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Room temperature deposition of highly conductive and transparent H and W co-doped ZnO film

Wang Yan-Feng Zhang Xiao-Dan Huang Qian Liu Yang Wei Chang-Chun Zhao Ying

Room temperature deposition of highly conductive and transparent H and W co-doped ZnO film

Wang Yan-Feng, Zhang Xiao-Dan, Huang Qian, Liu Yang, Wei Chang-Chun, Zhao Ying
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  • Highly conductive and transparent hydrogen and tungsten co-doped zinc oxide (HWZO) thin films are prepared at room temperature by pulsed DC magnetron sputtering using a WZO (98.5 wt.% ZnO, 1.5 wt.% WO3) ceramic target with different H2 flow rates. The influence of H2 flow rate on the structural, compositional, elemental valence state as well as electrical and optical properties are systematically investigated. The results indicate that the incorporation of H does not change the structure of tungsten doped zinc oxide (WZO) namely, both WZO and HWZO films are polycrystalline with hexagonal structure and a preferred orientation along c-axis, respectively whereas the crystallinity is firstly improved and then deteriorated with the increase of H2 flow rate. Furthermore, the reaction between Zn and O can be promoted by the incorporated H. With an optimal H2 flow rate, the carrier concentration increases from 3.32×1020 cm-3 for WZO film to 5.44×1020 cm-3 for HWZO film, and the resistivity decreases from 1.20×10-3 Ω·cm to 7.71×10-4 Ω·cm. The average transmittance in a range of 400-1100 nm is improved from 69.2% to 82.4 %, and the optical band gap is widened from 3.42 eV to 3.58 eV.
    • Funds: Project supported by the National Basic Research Program of China (Grant Nos. 2011CBA00706, 2011CBA00707), National Natural Science Foundation of China (Grant No. 60976051), Program for New Century Excellent Talents in University of China (Grant No. NCET-08-0295), Ministry of Education Key Laboratory of Topics (Grant No. 2011KFKT06) and the Fundamental Research Funds for the Central Universities, China (Grant No. 65011981).
    [1]

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    [2]

    Yan B J, Yue G Z, Sivec L, Yang J, Guha S, Jiang C S 2011 Appl. Phys. Lett. 99 113512

    [3]

    Zhang X D, Zheng X X, Wang G H, Xu S Z, Yue Q, Lin Q, Wei C C, Sun J, Zhang D K, Xiong S Z, Geng X H, Zhao Y 2010 Acta Phys. Sin. 59 8231 (in Chinese) [张晓丹, 郑新霞, 王光红, 许盛之, 岳强, 林泉, 魏长春, 孙建, 张德坤, 熊绍珍, 耿新华, 赵颖2010 物理学报 59 8231]

    [4]

    Zheng X X, Zhang X D, Yang S S, Wang G H, Xu S Z, Wei C C, Sun J, Geng X H, Xiong S Z, Zhao Y 2011 Acta Phys. Sin. 60 068801 (in Chinese) [郑新霞, 张晓丹, 杨素素, 王光红, 许盛之, 魏长春, 孙建, 耿新华, 熊绍珍, 赵颖2011 物理学报 60 068801]

    [5]

    Wang Y F, Zhang X D, Bai L S, Huang Q, Wei C C, Zhao Y 2012 Appl. Phys. Lett. 100 263508

    [6]

    Selvan J A A, Delahoy A E, Guo S Y, Li Y M 2006 Sol. Energy Mater. Sol. Cells 90 3371

    [7]

    Agashe C, Kluth O, Schöpe G, Siekmann H, Hrgen J, Rech B 2003 Thin Solid Films 442 167

    [8]

    Meng Y, Yang X L, Chen H X, Shen J, Jiang Y M, Zhang Z J, Hua Z Y 2001 Thin Solid Films 394 219

    [9]

    Wang Y F, Huang Q, Song Q G, Liu Y, Wei C C, Zhao Y, Zhang X D 2012 Acta Phys. Sin. 61 137801 (in Chinese) [王延峰, 黄茜, 宋庆功, 刘阳, 魏长春, 赵颖, 张晓丹2012 物理学报 61 137801]

    [10]

    Li X F, Zhang Q, Miao W N, Huang L, Zhang Z J, Hua Z Y 2006 J. Vac. Sci. Technol. A 24 1866

    [11]

    Wang Y F, Huang Q, Wei C C, Zhang D K, Zhao Y, Zhang X D 2012 Appl. Surf. Sci. 258 8797

    [12]

    Oh B Y, Jeong M C, Lee W, Myoung J M 2004 J. Crystal Growth 274 453

    [13]

    Lee J, Lee D, Lim D, Yang K 2007 Thin Solid Films 515 6094

    [14]

    Oliveira C, Rebouta L, Lacerda-Arôso T D, Lanceros-Mendez S, Viseu T, Tavares C J, Tovar J, Ferdov S, Alves E 2009 Thin Solid Films 517 6290

    [15]

    Wang Y P, Lu J G, Bie X, Gong L, Li X, Song D, Zhao X Y, Ye W Y, Ye Z Z 2011 J. Vac. Sci. Technol. A 29 031505

    [16]

    van de Walle C G, Neugebauer J 2003 Nature 423 626

    [17]

    van de Walle C G 2000 Phys. Rev. Lett. 85 1012

    [18]

    Lee S H, Lee T S, Lee K S, Cheong B, Kim Y D, Kim W M 2008 J. Phys. D: Appl. Phys. 41 095303

    [19]

    Chen L Y, Chen W H, Wang J J, Hong F C N, Su Y K 2004 Appl. Phys. Lett. 85 5628

    [20]

    Liu W F, Du G T, Sun Y F, Bian J M, Cheng Y, Yang T P, Chang Y C, Xu Y B 2007 Appl. Surf. Sci. 253 2999

    [21]

    Ellmer K 2001 J. Phys. D: Appl. Phys. 34 3097

    [22]

    Strohmeier B R, Hercules D M 1984 J. Catal. 86 266

    [23]

    Chen M, Wang X, Yu Y H, Pei Z L, Bai X D, Sun C, Huang R F, Wen L S 2000 Appl. Surf. Sci. 158 134

    [24]

    Nefedov V I, Gati D, Dzhurinskii B F, Sergushin N P, Salyn Y V 1975 Zh. Neorg. Khimii 20 2307

    [25]

    Ng K T, Hercules D M 1976 J. Phys. Chem. 80 2095

    [26]

    Sarkar A, Ghosh S, Chaudhuri S, Pal A K 1991 Thin Solid Films 204 255

    [27]

    Swanepoel R 1983 J. Phys. E: Sci. Instrum. 16 1214

  • [1]

    Meier J, Vallat-Sauvain E, Dubail S, Kroll U, Dubail J, Golay S, Feitknecht L, Torres P, Faÿ S, Fischer D, Shah A 2001 Sol. Energy Mater. Sol. Cells 66 73

    [2]

    Yan B J, Yue G Z, Sivec L, Yang J, Guha S, Jiang C S 2011 Appl. Phys. Lett. 99 113512

    [3]

    Zhang X D, Zheng X X, Wang G H, Xu S Z, Yue Q, Lin Q, Wei C C, Sun J, Zhang D K, Xiong S Z, Geng X H, Zhao Y 2010 Acta Phys. Sin. 59 8231 (in Chinese) [张晓丹, 郑新霞, 王光红, 许盛之, 岳强, 林泉, 魏长春, 孙建, 张德坤, 熊绍珍, 耿新华, 赵颖2010 物理学报 59 8231]

    [4]

    Zheng X X, Zhang X D, Yang S S, Wang G H, Xu S Z, Wei C C, Sun J, Geng X H, Xiong S Z, Zhao Y 2011 Acta Phys. Sin. 60 068801 (in Chinese) [郑新霞, 张晓丹, 杨素素, 王光红, 许盛之, 魏长春, 孙建, 耿新华, 熊绍珍, 赵颖2011 物理学报 60 068801]

    [5]

    Wang Y F, Zhang X D, Bai L S, Huang Q, Wei C C, Zhao Y 2012 Appl. Phys. Lett. 100 263508

    [6]

    Selvan J A A, Delahoy A E, Guo S Y, Li Y M 2006 Sol. Energy Mater. Sol. Cells 90 3371

    [7]

    Agashe C, Kluth O, Schöpe G, Siekmann H, Hrgen J, Rech B 2003 Thin Solid Films 442 167

    [8]

    Meng Y, Yang X L, Chen H X, Shen J, Jiang Y M, Zhang Z J, Hua Z Y 2001 Thin Solid Films 394 219

    [9]

    Wang Y F, Huang Q, Song Q G, Liu Y, Wei C C, Zhao Y, Zhang X D 2012 Acta Phys. Sin. 61 137801 (in Chinese) [王延峰, 黄茜, 宋庆功, 刘阳, 魏长春, 赵颖, 张晓丹2012 物理学报 61 137801]

    [10]

    Li X F, Zhang Q, Miao W N, Huang L, Zhang Z J, Hua Z Y 2006 J. Vac. Sci. Technol. A 24 1866

    [11]

    Wang Y F, Huang Q, Wei C C, Zhang D K, Zhao Y, Zhang X D 2012 Appl. Surf. Sci. 258 8797

    [12]

    Oh B Y, Jeong M C, Lee W, Myoung J M 2004 J. Crystal Growth 274 453

    [13]

    Lee J, Lee D, Lim D, Yang K 2007 Thin Solid Films 515 6094

    [14]

    Oliveira C, Rebouta L, Lacerda-Arôso T D, Lanceros-Mendez S, Viseu T, Tavares C J, Tovar J, Ferdov S, Alves E 2009 Thin Solid Films 517 6290

    [15]

    Wang Y P, Lu J G, Bie X, Gong L, Li X, Song D, Zhao X Y, Ye W Y, Ye Z Z 2011 J. Vac. Sci. Technol. A 29 031505

    [16]

    van de Walle C G, Neugebauer J 2003 Nature 423 626

    [17]

    van de Walle C G 2000 Phys. Rev. Lett. 85 1012

    [18]

    Lee S H, Lee T S, Lee K S, Cheong B, Kim Y D, Kim W M 2008 J. Phys. D: Appl. Phys. 41 095303

    [19]

    Chen L Y, Chen W H, Wang J J, Hong F C N, Su Y K 2004 Appl. Phys. Lett. 85 5628

    [20]

    Liu W F, Du G T, Sun Y F, Bian J M, Cheng Y, Yang T P, Chang Y C, Xu Y B 2007 Appl. Surf. Sci. 253 2999

    [21]

    Ellmer K 2001 J. Phys. D: Appl. Phys. 34 3097

    [22]

    Strohmeier B R, Hercules D M 1984 J. Catal. 86 266

    [23]

    Chen M, Wang X, Yu Y H, Pei Z L, Bai X D, Sun C, Huang R F, Wen L S 2000 Appl. Surf. Sci. 158 134

    [24]

    Nefedov V I, Gati D, Dzhurinskii B F, Sergushin N P, Salyn Y V 1975 Zh. Neorg. Khimii 20 2307

    [25]

    Ng K T, Hercules D M 1976 J. Phys. Chem. 80 2095

    [26]

    Sarkar A, Ghosh S, Chaudhuri S, Pal A K 1991 Thin Solid Films 204 255

    [27]

    Swanepoel R 1983 J. Phys. E: Sci. Instrum. 16 1214

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  • Received Date:  12 July 2012
  • Accepted Date:  08 August 2012
  • Published Online:  05 January 2013

Room temperature deposition of highly conductive and transparent H and W co-doped ZnO film

  • 1. Institute of Photo-Electronic Thin Film Devices and Technology of Nankai University, Key Laboratory of Photo-Electronic Thin Film Devices and Technology of Tianjin, Key Laboratory of Opto-Electronic Information Science and Technology, Ministry of Education, Tianjin 300071, China
Fund Project:  Project supported by the National Basic Research Program of China (Grant Nos. 2011CBA00706, 2011CBA00707), National Natural Science Foundation of China (Grant No. 60976051), Program for New Century Excellent Talents in University of China (Grant No. NCET-08-0295), Ministry of Education Key Laboratory of Topics (Grant No. 2011KFKT06) and the Fundamental Research Funds for the Central Universities, China (Grant No. 65011981).

Abstract: Highly conductive and transparent hydrogen and tungsten co-doped zinc oxide (HWZO) thin films are prepared at room temperature by pulsed DC magnetron sputtering using a WZO (98.5 wt.% ZnO, 1.5 wt.% WO3) ceramic target with different H2 flow rates. The influence of H2 flow rate on the structural, compositional, elemental valence state as well as electrical and optical properties are systematically investigated. The results indicate that the incorporation of H does not change the structure of tungsten doped zinc oxide (WZO) namely, both WZO and HWZO films are polycrystalline with hexagonal structure and a preferred orientation along c-axis, respectively whereas the crystallinity is firstly improved and then deteriorated with the increase of H2 flow rate. Furthermore, the reaction between Zn and O can be promoted by the incorporated H. With an optimal H2 flow rate, the carrier concentration increases from 3.32×1020 cm-3 for WZO film to 5.44×1020 cm-3 for HWZO film, and the resistivity decreases from 1.20×10-3 Ω·cm to 7.71×10-4 Ω·cm. The average transmittance in a range of 400-1100 nm is improved from 69.2% to 82.4 %, and the optical band gap is widened from 3.42 eV to 3.58 eV.

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