CIAS薄膜光伏材料的研究
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摘要
近年来,CuInSe_2类薄膜太阳能电池以其较高的转换效率,较低的成本以及较稳定的性能备受人们关注。而且其生产正趋于商业化,如何提高电池的光电转换效率成为研究的关键,而吸收层CIS类材料正是影响电池光电转换效率的关键因素。研究表明,通过掺杂第三或第四族元素可以增加CuInSe_2的禁带宽度(Eg)和太阳光谱的配合度得到更高的效率。由于Al的价格比较低廉,用Al来部分的替代In,不仅可获得较宽带系的合金层,改善CuInSe_2类薄膜太阳能电池的性能,而且还可以大大的降低成本,这也正是本实验研究用Al来部分的代替In,制备Cu(In_(1-x)Al_x)Se_2多晶薄膜材料的意义所在。
本实验使用DMX-220A型比较简单的常规小型镀膜设备,采用先沉积In-Al-Cu多层膜预制层,后用自制的真空硒化退火装置来获得Cu(In_(1-x)Al_x)Se_2多晶薄膜。进而,对制得的样品用X射线衍射仪(XRD)、扫描电镜(SEM)、能谱仪(EDX)、四探针电阻测试仪、分光光度计等进行了检测,并对结果进行了分析。研究最佳的制备工艺,并研究其中Al含量对薄膜形貌和结构的影响。
对薄膜制备工艺研究表明:真空蒸发制备In-Al-Cu预制层后,在500℃,退火1h的条件下,用一步硒化退火法制备的薄膜质量较好。而且通过SEM和XRD微观形貌结构分析发现,薄膜中Al的含量对薄膜的表面形貌和结构有一定的影响。Al/(In+Al)比例越大,越容易获得尺寸较小,分布比较均匀的晶粒。而且当Al的含量增加时, Cu(In_(1-X)Al_X)Se_2峰的位置会在更大的2θ处出现。同时Al含量对薄膜的方阻有一定的影响,Al含量越高,方阻越大。Al含量可以调节薄膜的禁带宽度的大小。正由于Cu(In_(1-X)Al_X)Se_2薄膜的这个特性,使其在太阳能电池应用方面有着突出的地位。
In recent years, CuInSe_2 thin film solar cells are took much attention with its higher conversion efficiency, lower costs and much more stable performance. As its production process moving towards commercialization, a key for researching is how to improve efficiency of photovoltaic conversion of battery, and the absorption layer material CIS is the key factor which affects battery photoelectric conversion efficiency. Study shows that: the CuInSe_2 band gap (Eg) can be increased to match the solar spectrum for higher efficiency by alloying the group III or VI elements. Because of the relatively low price, part of substituting In with Al, not only can be got of wider band gap alloys and improved the performance of thin film CuInSe_2 based solar cells, but also can significantly reduce costs. This is the significance that why substituting In with Al in part and propagating of Cu (In_(1-x)Al_x) Se_2 polycrystalline thin film materials in this experiment.
In this paper, Cu (In_(1-x)Al_x) Se_2 polycrystalline thin film is obtained by selenization with Self-madden vacuum equipment after that In-Al-Cu multilayer is deposited on glass substrates by vacuum evaporation with small-scale coating equipment which type is DMX-220A. SEM, XRD, Four Point probe resistance instrument and spectrophotometer are use to determine the performance of these thin films, and then study the best prep rational technology and Al content how to impact on surface morphology and structure of the thin film.
Study on preparation of film shows that: Using the method of selenized annealing at one step can prepared the best quality thin film with the conditions of annealing 1h and 500℃after preparating of In-Al-Cu layer with vacuum evaporation. The SEM and XRD results of micro structural morphology show that: The content of Al in thin films has a certain impact on surface morphology and structure. The larger ratio of Al / (In + Al), the more easy access to the grain of smaller sizes, and more evenly distributed. As the Al content increases, the position of the Cu (In_(1-X)Al_X) Se_2 peaks shift to higher 2θ.The content of Al also has a impact on sheet resistance, the higher content of Al, the greater in sheet resistance. And the band gap can be adjusted by controlling the Al content.Because of this characteristics, Cu (In_(1-x)Al_x) Se_2 have a prominent place on solar cells applications of film.
本实验使用DMX-220A型比较简单的常规小型镀膜设备,采用先沉积In-Al-Cu多层膜预制层,后用自制的真空硒化退火装置来获得Cu(In_(1-x)Al_x)Se_2多晶薄膜。进而,对制得的样品用X射线衍射仪(XRD)、扫描电镜(SEM)、能谱仪(EDX)、四探针电阻测试仪、分光光度计等进行了检测,并对结果进行了分析。研究最佳的制备工艺,并研究其中Al含量对薄膜形貌和结构的影响。
对薄膜制备工艺研究表明:真空蒸发制备In-Al-Cu预制层后,在500℃,退火1h的条件下,用一步硒化退火法制备的薄膜质量较好。而且通过SEM和XRD微观形貌结构分析发现,薄膜中Al的含量对薄膜的表面形貌和结构有一定的影响。Al/(In+Al)比例越大,越容易获得尺寸较小,分布比较均匀的晶粒。而且当Al的含量增加时, Cu(In_(1-X)Al_X)Se_2峰的位置会在更大的2θ处出现。同时Al含量对薄膜的方阻有一定的影响,Al含量越高,方阻越大。Al含量可以调节薄膜的禁带宽度的大小。正由于Cu(In_(1-X)Al_X)Se_2薄膜的这个特性,使其在太阳能电池应用方面有着突出的地位。
In recent years, CuInSe_2 thin film solar cells are took much attention with its higher conversion efficiency, lower costs and much more stable performance. As its production process moving towards commercialization, a key for researching is how to improve efficiency of photovoltaic conversion of battery, and the absorption layer material CIS is the key factor which affects battery photoelectric conversion efficiency. Study shows that: the CuInSe_2 band gap (Eg) can be increased to match the solar spectrum for higher efficiency by alloying the group III or VI elements. Because of the relatively low price, part of substituting In with Al, not only can be got of wider band gap alloys and improved the performance of thin film CuInSe_2 based solar cells, but also can significantly reduce costs. This is the significance that why substituting In with Al in part and propagating of Cu (In_(1-x)Al_x) Se_2 polycrystalline thin film materials in this experiment.
In this paper, Cu (In_(1-x)Al_x) Se_2 polycrystalline thin film is obtained by selenization with Self-madden vacuum equipment after that In-Al-Cu multilayer is deposited on glass substrates by vacuum evaporation with small-scale coating equipment which type is DMX-220A. SEM, XRD, Four Point probe resistance instrument and spectrophotometer are use to determine the performance of these thin films, and then study the best prep rational technology and Al content how to impact on surface morphology and structure of the thin film.
Study on preparation of film shows that: Using the method of selenized annealing at one step can prepared the best quality thin film with the conditions of annealing 1h and 500℃after preparating of In-Al-Cu layer with vacuum evaporation. The SEM and XRD results of micro structural morphology show that: The content of Al in thin films has a certain impact on surface morphology and structure. The larger ratio of Al / (In + Al), the more easy access to the grain of smaller sizes, and more evenly distributed. As the Al content increases, the position of the Cu (In_(1-X)Al_X) Se_2 peaks shift to higher 2θ.The content of Al also has a impact on sheet resistance, the higher content of Al, the greater in sheet resistance. And the band gap can be adjusted by controlling the Al content.Because of this characteristics, Cu (In_(1-x)Al_x) Se_2 have a prominent place on solar cells applications of film.
引文
[1]香港《大公报》,2001年3月31日(A2版)
[2]香港《大公报》,2001年3月30日(A4版)
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[2]香港《大公报》,2001年3月30日(A4版)
[3]耿新华,孙云,王宗畔,李长健.薄膜太阳电池的研究进展.物理,1999,28(2):96-97
[4]赵玉文.太阳电池新进展.物理学与新能源材料专题,2004,33(2):99
[5]雪莲,吴麟章等.太阳能电池及其应用.武汉科技学院学报,2005,18(10):6-37
[6]叶志镇等.硅上超高真空CVD生长硅锗外性研究.半导体学报,1999,20(1)
[7]阎明.半导体超晶格及其量子阱的原理.上海海运学院报,2000,21(1):2-107
[8]薛钰芝,Martin Green.Al/Al2O3多层膜的表面和界面的分析研究[J].真空科学与技术学报,2002, 22(1)
[9] Miguel A,Cont reras K,Ramanathan J,et al.Diode characteristics in state-of-the-art ZnO/CdS/Cu(In_(1-x)Ga_x )Se_2 solar cells[J].Prog Photovolt :Res Appl , 2005,13:209
[10] Jasenek A, Rau U, Hahn T, et al.Defect generation in polycrystalline Cu (In, Ga) Se_2 by high-nergy electron irradiation [J].Appl .Phys A, 2000, 70: 677
[11] Shay J L, Wernick J H.Tenary Chalcopyrite Semiconductors: Growth.Electronic Properties and Applications [M].PergamonPress: Oxford, 1975,47
[12] Yakushev M V, Mudryi A V, Gremenok V F, et al.Influence of growth conditions on the st ructural quality of Cu (InGa) Se_2 and CuInSe_2 thin films [J].Thin Solid Films.2004, 452:133
[13]王兴孔.CuInSe_2薄膜太阳电池[J].青岛大学报,2000,13:85
[14] Donnelly S E,Hinks J A,Edmondson P D,et al.In situtransmission electron microscopy studies of radiation damage in copper indium diselenide [J].Nuclear Instruments and Methods in Physics Research Section B:Beam Interactions with Materials and Atoms.2006,242:686
[15] Zheng Guangfu, Yang Hongxing.A novel semiconductor CIGS photovoltaic materialand thin-film ED technology[J].Chinese J Semiconductors.2001,22:1357
[16] Kushiya K,Ohshita M,Hara I,et al.Yield issues on the abrication of 30cm×30cm-sized Cu(In,Ga)Se_2 based thin-film modules[J].Sol Energy Mater Sol Cells.2003,75:17
[17] Powalla M, Dimmler B.Development of large-area CIGS modules [J].Sol Energy Mater Sol Cells.2003, 75:27
[18] Lundberg O,Edoff M,Stolt L.The effect of Ga-grading in CIGS thin film solar cells[J].Thin Solid Films.2005, 520: 480-481
[19]庄大明,张弓.CIGS薄膜太阳能电池研究现状及发展前景[J].新材料产业,2005,4:43
[20]徐知之,夏文建,黄文良.铜铟硒(CIS)薄膜太阳电池研究进展.真空, 2006,43(2):13-14
[21] Contreras M A, AbuShama J, Hasoon F, Young D, Egaas B and Noufi R.Diode Characteristics of State-of-the-Art ZnO/CdS/Cu(In_(1-x)Cax)Se_2 Solar Cells [C].To be submitted for publication in Prog. Photowolt.Res.Appl
[22] LOFERSKI J J. Stoichiometric effects on the properties of copper based chalcopyrite I - III - VI2 semiconductor thin films [J].Materials Science and Engineering B, 1992, 13:271~277
[23]郭杏元,许生,曾鹏举,范垂祯.CIGS薄膜太阳能电池吸收层制备工艺综述.真空与低温,2008,14 (3) :126-130
[24]徐知之,夏文建,黄文良.铜铟硒(CIS)薄膜太阳电池研究进展.真空,2006,43(2):13-14
[25]汤会香,严密,张辉等.磁控溅射金属预置层后硒化法制备CuInSe_2薄膜工艺条件的优化J.半导体学报,2004,25(6):741.
[26] Hunger Ralf, Sakurai Keiichiro, Yamada Akimasa, et al.In situdeposition rate monitoring duringthe three-stage-growth processof Cu(InGa)Se_2 absorber films J.Thin Solid Films,2003, 16:431-432
[27] Bhattacharya Raghu N, Fernandez Arturo M.Cu (In1- xGax) Se_2 based photovoltaic cells from electrodeposited precursor films [J].Sol.En.Mat & Sol.Cells, 2003, 76:331
[28]汤会香,严密,张辉等.热处理对化学水浴沉积法制备的CuInSe_2薄膜的影响[J].太阳能学报,2005, 2(26):363
[29] HollingsworhJ A, Banger K K, Jin M H C, et al.Single source precursorsfor fabrication of I-III-VI thin film solar cells via spray CVD [J].Thin Solid Film, 2003, 63:461-462
[30] Shioda R, Okada Y, Oyanagi H.Characterization of molecular beamepitaxy grown CuInSe_2 on GaAs (001) J.Journal of Crystal Growth, 1995, 150:1196
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