq.(9) and represented in Table 2. From the

calculated (ζ) values , we can conclude that it increases with decreasing EU values.

Electrical properties

The electrical properties of ZO and AZO thin films have been evaluated by four point probe

method and it is found that all samples have n-type conductivity. The sheet resistance values

have been presented in Table 2. These values vary between 770MΩ (for ZO) to 14.5MΩ (for

AZO-3). According to the results, sheet resistance values have decreased sharply at a rate of 2 -3

mole % with Al doping application and then increased with further doping concentration. The

ZO thin film has a considerable surface resistivity and this case can be explained with annealing

procedure. Owing to the heavy amounts of oxygen in the annealing atmosphere, oxygen

vacancies have decreased in the meantime. Consequently, sheet resistance has increased

dramatically. Similar results have been observed by R.Kim et al [33]. Additionally, the Al doping

effect can be explained by Al3+ atoms’ replace with Zn2+ atoms. The substitution of Zn2+ sites of

in the ZnO structure with Al3+ atoms is expressed by following formula [34]

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+ (10)

As a result of eq.(10), carrier concentration has risen with increasing Al dopant concentration

between 2 and 3 mole %. This has caused higher amount of formation of conduction electrons

and oxygen vacancies. Moreover, increasing sheet resistance between 4 and 5 mole % can be

clarified with increasing defects and lattice distortions due to high dislocation density and
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microstrain values observed from XRD analysis with more Al doping content.

Conclusion

In the present study, ZO and AZO thin films were successfully synthesized by sol-gel spin

coating technique. XRD results showed that all films had polycrystalline nature with hexagonal

wurtzite structure. The study revealed that crystallite of the films highly depended on the Al

doping. According to the SEM images, the films were formed like nanonetwork structure. All

samples had 80% optical transmittance in the visible region.The optical band gap increased from

3.279 eV to 3.314 eV and Urbach energy, decreased from 111 meV to 87 meV with various Al

doping concentrations. Besides, sheet resistance sharply decreased from 770 MΩ to 14.5 MΩ

with 3 mole % Al doping concentration and it was up to 82.25 MΩ for latter concentration.

Based on these results, some properties of ZO thin films were adjustable with Al contributions.

Consequently, AZO thin film could be an ideal candidate for nanotechnological applications.

Acknowledgement

This research was supported by Ataturk University Research Fund, Project Number 2013/152.

Corresponding author (Mehmet Yilmaz) is grateful to Esra Yilmaz (Dumlupinar University) for

technical support.

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Table 1. Some structural parameters of ZO and AZO thin films

Lattice
- 14 -
Sample 2ϴ FWHM ε (x10 δ (x10 linesm Constant
hkl d (Å) D(nm) 4 2 (Å)
name (deg.) (deg.) ) )
a c
100 32.272 2.7716 0.284
002 34.925 2.5670 0.227 36.73 31.51 7.41 3.20 5.18
ZO
101 36.733 2.4446 0.297
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100 32.293 2.7698 0.466

002 34.925 2.5669 0.287 29.05 39.83 11.85 3.19 5.18
AZO-2
101 36.761 2.4428 0.266
100 32.371 2.7634 0.409
002 34.967 2.5639 0.300 27.79 41.64 12.95 3.19 5.24
AZO-3
101 36.736 2.4444 0.393
100 32.503 2.7524 0.205
002 34.948 2.5653 0.367 22.72 50.94 19.37 3.17 5.14
AZO-4
101 37.016 2.4266 0.344
100 32.435 2.7581 0.352
002 34.880 2.5701 0.385 21.65 53.44 21.33 3.18 5.23
AZO-5
101 36.811 2.4396 0.352

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Table 2. Morphological, band gap, Urbach energy and steepness parameter values for ZO and

AZO films

Samples Al/Zn at.% Eg (eV) Eu (meV) ζ (x10-2) Rs(MΩ/sq)

ratio
ZO 0 3.279 111 23.29 770
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AZO-2 1.27 3.286 102 25.34 39.64

AZO-3 2.68 3.295 95 27.21 14.5
AZO-4 3.96 3.309 94 27.50 80.18
AZO-5 4.84 3.314 87 29.71 82.25

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Figure 1. XRD patterns of pure and Al doped ZnO thin films

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(a)

(b)
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(c)

(d)
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(e)
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Figure 2.SEM images and EDX spectra of Al doped ZnO thin films a) pure b) 2 mol.%Al doped

c) 3mol.% Al doped d) 4 mol.% Al doped e) 5 mol.% Al doped

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Figure 3. a) Optical transmittance spectrum of ZO and AZO thin films and b) the plot of (αhυ) 2

vs (hυ) for the ZO and AZO thin films.

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Figure 4.The Urbach plots of the ZO and AZO thin films

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Figure 5. Plot of Urbach energies and optical band gap vs different mole percent values of Al

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