A Solution Processed ZnO Thin Film

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1 Applied Mechanics and Materials Vols (2013) pp Online available since 2012/Dec/13 at (2013) Trans Tech Publications, Switzerland doi: / A Solution Processed ZnO Thin Film Yuh-Chung Hu 1, a, David T.W. Lin 2, b, Hai-Lin Lee 3, c and Pei-Zen Chang 3, d 1 Department of Mechanical and Electromechanical Engineering, National ILan University, ILan, Taiwan 2 Graduate Institute of Mechatronic System Engineering, National University of Tainan, Tainan, Taiwan 3 Institute of Applied Mechanics, National Taiwan University, Taipei, Taiwan a ychu@niu.edu.tw, b david@mail.nutn.edu.tw, c hllee@ntumems.net, d changpz@ntu.edu.tw Keywords: Thin Film Transistor, Thin Film Property, ZnO, Solution Process. Abstract. The effect of Zinc-Oxide (ZnO) thin film annealed in different ambiences is presented. To achieve low cost and environmentally friendly process, ZnO aqueous solution is synthesized by dissolving zinc acetate dihydrate in deionized water directly. Zinc oxide aqueous solution of high solubility and stability is presented. High quality and dense Zinc oxide thin film is formed by spin coating. Annealing temperatures are in the range of 300 C~500 C, and annealing ambiences of both air and N 2 are discussed. Introduction The oxide semiconductor has drawn much attention because of the application in the next-generation displays. ZnO, an II-IV compound semiconductor, has been widely investigated in recent years because of its attractive properties such as wide direct band gap, high excitation binding energy, optical transparency, biocompatibility, piezoelectricity, and pyroelectricity. There are several applications in sensors [1]-[5], transparent Thin Film Transistor (TFT) [6]-[8], flexible electronics [10], light emitting device [10]-[12]. There are many methods for depositing ZnO thin film, such as pulsed laser deposition, atomic layer deposition, ion beam sputtering, RF sputtering, spray pyrolysis, chemical bath deposition, inkjet printing [13], and so on. Post annealing is a common treatment to improve the quality of thin film. In this paper, we employ solution process to grow ZnO thin film. We demonstrate an extremely environmentally friendly and simple ZnO aqueous solution. The effects of post-annealing temperature under different ambiences, namely air and N 2, on the electrical characteristics of ZnO thin film are investigated. A better post-annealing temperature is defined based on Thermogravimetric Analysis (TGA). Experimental Detail ZnO precursor solution was synthesized by dissolving zinc acetate dihydrate in DI water to the concentration of 0.5 M. After rigorous stirring at room temperature for 1 hr, the ZnO aqueous solution revealed high solubility, stability, and transparency. The ZnO thin film was carried out by spin coating followed by annealing in ambience of both air and N 2 for 1 hr. The annealing temperatures are varied between 300 C and 500 C selected by taking the result of TGA analysis into account. ZnO thin film was deposited on glass substrate by spin coating at 500 rpm/10s followed by 1500 rpm/30s. The ZnO thin films were preheated at 150 C on hot plate to desiccate moisture followed by annealing in furnace in ambiences of both air and N 2 at the temperatures varied between 300 C and 500 C for 1 hr. The thermal property of ZnO was investigated by TGA with the heating rate of 10 C /min. The crystalline quality was examined by x-ray diffraction (XRD) performed by PANalytical X Pert PRO MRD at 45 kv and 40 ma with Cu Kα radiation (λ=0.154 nm). Absorbance and transmittance spectrum were measured by Lambda 900-TNO manual reflectance/transmittance, UV-VIS spectrometer. Surface morphology was observed by JEOL JSM-7600F, high resolution scanning electron microscopy. All rights reserved. No part of contents of this paper may be reproduced or transmitted in any form or by any means without the written permission of TTP, (ID: /01/13,01:10:59)

2 1586 Measurement Technology and its Application Results and Discussion As shown in Fig. 1, the weight loss in the range from room temperature to 100 C is due to the evaporation of solvent while the second weight loss at 150 C to 250 C was dramatic and is attributed to the decomposition of residual organic compounds. As shown in Fig. 2, the diffraction peaks (100), (002), and (101) imply that ZnO crystals are wurtzite structure and comprised of hexagonal column. Moreover, the prevailing peak (002) indicates the crystal lattice with preferential c-axis orientation perpendicular to the substrate. The other minor diffraction peaks stand for crystal with random orientation. Diffraction peaks of ZnO thin film annealed at 300 C in air are obscure, which indicates that the crystalline quality is unfavorable. Diffraction peaks of ZnO thin film annealed at 400 C and 500 C in air show stronger intensity, which means that crystalline quality enhanced. The foremost diffraction peak (002) is more predominant at 500 C in air and diffraction peaks (100) and (101) are relatively weaker, which indicates the majority of ZnO crystals are with preferential c-axis orientation. The ZnO thin films annealed in N 2 have more distinct diffraction peaks than that annealed in air no matter at the annealing temperature of 300 C, 400 C, and 500 C. The intensity of diffraction peak (002) increased gradually with increasing annealing temperature. Fig. 3 shows the morphology of ZnO thin films. Fig. 3(a) shows that the crystallites of ZnO thin film annealed at 300 C in air are unclear. Fig. 3(b) and (c) show obvious progress at the annealing temperature of 400 C and 500 C in air. The grain sizes grow larger with increasing annealing temperature. ZnO crystallites annealed at 500 C in air grow dramatically even reaching the size of 120 nm. Fig. 3(d) shows distinct crystallites at the annealing temperature of 300 C in N 2. At the annealing temperatures of 400 C and 500 C, as seen in Fig. 3(e) and (f), the grain sizes grow drastically with annealing temperature rising. The grain sizes at 500 C in N 2 attaining around 120 nm. In N 2 ambient, manifest ZnO crystallites are formed and larger grain size than crystallites annealed in air can be distinguished evidently. At the temperature of 500 C, the grain size of crystallite annealed in air increases significantly. All SEM results are congruent with evidence of XRD. Fig. 4 exhibits the spectrum of ZnO thin films under different annealing temperatures and ambiences. The absorption edge of ZnO thin films can be observed sharper owing to the enhancement of ZnO crystal quality. The band gaps of ZnO under different conditions were investigated via the absorbance spectrum. No clear tendency is founded at 300 C~500 C under different ambiences. 100 ZnO-TGA Weight(%) % Temperature( o C) Fig. 1. Thermogravimetric analysis of zinc acetate dehydrate at the rate of 10 C/min.

3 Applied Mechanics and Materials Vols Air-300 Air-400 Intensity N N (002) (101) (100) (102) (110) (103) (112) N θ(degree) Fig. 2. XRD image of ZnO thin film grown on glass substrate at different annealing temperature and in different ambience. Fig. 3. SEM image of solution process ZnO thin films annealed in air at (a) 300 C. (b) 400 C. (c) 500 C., and annealed in N 2 at (d) 300 C. (e) 400 C. (f) 500 C. Absorbance(a.u.) N N N Air-300 Air-400 (αhν)2 (ev 2nm-2 ) Band gap Wavelength(nm) Fig. 4. Absorption spectra at different annealing temperature and in ambiences. The inset shows the plot of (αhν) 2 versus photon energy of ZnO thin film annealed at 500 C in air.

4 1588 Measurement Technology and its Application Conclusions This paper presents a simple and environmentally friendly method to fabricate solution process ZnO thin film. The ZnO thin films annealed in N 2 have more distinct diffraction peaks than that annealed in air no matter at the annealing temperature of 300 C, 400 C, and 500 C. The grain sizes grow larger with increasing annealing temperature. The grain size annealed in N2 ambient is larger than that in air. The absorption edge of ZnO thin films can be observed sharper owing to the enhancement of ZnO crystal quality. According to the absorbance spectrum, the band gaps of ZnO under different annealing conditions appear no clear difference. Acknowledgements This work was financially supported by the National Science Council of Taiwan under grant no. NSC E References [1] D.-T. Phan, G.-S. Chung, Fabrication and characteristics of a surface acoustic wave UV sensor based on ZnO thin films grown on a polycrystalline 3C-SiC buffer layer, Curr. Appl. Phys. 12 (2012) [2] H.-G. Li, G. Wu, H.-Z. Chen, Polymer/ZnO hybrid materials for near-uv sensors with wavelength selective response, Sensor. Actuat. B-Chem. 160 (2011) [3] N. Singh, et al, Synthesis of In2O3-ZnO core-shell nanowires and their application in gas sensing, Sensor. Actuat. B-Chem. 160 (2011) [4] K. Wetchakun, et al, Semiconducting metal oxides as sensors for environmentally hazardous gases, Sensor. Actuat. B-Chem. 160 (2011) [5] J. Chen, X. Yan, W. Liu, Q. Xue, The ethanol sensing property of magnetron sputtered ZnO thin films modified by Ag ion implantation, Sensor. Actuat. B-Chem. 160 (2011) [6] H.Q. Chiang, et al, High mobility transparent thin-film transistors with amorphous zinc tin oxide channel layer, Appl. Phys. Lett. 86 (2005) [7] S.-Y. Han, et al, Inkjet-printed high mobility transparent oxide semiconductors, J. Display Technol. 5 (2009) [8] J. Tellier, et al, Transparent amorphous and organics-free ZnO thin films produced by chemical solution deposition at 150 o, Thin Solid Films 518 (2010), [9] F. Fleischhaker, V. Wloka, I. Hennig, ZnO based field-effect transistors (FETs): solution-processable at low temperatures on flexible substrates, J. Mater. Chem. 20 (2010) [10] P. Tao, et al, Electroluminescence from ZnO nanowires homojunction LED grown on Si substrate by simple chemical vapor deposition, Chem. Phys. Lett. 522 (2012) [11] J. Chen, et al, Fabrication processing of ZnO-based LEDs, State-of-the-Art Program on Compound Semiconductors XLIV. 2 (2006) [12] Y. Ryu, et al, Next generation of oxide photonic devices: ZnO-based ultraviolet light emitting diodes, Appl. Phys. Lett. 88 (2006) [14] S.T. Meyers, et al, Aqueous inorganic inks for low-temperature fabrication of ZnO TFTs, J. Am. Chem. Soc. 130 (2008)

5 Measurement Technology and its Application / A Solution Processed ZnO Thin Film /

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