Insight of the doping mechanism of F and Al co-doped ZnO transparent conductive films

Wang Yan-Feng; Xie Xi-Cheng; Liu Xiao-Jie; Han Bing; Wu Han-Han; Lian Ning-Ning; Yang Fu; Song Qing-Gong; Pei Hai-Lin; Li Jun-Jie

doi:10.7498/aps.69.20200580

Abstract

Transparent conductive oxide (TCO) films, as transparent electrodes, are widely used in thin-film solar cells. The performance of TCO film has a significant influence on the conversion efficiency of the film solar cell fabricated byusing it. Although the conductivity can be improved by increasing the carrier concentration, the transmittance in the long wave will be sacrificed. Therefore, the only feasible method is to increase the carrier mobility within a certain carrier concentration range, rather than increase the mobility by reducing carrier concentration. In this paper, the F and Al co-doped ZnO (FAZO) films are deposited on glass substrates (Corning XG) by an RF magnetron sputtering technique with using a small amount of ZnF₂ (1 wt.%) and Al₂O₃ (1 wt.%) dopant. The influences of sputtering pressure on the structure, morphology and photoelectric characteristics of the films are respectively investigated by X-ray diffraction analysis, scanning electron microscope, Hall effect measurement, and ultraviolet–visible–near infrared spectrophotometry. All the thin films show typical wurtzite structure with the c axis preferentially oriented perpendicular to the substrate. With the increase of sputtering pressure, the deposition rate of FAZO film decreases, the crystallization quality is deteriorated, surface topography changes gradually from “crater-like” to co-existent “crater-like” and “granular-like”, and the surface roughness increases. The FAZO film deposited at 0.5 Pa presents the optimal performance with a mobility of 40.03 cm²/V·s, carrier concentration of 3.92 × 10²⁰ cm^–3, resistivity of 3.98 × 10^–4 Ω·cm, and about 90% average transmittance in a range of 380－1200 nm. The theoretical result shows that the co-doping of F and Al takes the advantages of single F and Al doped ZnO films, and overcomes the shortcoming of metal elements doping, which donates the carriers just from doped metal elements. Furthermore, the co-doping of F and Al not only increases the carriers but also reduces the scatterings caused by the inter-orbital interaction of doped atoms. The doped F 2p electron orbitals repel the O 2p and Zn 4s electron orbitals, making them move down and donate electrons. At the same time, the orbitals of Al 3s and Al 3p also make a contribution to the conductivity. After co-doping of F and Al, both the carrier concentration and conductivity increase significantly.

Keywords:

Authors and contacts

1.
Institute of New Energy Science and Technology, College of Science, Hebei North University, Zhangjiakou 075000, China
2.
College of Science, Civil Aviation University of China, Tianjin 300300, China
3.
General Courses Department, Army Military Transportation University, Tianjin 300161, China

Corresponding author: Li Jun-Jie, ljj888999@hebeinu.edu.cn

Funds: Project Supported by the Natural Science Foundation of Hebei Province, China (Grant No. A2019405059), the Key Research and Development Program of Hebei Province, China (Grant No. 19214301D), the Fundamental Research Fund of Hebei North University, China (Grant No. JYT2019001), the General Projects of Hebei North University, China (Grant No. YB2018014), and the Innovation and Entrepreneurship Training Program for College Students of Hebei North University, China (Grant No. 201910092010)

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References

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Cited By

图 1 不同溅射气压制备FAZO薄膜的沉积速率

Figure 1. The deposition rate of FAZO films deposited at different pressures.

DownLoad: Full-Size Img PowerPoint

图 2 不同溅射气压制备FAZO薄膜的XRD衍射谱　(a) XRD 衍射谱; (b)半高宽(FWHM)和晶粒尺寸(D)

Figure 2. XRD patterns of FAZO films deposited at different pressures: (a) XRD patterns; (b) full width at half maximum (FWHM) and grain size (D).

DownLoad: Full-Size Img PowerPoint

图 3 不同溅射气压制备FAZO薄膜的表面形貌图　(a) 0.3 Pa; (b) 0.8 Pa; (c) 3.0 Pa

Figure 3. SEM images of FAZO films deposited at different pressures: (a) 0.3 Pa; (b) 0.8 Pa; (c) 3.0 Pa.

DownLoad: Full-Size Img PowerPoint

图 4 不同溅射气压制备FAZO薄膜的电学特性

Figure 4. Electrical properties of FAZO films deposited at different pressures.

DownLoad: Full-Size Img PowerPoint

图 5 FZO, AZO和FAZO能带结构图　(a) FZO; (b) AZO; (c) FAZO

Figure 5. Band structure of FZO, AZO and FAZO: (a) FZO; (b) AZO; (c) FAZO.

DownLoad: Full-Size Img PowerPoint

图 6 FZO, AZO和FAZO态密度图　(a) FZO; (b) AZO; (c) FAZO

Figure 6. Density of states of FZO, AZO and FAZO: (a) FZO; (b) AZO; (c) FAZO.

DownLoad: Full-Size Img PowerPoint

图 7 不同溅射气压制备FAZO薄膜以及AZO薄膜的光学特性　(a)透过谱; (b)反射谱; (c)吸收谱

Figure 7. Optical properties of FAZO films deposited at different pressures and AZO film: (a) Transmittance; (b) reflection; (c) absorption.

DownLoad: Full-Size Img PowerPoint

图 8 不同溅射气压制备FAZO薄膜和AZO薄膜的光学带隙

Figure 8. Optical bandgap of FAZO films deposited at different pressures and AZO film.

DownLoad: Full-Size Img PowerPoint

map

[1]	Gordon R G 2000 MRS Bull. 25 52
[2]	Minami T 2000 MRS Bull. 25 38
[3]	Moulin E, Bittkau K, Ghosh M, Bugnon G, Stuckelberger M, Meier M, Haug F J, Hüpkes J, Ballif C 2016 Sol. Energy Mater. Sol. Cells 145 185 Google Scholar
[4]	Jost G, Merdzhanova T, Zimmermann T, Hüpkes J 2013 Thin Solid Films 532 66 Google Scholar
[5]	Tao K, Sun Y, Cai H K, Zhang D X, Xie K, Wang Y 2012 Appl. Surf. Sci. 258 5943 Google Scholar
[6]	Warasawa M, Kaijo A, Sugiyama M 2012 Thin Solid Films 520 2119 Google Scholar
[7]	Wang Y F, Song J M, Bai L S, Yang F, Han B, Guo Y J, Dai B T, Zhao Y, Zhang X D 2018 Sol. Energy Mater. Sol. Cells 179 401 Google Scholar
[8]	Liu B F, Bai L S, Li T T, Wei C C, Li B Z, Huang Q, Zhang D K, Wang G C, Zhao Y, Zhang X D 2017 Energy Environ. Sci. 10 1134 Google Scholar
[9]	Zhang L, Huang J, Yang J, Tang K, Ren B, Zhang S W, Wang L J 2016 Surf. Coat. Technol. 307 1129 Google Scholar
[10]	Tsay C Y, Pai K C 2018 Thin Solid Films 654 11 Google Scholar
[11]	Kirby S D, van Dover R B 2009 Thin Solid Films 517 1958 Google Scholar
[12]	Li Q, Zhu L P, Li Y G, Zhang X Y, Niu W Z, Guo Y M, Ye Z Z 2017 J. Alloys Compd. 697 156 Google Scholar
[13]	Mallick A, Basak D 2017 Appl. Surf. Sci. 410 540 Google Scholar
[14]	Shi Q, Zhou K S, Dai M J, Lin S S, Hou H J, Wei C B, Hu F 2014 Ceram. Int. 40 211 Google Scholar
[15]	Ji X Z, Song J M, Wu T T, Tian Y, Han B, Liu X N, Wang H W, Gui Y B, Ding Y, Wang Y F 2019 Sol. Energy Mater. Sol. Cells 190 6 Google Scholar
[16]	Wang Y F, Song J M, Song W Y, Tian Y, Han B, Meng X D, Yang F, Ding Y, Li J J 2019 Sol. Energy 186 126 Google Scholar
[17]	Zheng G X, Song J M, Zhang J, Li J J, Han B, Meng X D, Yang F, Zhao Y, Wang Y F 2020 Mater. Sci. Semicond. Process. 112 105016 Google Scholar
[18]	王延峰, 黄茜, 宋庆功, 刘阳, 魏长春, 赵颖, 张晓丹 2012 61 137801 Google Scholar Wang Y F, Huang Q, Song Q G, Liu Y, Wei C C, Zhao Y, Zhang X D 2012 Acta Phys. Sin. 61 137801 Google Scholar
[19]	王延峰, 张晓丹, 黄茜, 杨富, 孟旭东, 宋庆功, 赵颖 2013 62 247802 Google Scholar Wang Y F, Zhang X D, Huang Q, Yang F, Meng X D, Song Q G, Zhao Y 2013 Acta Phys. Sin. 62 247802 Google Scholar
[20]	Segall M D, Lindan P J D, Probert M J, Pickard C J, Hasnip P J, Clark S J, Payne M C 2002 J. Phys. Condens. Matter 14 2717 Google Scholar
[21]	Perdew J P, Burke K, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865 Google Scholar
[22]	Vanderbilt D 1990 Phys. Rev. B 41 7892 Google Scholar
[23]	Sheetz R M, Ponomareva I, Richter E, Andriotis A N, Menon M 2009 Phys. Rev. B 80 195314 Google Scholar
[24]	王延峰, 孟旭东, 郑伟, 宋庆功, 翟昌鑫, 郭兵, 张越, 杨富, 南景宇 2016 65 087802 Google Scholar Wang Y F, Meng X D, Zheng W, Song Q G, Zhai C X, Guo B, Zhang Y, Yang F, Nan J Y 2016 Acta Phys. Sin. 65 087802 Google Scholar
[25]	Hsu F H, Wang N F, Tsai Y Z, Chuang M C, Cheng Y S, Houng M P 2013 Appl. Surf. Sci. 280 104 Google Scholar
[26]	Yue H, Wu A, Feng Y, Zhang X, Li T 2011 Thin Solid Films 519 5577 Google Scholar
[27]	Kluth O, Schöpe G, Hüpkes J, Agashe C, Müller J, Rech B 2003 Thin Solid Films 442 80 Google Scholar
[28]	Assunção V, Fortunato E, Marques A, Águas H, Ferreira I, Costa M E V, Martins R 2003 Thin Solid Films 427 401 Google Scholar
[29]	Maccoa B, Knoops H C M, Verheijen M A, Beyer W, Creatore M, Kessels W M M 2017 Sol. Energy Mater. Sol. Cells 173 111 Google Scholar
[30]	Pei Z L, Sun C, Tan M H, Xiao J Q, Guan D H, Huang R F, Wen L S 2001 J. Appl. Phys. 90 3432 Google Scholar
[31]	Sreedhar A, Kwon J H, Yi J, Gwag J S 2016 Ceram. Int. 42 14456 Google Scholar
[32]	Cao L, Zhu LvP, Jiang J, Zhao R, Ye Z Z, Zhao B H 2011 Sol. Energy Mater. Sol. Cells 95 894 Google Scholar
[33]	Xu H Y, Liu Y C, Mu R, Shao C L, Lu Y M, Shen D Z, Fan X W 2005 Appl. Phys. Lett. 86 123107
[34]	Burstein E 1954 Phys. Rev. 93 632 Google Scholar
[35]	Moss T S 1954 Proc. Phys. Soc. London, Sect. B 67 775 Google Scholar
[36]	Slassi A 2015 Opt. Quantum Electron. 47 2465 Google Scholar
[37]	张富春, 张志勇, 张威虎, 阎军峰, 贠江妮 2009 光学学报 29 2015 Zhang F C, Zhang Z Y, Zhang W H, Yan J F, Yun J N 2009 Acta Opt. Sin. 29 2015
[38]	Wang Y F, Zhang X D, Meng X D, Cao Y, Yang F, Nan J Y, Song Q G, Huang Q, Wei C C, Zhang J J, Zhao Y 2016 Sol. Energy Mater. Sol. Cells 145 171 Google Scholar

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