Optik 124 (2013) 491492

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Optik
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Fabrication and characterization of ZnO thin lm using solgel method

A.J. Hashim , M.S. Jaafar, Alaa J. Ghazai, N.M. Ahmed
Nano-Optoelectronics Research and Technology Laboratory, School of Physics, Universiti Sains Malaysia, 11800 Pinang, Malaysia

a r t i c l e

i n f o

a b s t r a c t
In this work, the solgel method used to fabricate zinc oxide (ZnO) thin lm on silicon (Si) substrate. To this purpose, zinc acetate dihydrate and monoethanolamine were used as solvent and stabilizer materials respectively. Structural and optical properties of ZnO lms were studied. X-ray diffraction (XRD) analysis of the lms showed polycrystalline nature of the prepared lms. Depend on XRD peak of ZnO lm with orientation (1 0 0), therefore, Scherrers formula was used to calculate crystallite size of prepared lms. Scanning electron microscopy (SEM) used to describe the surface morphology and Photoluminescence (PL) measurements revealed the energy bandgap of the lms was in UV emission at 380 nm. Finally, thickness of the lms was measured with Filmetric (F-20). The result showed that we successful to fabricate ZnO lms in simple and low cost method with high quality. 2012 Elsevier GmbH. All rights reserved.

Article history: Received 2 August 2011 Accepted 14 December 2011

Keywords: ZnO SolGel Spin coat SEM

1. Introduction Znic oxide (ZnO) is an oxidic compound naturally occurring as the rare mineral zincite, which crystallizes in the hexagonal wurtzite structure Pb3 mc [1]. Good properties of ZnO were reported with special emphasis on the use of ZnO as transparent conductive electrode in thin lm solar cells. As well as, ZnO have specic properties such as low costs, nontoxicity, high transparency in VIS/near IR spectral region, good contacts to the active semiconductors (absorb layers), and others [2]. These numbers of properties make ZnO as a one of promising semiconductor materials to use in many scientic and industrials areas such as piezoelectric tranducers, optical waveguides, acousto-optic media, conductive gas sensors, and varistors [3]. In the past decades, silicon (Si) had also attracted considerable interests due to the characteristics of low costs, high resistance, strong absorbability, and its potential application in the development of Si-based optoelectronic devices [4]. ZnO thin lms have been prepared by a variety of thin lm deposition techniques, such as pulsed-laser deposition, RF magnetron sputtering, chemical vapor deposition, spray pyrolysis, and solgel process [5]. Among them, the solgel technique offers the possibility of preparing a small at low cost for technological applications. In this work, ZnO lms grown on silicon substrates using solgel method were fabricated and intensively investigated. Many parameters were studied in order to fabricate lms with high quality.

2. Materials and methods ZnO thin lms grown on Si substrate using spin coating method and the deposition process have been reported. Si substrates were cleaned thoroughly and the cleaning procedures achieved using the RCA method. In spin coating method, the seed layer was rstly coated with spinon solgel method which has molar ratio of monoethanolamine (MEA) and zinc acetate Zn(CH3 COO)2 2H2 O equal to 1:4, and the concentration of zinc acetate equal to 0.548 mol/L [6]. The solgel layers were followed two steps heat treatment in order to optimize the seed layer properties which will improve the uniformity grain structure. Thickness of lms was measured by using optical reectometry system Filmetric F20-VIS. The crystalline structure of the lm was studied using high resolution X-ray diffraction (HRXRD) Model; PANalytical Xpert Pro MRD with a Cu K1 radiation source of The microstructure of the lms were studied by imag= 1.5406 A. ing the morphology of the lms surface using scanning electron microscopy (SEM), while the photoluminescence (PL) spectra were recorded using photoluminescence spectroscopy system Model: Jobin Yvon HR 800 UV with HeCd laser of 325 nm excitation source.

3. Results and discussion 3.1. Structural properties The crystal structure of ZnO lm was studied using high resolution X-ray diffraction (XRD). XRD spectra of ZnO lms were showed in Fig. 1. The XRD peaks of 31.92 , 34.77 , 36.17 , 47.57 ,

Corresponding author. E-mail address: abduljalelphys@gmail.com (A.J. Hashim). 0030-4026/$ see front matter 2012 Elsevier GmbH. All rights reserved. doi:10.1016/j.ijleo.2011.12.059

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A.J. Hashim et al. / Optik 124 (2013) 491492

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Intensity (a.u)

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ZnO (102)

20

10

0 30 40 50 60

2 (degrees)

ZnO ()

ZnO (110)

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ZnO (100)

ZnO (101)

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ZnO (002)

Fig. 2. SEM image of ZnO thin lms prepared using spin coating method.

Fig. 1. XRD spectrum of ZnO thin lms prepared using spin coating method.

and 56.17 were correspond to ZnO (1 0 0), (0 0 2), (1 0 1), (1 0 2), and (1 1 0) respectively. Theses peaks conrmed that the lms are polycrystalline in nature. In order to attain the detailed structure information, the grain size along the c-axis was calculated according to the Scherrer formula [7]: D= 0.9 B cos (1)

where is the X-ray wavelength, is Bragg angle of (0 0 2) peak, and B is FWHM value. The grain size of ZnO on Si was 4.87 nm, it shows that the grain become more uniform and bigger in size on our sample. The average uniform strain zz for the lattice along the c-axis in the randomly oriented ZnO lms deposited on Si substrate has been estimated from the lattice parameters using the equation below: zz = c co 100% co (2)

Fig. 3. Photoluminescence (PL) spectrum of ZnO thin lms prepared using spin coating method.

where co is the lattice constant for the unstrained ZnO. The numerical value of c is calculated from XRD data according to the following equations: 2dh k l sin = (3)

where dh k l is the lattice spacing of (h k l), (is the X-ray wavelength and is Bragg angle. At the same time, ZnO is a hexagonal structure which follows the formula [7]: dh k l = 1 4/3(h2 + hk + k2 )/a2 + l2 /c 2 (4)

emission (NBE) due to the electronic transition from near conduction band to valence band. The other one is in the visible region which may be due to the defect related deep level emission. The UV emission peak was found to be at 391.5 nm for the sample. Second luminescence peak shows a broad greenyellow band peaked at 521.0 nm was observed for the sample. The Eg also could be derived from the PL spectra. The value was found to be 3.16 eV for ZnO on Si. This result is blue shift to the bulk ZnO Eg which equal to 3.37 eV. In summary, the high quality ZnO lm on Si substrate was fabricated. The low grain size and smoothly surface observed in the ZnO sample. ZnO lm has two PL peaks with high intensity in UV region at 391 nm make it promising to use in near UV optoelectronic devices. References
[1] G. Haacke, New gure of merit for transparent conductors, Appl. Phys. Lett. 47 (1976) 40864089. [2] E. Klaus, K. Andreas, R. Brend, Transparent Conductive Zinc Oxide Springer Series in Material Science, vol. 104, 2008, p. 446. [3] N.H. Nickel, Zinc OxideA Material for Micro and Optoelectronic Applications, Springer, 2005. [4] J.H. Lee, K.H. Ko, B.O. Park, Electrical and optical properties of ZnO transparent conduction lms by the solgel method, J. Cryst. Growth 247 (2003) 119125. [5] E. Sub, S.H.S. Kang, J.S. Kang, J.H. Kim, S.Y. Lee, Effect of the variation of lm thickness on the structural and optical properties of ZnO thin lm deposited on sapphire substrate using PLD, Appl. Surf. Sci. 186 (2002) 474476. [6] International Center for Different Datas, Joint Committee on Powder Diffraction Standards, Swarthmore, PA, 1986, pp. 361451. [7] R. Ghosh, D. Basak, S. Fujihara, Effect of substrate-induced strain on the structural, electrical, and optical properties of polycrystalline ZnO thin lms, J. Appl. Phys. 96 (2004) 26892696.

where a and c are the lattice constants. The calculated c of ZnO thin lm is 0.5212 nm, using co for ZnO of 0.52 nm [6]. The strain was equal to 0.23% for the ZnO thin lm deposited on Si substrate. Negative value of the strain in the lm means that the sample is in a tensile condition. The surface morphology of fabricated ZnO thin lms onto Si substrate using SEM was investigated. The SEM image of ZnO lms is shown in Fig. 2 which indicated that the deposited ZnO thin lm on Si substrate has rough surface morphology and relatively big particles which are well connected to each other. 3.2. Optical properties The PL spectrum of the prepared ZnO thin lm on Si is shown in Fig. 3. Two luminescence peaks can be observed in the sample, the rst peak is the UV emission corresponding to the near band edge