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In situ growth and characterization of Cu2ZnSnS4 thin films by reactive magnetron co-sputtering for solar cells

Zhang Kun Liu Fang-Yang Lai Yan-Qing Li Yi Yan Chang Zhang Zhi-An Li Jie Liu Ye-Xiang

In situ growth and characterization of Cu2ZnSnS4 thin films by reactive magnetron co-sputtering for solar cells

Zhang Kun, Liu Fang-Yang, Lai Yan-Qing, Li Yi, Yan Chang, Zhang Zhi-An, Li Jie, Liu Ye-Xiang
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  • Cu2ZnSnS4 (CZTS) thin films have been first in situ grown by reactive magnetron co-sputtering and its characterizations has been carried out by energy dispersive spectroscopy(EDS), X-ray diffraction(XRD), scan electron microscope(SEM), optical transmittance and electronic measurement. It was observed that the grown film shows homogeneous, compact surface morphology, and consists of large columnar grains throughout the thickness. The atom ratio Cu/(Zn+Sn) is about 1, while Zn/Sn is larger than 1 and decreases with the increase of substrate temperature. XRD analysis indicates that the grown film exhibits strong preferential orientation along (112) plane and the structural properties depend on growth temperature and Cu/(Zn+Sn) ratio. The in situ grown CZTS film has an optical absorption coefficient higher than 104 cm-1, and the optical band gap becomes narrow with the increase of substrate temperature and achieves (1.51±0.01)eV at 500℃. The conduction type of the CZTS films is p-type and the value of carrier concentration is comparable with values of device quality CIGS.
    • Funds:
    [1]

    Hnes K, Zscherpel E, Scragg J, Siebentritt S 2009 Physica B: Condensed Matter 404 4949

    [2]

    Katagiri H, Jimbo K, Maw W S, Oishi K, Yamazaki M, Araki H, Takeuchi A 2009 Thin Solid Films 517 2455

    [3]

    Steinhagen G, Panthani M G, Akhavan V, Goodfellow B, Koo B, Korgel B A 2009 J. Am. Chem. Soc. 131 12554

    [4]

    Seol G, Lee Y S, Lee J C, Nam H D, Ki H K 2003 Sol. Energy Mater. Sol. Cells 75 155

    [5]

    Goetzberger A, Hebling C, Schock H W 2003 Mater. Sci. Eng. R 40 1

    [6]

    Lai Y Q, Kuang S S, Liu F Y, Zhang Z A, Liu J, Li J, Liu Y X 2010 Acta Phys. Sin. 59 1198 (in Chinese) [赖延清、 匡三双、 刘芳洋、 张志安、 刘 军、 李 劼、 刘业翔 2010 物理学报 59 1198]

    [7]

    Ito K, Nakazawa T 1988 Jpn. J. Appl. Phys. 27 2094

    [8]

    Teodor K T, Kathleen B R, David B M 2010 Adv. Mater. 22 1

    [9]

    Weber A, Krauth H, Perlt S, Schubert B, Ktschau I, Schorr S, Schock H W 2009 Thin Solid Films 517 2524

    [10]

    Friedlmeier T M, Wieser N, Walter T, Dittrich H, Schock H W 1997 Proceedings of the 14th European PVSEC and Exhibition Barcelona, July 4—30, 1997 P4B. 10

    [11]

    Tanaka T, Kawasaki D, Nishio M, Guo Q, Ogawa H 2006 Phys. Status Solidi C 3 2844

    [12]

    Jimbo K, Kimura R, Kamimura T, Yamada S, Maw W, Araki H, Oishi K, Katagiri H 2007 Thin Solid Films 515 5997

    [13]

    Xie D T, Zhao K, Wang L F, Zhu F, Quan S W, Meng T J, Zhang B C, Chen J E 2002 Acta Phys. Sin. 51 1377 (in Chinese) [谢大弢、 赵 夔、 王莉芳、 朱 凤、 全胜文、 孟铁军、 张保澄、 陈佳洱 2002 物理学报 51 1377]

    [14]

    Kobayashi T, Jimbo K, Tsuchida K, Shinoda S, Oyanagi T, Katagiri H 2005 Jpn. J. Appl. Phys. 44 783

    [15]

    Sekiguchi K, Tanaka K, Moriya K, Uchiki H 2006 Phys. Status Solidi C 3 2618

    [16]

    Moriya K, Watabe J, Tanaka K, Uchiki H 2006 Phys. Status Solidi C 3 2848

    [17]

    Kumar Y B K, Babu G S, Bhaskar P U, Raja V S 2009 Sol. Energy Mater. Sol. Cells 93 1230

    [18]

    Tanaka K, Moritake N, Uchiki H 2007 Sol. Energy Mater. Sol. Cells 91 1199

    [19]

    Zhang X, Shi X Z, Ye W C, Ma C L, Wang C M 2009 Appl. Phys. A 94 381

    [20]

    Li A, Ao J P, He Q, Liu F F, Li F Y, Li C J, Sun Y 2007 Acta Phys. Sin. 56 5009 (in Chinese)[李 微、 敖建平、 何 青、 刘芳芳、 李凤岩、 李长健、 孙 云 2007 物理学报 56 5009]

    [21]

    Li W, Sun Y, Liu W, Li F Y, Zhou L 2006 Chin. Phys. 15 878

    [22]

    Liu X P, Shao L X 2007 Surf. Coat. Technol. 201 5340

    [23]

    Unold T, Sieber I, Ellmer K 2006 Appl. Phys. Lett. 88 213502

    [24]

    Katagiri H 2005 Thin Solid Films 480—481 426

    [25]

    Chen S Y, Gong X G, Walsh A, Wei S H 2009 Appl. Phys. Lett. 94 041903

    [26]

    Tanaka T, Nagatomo T, Kawasaki D, Nishio M, Guo Q, Wakahara A, Yoshida A, Ogawa H 2005 J. Phys. Chem. Solids 66 1978

    [27]

    Guo Q J, Hillhouse H W, Agrawal R 2009 J. An. Chem. Soc. 131 11672

    [28]

    Chen S Y, Gong X G, Walsh A, Wei S H 2009 Phys. Rev. B 79 165211

    [29]

    Paier J, Asahi R, Nagoya A, Kresse G 2009 Phys. Rev. B 79 115126

    [30]

    Guillén C, Herrero J 1994 J. Electrochem. Soc. 141 225

    [31]

    Jean F, Guillemoles O, Pierre C, Alain L, Kamel F, Frederic B, Jacques V, Daniel L 1996 J. Appl. Phys. 9 79

    [32]

    Nadenau V, Braunger D, Hariskos D, Kaiser M, Kble C, Oberacker A, Ruck M, Rühle U, Schffler R, Schmid D, Walter T, Zweigart S, Schock H W 1995 Prog. Photovolt. 3 363

    [33]

    Tuttle J R, Albin D S, Goral J P, Noufi R 1990 21th IEEE Photovoltaic Specialists Conference Kissimmee, May 21—25, 1990 p748

    [34]

    Ingrid R, Miguel A C, Brian E, Clay D, John S, Craig L P, Bobby T, Rommel N 2008 Prog. Photovolt: Res. Appl. 16 235

    [35]

    Pawar S M, Moholkar A V, Suryavanshi U B, Rajpure K Y, Bhosale C H 2007 Sol. Energy Mater. Sol. Cells 91 560

    [36]

    Stratieva N, Tzvetkova E, Ganchev M, Kochev K, Tomov I 1997 Sol. Energy Mater. Sol. Cells 45 87

    [37]

    Fiederling R, Keim R, Reuscher G, Ossau W, Schmidt G, Waag A, Molenkamp L W 1999 Nature 402 787

    [38]

    Rincón C, Hernández E, Wasim S M, Molina I 1998 Phys. Chem. Solids 59 1015

    [39]

    Müller J, Nowoczin J, Schmitt H 2006 Thin Solid Films 496 364

    [40]

    Lincot D, Meier H G, Kessler J, Vedel J, Dimmler B, Schock H W 1990 Sol. Energy Mater. 20 67

    [41]

    Guillen C, Herrero J, Lincot D 1994 J. Appl. Phys. 76 359

    [42]

    Scragg J J, Dale P J, Peter L M 2009 Thin Solid Films 517 2481

    [43]

    Zhang J, Shao L X 2009 Sci. China Ser. E 52 269

    [44]

    Katagiri H, Sasaguchi N, Hando S, Hoshino S, Ohashi J, Yokota T 1997 Sol. Energy Mater. Sol. Cells 49 407

    [45]

    Kumar Y B K, Babu G S, Bhaskar P U, Raja V S 2009 Phys. Status Solidi A 206 1525

    [46]

    Nakayama N, Ito K 1996 Appl. Surf. Sci. 92 171

  • [1]

    Hnes K, Zscherpel E, Scragg J, Siebentritt S 2009 Physica B: Condensed Matter 404 4949

    [2]

    Katagiri H, Jimbo K, Maw W S, Oishi K, Yamazaki M, Araki H, Takeuchi A 2009 Thin Solid Films 517 2455

    [3]

    Steinhagen G, Panthani M G, Akhavan V, Goodfellow B, Koo B, Korgel B A 2009 J. Am. Chem. Soc. 131 12554

    [4]

    Seol G, Lee Y S, Lee J C, Nam H D, Ki H K 2003 Sol. Energy Mater. Sol. Cells 75 155

    [5]

    Goetzberger A, Hebling C, Schock H W 2003 Mater. Sci. Eng. R 40 1

    [6]

    Lai Y Q, Kuang S S, Liu F Y, Zhang Z A, Liu J, Li J, Liu Y X 2010 Acta Phys. Sin. 59 1198 (in Chinese) [赖延清、 匡三双、 刘芳洋、 张志安、 刘 军、 李 劼、 刘业翔 2010 物理学报 59 1198]

    [7]

    Ito K, Nakazawa T 1988 Jpn. J. Appl. Phys. 27 2094

    [8]

    Teodor K T, Kathleen B R, David B M 2010 Adv. Mater. 22 1

    [9]

    Weber A, Krauth H, Perlt S, Schubert B, Ktschau I, Schorr S, Schock H W 2009 Thin Solid Films 517 2524

    [10]

    Friedlmeier T M, Wieser N, Walter T, Dittrich H, Schock H W 1997 Proceedings of the 14th European PVSEC and Exhibition Barcelona, July 4—30, 1997 P4B. 10

    [11]

    Tanaka T, Kawasaki D, Nishio M, Guo Q, Ogawa H 2006 Phys. Status Solidi C 3 2844

    [12]

    Jimbo K, Kimura R, Kamimura T, Yamada S, Maw W, Araki H, Oishi K, Katagiri H 2007 Thin Solid Films 515 5997

    [13]

    Xie D T, Zhao K, Wang L F, Zhu F, Quan S W, Meng T J, Zhang B C, Chen J E 2002 Acta Phys. Sin. 51 1377 (in Chinese) [谢大弢、 赵 夔、 王莉芳、 朱 凤、 全胜文、 孟铁军、 张保澄、 陈佳洱 2002 物理学报 51 1377]

    [14]

    Kobayashi T, Jimbo K, Tsuchida K, Shinoda S, Oyanagi T, Katagiri H 2005 Jpn. J. Appl. Phys. 44 783

    [15]

    Sekiguchi K, Tanaka K, Moriya K, Uchiki H 2006 Phys. Status Solidi C 3 2618

    [16]

    Moriya K, Watabe J, Tanaka K, Uchiki H 2006 Phys. Status Solidi C 3 2848

    [17]

    Kumar Y B K, Babu G S, Bhaskar P U, Raja V S 2009 Sol. Energy Mater. Sol. Cells 93 1230

    [18]

    Tanaka K, Moritake N, Uchiki H 2007 Sol. Energy Mater. Sol. Cells 91 1199

    [19]

    Zhang X, Shi X Z, Ye W C, Ma C L, Wang C M 2009 Appl. Phys. A 94 381

    [20]

    Li A, Ao J P, He Q, Liu F F, Li F Y, Li C J, Sun Y 2007 Acta Phys. Sin. 56 5009 (in Chinese)[李 微、 敖建平、 何 青、 刘芳芳、 李凤岩、 李长健、 孙 云 2007 物理学报 56 5009]

    [21]

    Li W, Sun Y, Liu W, Li F Y, Zhou L 2006 Chin. Phys. 15 878

    [22]

    Liu X P, Shao L X 2007 Surf. Coat. Technol. 201 5340

    [23]

    Unold T, Sieber I, Ellmer K 2006 Appl. Phys. Lett. 88 213502

    [24]

    Katagiri H 2005 Thin Solid Films 480—481 426

    [25]

    Chen S Y, Gong X G, Walsh A, Wei S H 2009 Appl. Phys. Lett. 94 041903

    [26]

    Tanaka T, Nagatomo T, Kawasaki D, Nishio M, Guo Q, Wakahara A, Yoshida A, Ogawa H 2005 J. Phys. Chem. Solids 66 1978

    [27]

    Guo Q J, Hillhouse H W, Agrawal R 2009 J. An. Chem. Soc. 131 11672

    [28]

    Chen S Y, Gong X G, Walsh A, Wei S H 2009 Phys. Rev. B 79 165211

    [29]

    Paier J, Asahi R, Nagoya A, Kresse G 2009 Phys. Rev. B 79 115126

    [30]

    Guillén C, Herrero J 1994 J. Electrochem. Soc. 141 225

    [31]

    Jean F, Guillemoles O, Pierre C, Alain L, Kamel F, Frederic B, Jacques V, Daniel L 1996 J. Appl. Phys. 9 79

    [32]

    Nadenau V, Braunger D, Hariskos D, Kaiser M, Kble C, Oberacker A, Ruck M, Rühle U, Schffler R, Schmid D, Walter T, Zweigart S, Schock H W 1995 Prog. Photovolt. 3 363

    [33]

    Tuttle J R, Albin D S, Goral J P, Noufi R 1990 21th IEEE Photovoltaic Specialists Conference Kissimmee, May 21—25, 1990 p748

    [34]

    Ingrid R, Miguel A C, Brian E, Clay D, John S, Craig L P, Bobby T, Rommel N 2008 Prog. Photovolt: Res. Appl. 16 235

    [35]

    Pawar S M, Moholkar A V, Suryavanshi U B, Rajpure K Y, Bhosale C H 2007 Sol. Energy Mater. Sol. Cells 91 560

    [36]

    Stratieva N, Tzvetkova E, Ganchev M, Kochev K, Tomov I 1997 Sol. Energy Mater. Sol. Cells 45 87

    [37]

    Fiederling R, Keim R, Reuscher G, Ossau W, Schmidt G, Waag A, Molenkamp L W 1999 Nature 402 787

    [38]

    Rincón C, Hernández E, Wasim S M, Molina I 1998 Phys. Chem. Solids 59 1015

    [39]

    Müller J, Nowoczin J, Schmitt H 2006 Thin Solid Films 496 364

    [40]

    Lincot D, Meier H G, Kessler J, Vedel J, Dimmler B, Schock H W 1990 Sol. Energy Mater. 20 67

    [41]

    Guillen C, Herrero J, Lincot D 1994 J. Appl. Phys. 76 359

    [42]

    Scragg J J, Dale P J, Peter L M 2009 Thin Solid Films 517 2481

    [43]

    Zhang J, Shao L X 2009 Sci. China Ser. E 52 269

    [44]

    Katagiri H, Sasaguchi N, Hando S, Hoshino S, Ohashi J, Yokota T 1997 Sol. Energy Mater. Sol. Cells 49 407

    [45]

    Kumar Y B K, Babu G S, Bhaskar P U, Raja V S 2009 Phys. Status Solidi A 206 1525

    [46]

    Nakayama N, Ito K 1996 Appl. Surf. Sci. 92 171

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  • Received Date:  22 April 2010
  • Accepted Date:  05 May 2010
  • Published Online:  05 January 2011

In situ growth and characterization of Cu2ZnSnS4 thin films by reactive magnetron co-sputtering for solar cells

  • 1. School of Metallurgical Science and Engineering, Central South University, Changsha 410083, China

Abstract: Cu2ZnSnS4 (CZTS) thin films have been first in situ grown by reactive magnetron co-sputtering and its characterizations has been carried out by energy dispersive spectroscopy(EDS), X-ray diffraction(XRD), scan electron microscope(SEM), optical transmittance and electronic measurement. It was observed that the grown film shows homogeneous, compact surface morphology, and consists of large columnar grains throughout the thickness. The atom ratio Cu/(Zn+Sn) is about 1, while Zn/Sn is larger than 1 and decreases with the increase of substrate temperature. XRD analysis indicates that the grown film exhibits strong preferential orientation along (112) plane and the structural properties depend on growth temperature and Cu/(Zn+Sn) ratio. The in situ grown CZTS film has an optical absorption coefficient higher than 104 cm-1, and the optical band gap becomes narrow with the increase of substrate temperature and achieves (1.51±0.01)eV at 500℃. The conduction type of the CZTS films is p-type and the value of carrier concentration is comparable with values of device quality CIGS.

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