电子束蒸镀法制备CuIn_(0.7)Ga_(0.3)Se_2薄膜太阳电池的性能
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摘要
封装石英管真空熔炼合成CuIn_(0.7)Ga_(0.3)Se_2(CIGS)块体,再采用电子束蒸镀此块体,制备用于太阳电池吸收层的CIGS薄膜,然后对薄膜进行不同温度的真空退火处理。分别采用XRD、EDS、SEM及光谱分析等方法,研究CIGS块体和退火薄膜的表面形貌、晶体结构、成分或者光电性能。结果表明:在1200℃、保温2 h后,采用真空熔炼获得结晶性能较好、单一黄铜矿结构的CuIn_(0.7)Ga_(0.3)Se_2块体。随着退火温度的升高,薄膜中In-Se杂质相分解,从而获得单一相的CIGS薄膜;并且颗粒不断长大,达到1.0~3.5μm;成分和光学禁带不断得到优化。600℃退火薄膜是比较符合理想太阳电池要求的吸收层材料。
The CuIn_(0.7)Ga_(0.3)Se_2(CIGS) thin films used as absorber layers of solar cell were deposited by electron-beam evaporation utilizing CIGS bulk synthesized by quartz-tube vacuum smelting,followed by annealing treatment in vacuum atmosphere at different temperatures.The performances of CIGS bulk and annealed films on the surface morphology,compositions,crystal microstructure and photoelectric property were studied by X-ray diffractometry(XRD),scanning electron microscopy(SEM),energy dispersive spectrometry(EDS) or spectroscopic analysis,respectively.The results show that ideal CuIn_(0.7)Ga_(0.3)Se_2 bulk with good crystallization property and single chalcopyrite structure is obtained by vacuum smelting at 1200 ℃for 120 min.With the increase of annealing temperature,single phase CIGS presents,accompanying by decomposition of In-Se impurity phase.Meanwhile,the grain size continuously grows up to 1.0-3.5μm,and the composition and optical band gap are gradually optimized.Therefore,the as-annealed film at 600 ℃ is in much more consistent with the absorber layers material of ideal solar cell.
The CuIn_(0.7)Ga_(0.3)Se_2(CIGS) thin films used as absorber layers of solar cell were deposited by electron-beam evaporation utilizing CIGS bulk synthesized by quartz-tube vacuum smelting,followed by annealing treatment in vacuum atmosphere at different temperatures.The performances of CIGS bulk and annealed films on the surface morphology,compositions,crystal microstructure and photoelectric property were studied by X-ray diffractometry(XRD),scanning electron microscopy(SEM),energy dispersive spectrometry(EDS) or spectroscopic analysis,respectively.The results show that ideal CuIn_(0.7)Ga_(0.3)Se_2 bulk with good crystallization property and single chalcopyrite structure is obtained by vacuum smelting at 1200 ℃for 120 min.With the increase of annealing temperature,single phase CIGS presents,accompanying by decomposition of In-Se impurity phase.Meanwhile,the grain size continuously grows up to 1.0-3.5μm,and the composition and optical band gap are gradually optimized.Therefore,the as-annealed film at 600 ℃ is in much more consistent with the absorber layers material of ideal solar cell.
引文
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[13]ZHANG Li,XUE Yu-ming,XU Chuan-ming,HE Qing,LIU Fang-fang,LI Chang-jian,SUN Yun.Microstructural characterization of Cu-poor Cu(In,Ga)Se2 surface layer[J].Thin Solid Films,2012,520:2873-2877.
[14]LIU Jiang,ZHUANG Da-ming,LUAN He-xin,CAO Ming-jie,XIE Min,LI Xiao-long.Preparation of Cu(In,Ga)Se2 thin film by sputtering from Cu(In,Ga)Se2 quaternary target[J].Progress in Natural Science:Materials International,2013,23(2):133-138.
[15]耿魁伟,曾飞,谷宇,李晓伟,宋成,潘峰.超高真空电子束蒸镀Fe/Ru多层膜的结构和磁性[J].中国有色金属学报,2005,15(11):1833-1837.GENG Kui-wei,ZENG Fei,GU Yu,LI Xiao-wei,SONG Chen,PAN Feng.Structural and magnetic properties of Fe/Ru multilayers prepared by ultra-high vacuum electron-gun evaporation[J].The Chinese Journal of Nonferrous Metals,2005,15(11):1833-1837.
[16]郝安林.电子束蒸发法制备Co/Ru多层膜的微观结构与磁电阻[J].粉末冶金材料科学与工程,2014,19(5):832-838.HAO An-lin.Microstructure and magneto-resistor of Co/Ru multimembranes fabricated by electron beam vapor deposition method[J].Materials Science and Engineering of Powder Metallurgy,2014,19(5):832-838.
[17]MEN Chuan-ling,TIAN Ziao,SHAO Qiu-ping,ZHANG Hua,AN Zheng-hua.Characterization of Cu(In,Ga)Se2 films deposited by single-step electron beam evaporation for solar cell applications[J].Applied Surface Science,2012,258:10195-10198.
[18]VENKATACHALAMA M,KANNANA M D,JAYAKUMARA S,BALASUNDARAPRABHUA R,NANDAKUMARA A K,MUTHUKUMARASAMY N.Cu Inx Ga1-x Se2 thin films prepared by electron beam evaporation[J].Solar Energy Materials and Solar Cells,2008,92:571-575.
[19]LEI C,LI C M,ROCKETT A,ROBERTSON I M.Grain boundary compositions in Cu(In,Ga)Se2[J].Journal of Applied Physics,2007,101:024909–1-7.
[20]BAEK E R,ASTINI V,TIRTA A,KIM B.Phase evolution of CIGS alloyed compound synthesis by direct melting method[J].Current Applied Physics,2011,11:S76-S80.
[21]CONTRERAS M A,ROMERO M J,NOUFI R.Characterization of Cu(In,Ga)Se2 materials used in record performance solar cells[J].Thin Solid Films,2006,511/512:51-54.
[22]戴永年,杨斌.有色金属材料的真空冶金[M].北京:冶金工业出版社,2000:24-28.DAI Yong-nian,YANG Bin.Vacuum metallurgy of nonferrous metal materials[M].Beijing:Metallurgical Industry Press,2000:24-28.
[23]VENKATACHALAM M,KANNAN M D,MUTHUKUMARASAMY N,PRASANNA S,JAYAKUMAR S,BALASUNDARAPRABHU R,SAROJA M.Investigations on electron beam evaporated Cu(In0.85Ga0.15)Se2 thin film solar cells[J].Solar Energy,2009,83:1652-1655.
[24]ROCKETT A.The effect of Na in polycrystalline and epitaxial single-crystal Cu In1-x Gax Se2[J].Thin Solid Films,2005,480/481:2-7.
[25]LI Z H,CHO E S,KWON S J.Properties of the Cu(In,Ga)Se2absorbers deposited by electron-beam evaporation method for solar cells[J].Current Applied Physics,2011,11:28-33.
[26]MADHURI K V,NAIDU B S,HUSSAIN O M,EDDRIEF M,JULIEN C.Physical investigations on electron beam evaporated V2O5-Mo O3 thin films[J].Materials Science and Engineering B,2001,86:165-171.
[27]周丽梅,高宏,薛钰芝.铜铟铝硒(CIAS)薄膜太阳电池关键材料–制备和性能[M].北京:化学工业出版社,2014:11-14.ZHOU Li-mei,GAO Hong,XUE Yu-zhi.The preparation and properties research of copper indium aluminum selenium for key material of thin film solar cells[M].Beijing:Chemical Industry Press,2014:11-14.
[2]JACKSON P,HARISKOS D,WUERZ R,KIOWSKI O,BAUER A,FRIEDLMEIER T M,POWALLA M.Properties of Cu(In,Ga)Se2 solar cells with new record efficiencies up to21.7%[J].Physica Status Solidi-Rapid Research Litters,2015,9(1):28-31.
[3]栾和新,庄大明,曹明杰,刘江.磁控溅射法制备CIGS薄膜太阳电池的工艺及性能研究[J].真空科学与技术学报,2012,32(8):661-668.LUAN He-xin,ZHUANG Da-ming,CAO Ming-jie,LIU Jiang.Growth and characterization of copper indium gallium diselenide films for solar cells fabrication[J].Chinese Journal of Vacuum Science and Technology,2012,32(8):661-668.
[4]张秀清,李艳红,张超.太阳电池研究进展[J].中国材料进展,2014,33(7):436-441.ZHANG Xiu-qing,LI Yan-hong,ZHANG Chao.Research progress on solar cell[J].Materials China,2014,33(7):436-441.
[5]朱晓晶,马建华,姚娘娟,梁艳,江锦春,王善力,褚君浩.Cu In Se2薄膜的化学溶液制备方法[J].红外与毫米波学报,2014,33(3):231-236.ZHU Xiao-jing,MA Jian-hua,YAO Niang-juan,LIANG Yan,JIANG Jin-chun,WANG Shan-li,CHU Jun-hao.Preparation of Cu In Se2 thin films by chemical solution method[J].J Infrared Millim&Waves,2014,33(3):231-236.
[6]PARK J W,CHOI Y W,LEE E,JOO O S,YOON S,MIN B K.Synthesis of CIGS absorber layers via a paste coating[J].Journal of Crystal Growth,2009,311:2621-2625.
[7]XIA Dong-lin,LI Jang-zhuang,XU Man,ZHAO Xiu-jian.Electrodeposited and selenized CIGS thin films for solar cells[J].Journal of Non-Crystalline Solids,2008,354:1447-1450.
[8]REPINS I,CONTRERAS M A,EGAAS B,DEHART C,SCHARF J,PERKINS C L,TO B,NOUFI R.19.9%-efficient Zn O/Cd S/Cu In Ga Se2 solar cell with 81.2%fill factor[J].Progress in Photovoltaics:Research and Applications,2008,16:235-239.
[9]SHI J H,LI Z Q,ZHANG D W,LIU Q Q,SUN Z,HUANG S M.Fabrication of Cu(In,Ga)Se2 thin films by sputtering from a single quaternary chalcogenide target[J].Progress in Photovoltaics:Research and Applications,2011,19:160-164.
[10]张晓科,王可,解晶莹.CIGS太阳电池的低成本制备工艺[J].电源技术,2005,29(12):849-852.ZHANG Xiao-ke,WANG Ke,XIE Jing-ying.Low costprocessing of CIGS solar cells[J].Chinese Journal of Power Sources,2005,29(12):849-852.
[11]李伟,刘平,王卫兵,马凤仓,刘新宽,陈勤妙,韩朝霞.CIGS薄膜太阳电池吸收层的非真空制备工艺研究进展[J].材料导报A,2012,26(5):134-137.LI Wei,LIU Ping,WANG Wei-bing,MA Feng-cang,LIU Xin-kuan,CHEN Qin-miao,HAN Zhao-xia.Research progress in non-vacuum processing for absorber layer of CIGS thin film solar cell[J].Material Review A,2012,26(5):134-137.
[12]郭杏元,许生,曾鹏举,范垂祯.CIGS薄膜太阳电池吸收层制备工艺综述[J].真空与低温,2008,14(3):125-132.GUO Xing-yuan,XU Sheng,ZENG Peng-ju,FAN Chui-zhen.Review on fabrication process of the absorber layer of the CIGS thin-film solar cell[J].Vacuum&Cryogenics,2008,14(3):125-132.
[13]ZHANG Li,XUE Yu-ming,XU Chuan-ming,HE Qing,LIU Fang-fang,LI Chang-jian,SUN Yun.Microstructural characterization of Cu-poor Cu(In,Ga)Se2 surface layer[J].Thin Solid Films,2012,520:2873-2877.
[14]LIU Jiang,ZHUANG Da-ming,LUAN He-xin,CAO Ming-jie,XIE Min,LI Xiao-long.Preparation of Cu(In,Ga)Se2 thin film by sputtering from Cu(In,Ga)Se2 quaternary target[J].Progress in Natural Science:Materials International,2013,23(2):133-138.
[15]耿魁伟,曾飞,谷宇,李晓伟,宋成,潘峰.超高真空电子束蒸镀Fe/Ru多层膜的结构和磁性[J].中国有色金属学报,2005,15(11):1833-1837.GENG Kui-wei,ZENG Fei,GU Yu,LI Xiao-wei,SONG Chen,PAN Feng.Structural and magnetic properties of Fe/Ru multilayers prepared by ultra-high vacuum electron-gun evaporation[J].The Chinese Journal of Nonferrous Metals,2005,15(11):1833-1837.
[16]郝安林.电子束蒸发法制备Co/Ru多层膜的微观结构与磁电阻[J].粉末冶金材料科学与工程,2014,19(5):832-838.HAO An-lin.Microstructure and magneto-resistor of Co/Ru multimembranes fabricated by electron beam vapor deposition method[J].Materials Science and Engineering of Powder Metallurgy,2014,19(5):832-838.
[17]MEN Chuan-ling,TIAN Ziao,SHAO Qiu-ping,ZHANG Hua,AN Zheng-hua.Characterization of Cu(In,Ga)Se2 films deposited by single-step electron beam evaporation for solar cell applications[J].Applied Surface Science,2012,258:10195-10198.
[18]VENKATACHALAMA M,KANNANA M D,JAYAKUMARA S,BALASUNDARAPRABHUA R,NANDAKUMARA A K,MUTHUKUMARASAMY N.Cu Inx Ga1-x Se2 thin films prepared by electron beam evaporation[J].Solar Energy Materials and Solar Cells,2008,92:571-575.
[19]LEI C,LI C M,ROCKETT A,ROBERTSON I M.Grain boundary compositions in Cu(In,Ga)Se2[J].Journal of Applied Physics,2007,101:024909–1-7.
[20]BAEK E R,ASTINI V,TIRTA A,KIM B.Phase evolution of CIGS alloyed compound synthesis by direct melting method[J].Current Applied Physics,2011,11:S76-S80.
[21]CONTRERAS M A,ROMERO M J,NOUFI R.Characterization of Cu(In,Ga)Se2 materials used in record performance solar cells[J].Thin Solid Films,2006,511/512:51-54.
[22]戴永年,杨斌.有色金属材料的真空冶金[M].北京:冶金工业出版社,2000:24-28.DAI Yong-nian,YANG Bin.Vacuum metallurgy of nonferrous metal materials[M].Beijing:Metallurgical Industry Press,2000:24-28.
[23]VENKATACHALAM M,KANNAN M D,MUTHUKUMARASAMY N,PRASANNA S,JAYAKUMAR S,BALASUNDARAPRABHU R,SAROJA M.Investigations on electron beam evaporated Cu(In0.85Ga0.15)Se2 thin film solar cells[J].Solar Energy,2009,83:1652-1655.
[24]ROCKETT A.The effect of Na in polycrystalline and epitaxial single-crystal Cu In1-x Gax Se2[J].Thin Solid Films,2005,480/481:2-7.
[25]LI Z H,CHO E S,KWON S J.Properties of the Cu(In,Ga)Se2absorbers deposited by electron-beam evaporation method for solar cells[J].Current Applied Physics,2011,11:28-33.
[26]MADHURI K V,NAIDU B S,HUSSAIN O M,EDDRIEF M,JULIEN C.Physical investigations on electron beam evaporated V2O5-Mo O3 thin films[J].Materials Science and Engineering B,2001,86:165-171.
[27]周丽梅,高宏,薛钰芝.铜铟铝硒(CIAS)薄膜太阳电池关键材料–制备和性能[M].北京:化学工业出版社,2014:11-14.ZHOU Li-mei,GAO Hong,XUE Yu-zhi.The preparation and properties research of copper indium aluminum selenium for key material of thin film solar cells[M].Beijing:Chemical Industry Press,2014:11-14.
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