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通过直流反应磁控溅射技术,原位生长制备了太阳电池用Cu2ZnSnS4(CZTS)薄膜.采用X射线能量色散谱仪、扫描电镜、X射线衍射仪、紫外可见分光光度计和霍尔效应测试系统对薄膜进行了表征.结果表明,原位生长的CZTS薄膜具有均质、致密和平整的形貌,且由贯穿整个薄膜厚度的柱状颗粒组成.不同基底温度下生长所得薄膜的Cu/(Zn+Sn) 值均约为1,而Zn/Sn值均大于1且随着基底温度升高而减小.所得薄膜在(112)方向上择优取向明显,且结构特征受基底温度和Cu/(Zn+Sn)的共同影响.所得薄膜均具有高达104cm-1的光吸收系数,其带隙宽度随着生长温度的增加而降低,并且在500℃时为(1.51±0.01)eV.薄膜的导电类型均为p型,且具有与器件级Cu(In,Ga)Se2(CIGS)相当的载流子浓度.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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Keywords:
- Cu2ZnSnS4 /
- reactive magnetron co-sputtering /
- in situ growth /
- solar cell
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[4] Seol G, Lee Y S, Lee J C, Nam H D, Ki H K 2003 Sol. Energy Mater. Sol. Cells 75 155
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[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
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[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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[1] Hnes 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 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, Ktschau 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 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 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, Kble C, Oberacker A, Ruck M, Rühle U, Schffler 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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