电子束蒸发技术生长高迁移率IWO（In_2O_3：WO_3）薄膜的研究
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摘要
本文采用电子束反应蒸发法,选用自制的掺WO_3的In_2O_3陶瓷靶材,制备IWO(In_2O_3:WO_3)透明导电氧化物薄膜。研究WO_3掺杂浓度、衬底温度、氧流量、薄膜厚度、退火处理、SiO_2和Al_2O_3阻挡层以及梯度速率等因素对IWO薄膜结构特性、光学特性和电学特性的影响。
在WO_3掺杂浓度为0.35%、衬底温度为350℃、氧流量为35sccm、薄膜厚度为800?(实测为120nm)条件下制备的IWO薄膜的载流子迁移率μ为47.9cm2V-1s-1,载流子浓度n为2.66×1020cm~(-3),电阻率ρ为4.89×10-4?cm,400nm-1000nm波长范围光平均透过率为76%(含玻璃衬底)。Ar氛围中500℃退火1h,得到最高载流子迁移率μ为66.2 cm2V-1s-1。一定厚度的SiO_2和Al_2O_3薄膜作为阻挡层,改善了薄膜的电学性能,提高了薄膜的载流子迁移率μ。梯度速率生长方式制备IWO薄膜,得到了质量较好的薄膜:载流子迁移率μ为67.1 cm2V-1s-1,载流子浓度n为1.84×1020cm~(-3),最低电阻率ρ为5.05×10-4?cm,而400nm-1100nm波段的平均透过率约为77%(含玻璃衬底)。
最后,将常规生长的IWO薄膜应用到有机薄膜太阳电池中,得到电池的转换效率为3.426%。
Tungsten doped indium oxide (IWO-In_2O_3:WO_3) thin films were deposited on glass substrates by reactive electron beam deposition technique, using homemade In_2O_3 ceramics targets with WO_3 dopant. The influence of doping concentration, substrate temperature, oxygen flow rate, film thickness, annealing, SiO_2 and Al_2O_3 buffer layer and gradual growth rates on the structural, optical and electrical properties of the IWO films were investigated in detail.
The IWO thin films as the deposited by reactive electron beam deposition technique under the conditions of the doping concentration~0.35%, substrate temperature~ 350℃, the O_2 flows~35sccm, and the film thickness is 800?(~120nm). Typical thin film performances: the mobilityμ~47.9cm2V-1s-1 , the carrier concentration n~2.66×1020cm~(-3) and the resistivityρ~4.89×10-4?cm. The optimizing optical transmittance is ~76% (including float glass) at the light wavelength between 400 to 1100 nm. The mobility is improved to 66.2cm2V-1s-1 after annealing at 500℃in an Ar atmosphere. SiO_2 and Al_2O_3 films as buffer layers on glass substrates also can improve the quality of the IWO thin films. The IWO thin films obtained with the gradual growth rates have good thin film quality, with the high mobilityμ~67.1cm2V-1s-1,the carrier concentration n~1.84×1020cm~(-3) and the low resistivityρ~5.05×10-4?cm. The optimizing average transmittance is ~77% (including float glass substrate) in the light wavelength range from 400nm to 1100 nm.
Finally, IWO(In_2O_3:WO_3) thin film was applied in organic thin film solar cell with an efficiency of ~3.426%.
在WO_3掺杂浓度为0.35%、衬底温度为350℃、氧流量为35sccm、薄膜厚度为800?(实测为120nm)条件下制备的IWO薄膜的载流子迁移率μ为47.9cm2V-1s-1,载流子浓度n为2.66×1020cm~(-3),电阻率ρ为4.89×10-4?cm,400nm-1000nm波长范围光平均透过率为76%(含玻璃衬底)。Ar氛围中500℃退火1h,得到最高载流子迁移率μ为66.2 cm2V-1s-1。一定厚度的SiO_2和Al_2O_3薄膜作为阻挡层,改善了薄膜的电学性能,提高了薄膜的载流子迁移率μ。梯度速率生长方式制备IWO薄膜,得到了质量较好的薄膜:载流子迁移率μ为67.1 cm2V-1s-1,载流子浓度n为1.84×1020cm~(-3),最低电阻率ρ为5.05×10-4?cm,而400nm-1100nm波段的平均透过率约为77%(含玻璃衬底)。
最后,将常规生长的IWO薄膜应用到有机薄膜太阳电池中,得到电池的转换效率为3.426%。
Tungsten doped indium oxide (IWO-In_2O_3:WO_3) thin films were deposited on glass substrates by reactive electron beam deposition technique, using homemade In_2O_3 ceramics targets with WO_3 dopant. The influence of doping concentration, substrate temperature, oxygen flow rate, film thickness, annealing, SiO_2 and Al_2O_3 buffer layer and gradual growth rates on the structural, optical and electrical properties of the IWO films were investigated in detail.
The IWO thin films as the deposited by reactive electron beam deposition technique under the conditions of the doping concentration~0.35%, substrate temperature~ 350℃, the O_2 flows~35sccm, and the film thickness is 800?(~120nm). Typical thin film performances: the mobilityμ~47.9cm2V-1s-1 , the carrier concentration n~2.66×1020cm~(-3) and the resistivityρ~4.89×10-4?cm. The optimizing optical transmittance is ~76% (including float glass) at the light wavelength between 400 to 1100 nm. The mobility is improved to 66.2cm2V-1s-1 after annealing at 500℃in an Ar atmosphere. SiO_2 and Al_2O_3 films as buffer layers on glass substrates also can improve the quality of the IWO thin films. The IWO thin films obtained with the gradual growth rates have good thin film quality, with the high mobilityμ~67.1cm2V-1s-1,the carrier concentration n~1.84×1020cm~(-3) and the low resistivityρ~5.05×10-4?cm. The optimizing average transmittance is ~77% (including float glass substrate) in the light wavelength range from 400nm to 1100 nm.
Finally, IWO(In_2O_3:WO_3) thin film was applied in organic thin film solar cell with an efficiency of ~3.426%.
引文
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[2]范永杰,於黄忠,林文健.太阳电池的原理及结构研究进展[J].中国材料科技与设备(双月刊),2008,2:16～18
[3] JN.B.Chaure, J.Young, A.P.Samantilleke, et al. Electro-deposition of p-i-n CulnSe2 multi-layer for photovoltaic applications[J].Solar Energy Materials and Solar Cells.2004,81:125～133
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[7]崔海昱,涂洁磊,邓菊莲,等.玻璃衬底多晶硅薄膜太阳电池的制备[J].可再生能源,2008,26(5):72～75
[8]鲁大学.透明导电氧化物镀膜玻璃在光伏电池中的应用[J].玻璃深加工,2008,10:33～37
[9]望咏林,颜悦,沈玫,等.透明导电氧化物薄膜研究进展[J].材料导报,2006,20(5):317～320
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[11]陈辉明.浙江大学硕士论文.1998.61
[12] Al-Ajili A N H,Bayliss S C.A study of the optical,electrical and structural properties of reactively sputtered InOx and ITOx thin film. Thin Solid Films,1997,305:106
[13] Yang M,Yang X L,Chen H X,et al.A new transparent conductive thin film In2O3:Mo.Thin Solid Films,2001,394(1-2):218
[14]孟扬,杨锡良,陈华仙,等.高价态差掺杂氧化物透明导电薄膜的研究[J].光电子技术,2001,21(1):17～21
[15] Yang Zhiwei, Han Shenghao, Yan Tianlin,et al. Preparation of ITO films on water-cooled flexible substrate by bias R.F.Magnetron Sputtering[J]. J.Phys, 2000,6(49):1196～1201
[16]孟扬,沈杰,蒋益明,等.透明导电氧化物薄膜的新进展[J] .光电子技术,2002,22(3):125～144
[17]王敏,蒙继龙.透明导电氧化物薄膜的研究进展[J].表面技术,2003,32(1):5～7
[18]赵谢群.透明导电氧化物薄膜研究现状与产业化进展[J].电子元件与材料,2000,2:40～41
[19]徐慢,夏冬林,赵修建.透明导电氧化物薄膜材料及其制备技术研究进展[J].材料导报,2006,20:312～322
[20] Vossen J L.In:Hass G, Francombe M H, Hoffman R H(Eds.) .Phusics of Thin Fillms.New York:Academic Press,1977
[21] Choong H Y,Itaru Y,Shigesato Y.Effects of tin concentration on structural characteristics and electro optical properties of tin-doped indium oxide films prepared bu r.f.magnetron sputtering[J] .Jpn J Appl Phys,1995,34:600
[22]孟扬,杨锡良,陈华仙,等.新型透明导电薄膜In2O3:Mo[J] .真空科学与技术,2000,20(5) :331
[23] Goebberta C, Nonningerb R, Aegerter M A, etal. Wetchemical deposition of ATO and ITO coatigs using crystalline nanoparticles redispersable in solutions[J].Thin Solid Films,1999,351:79
[24] Kelly P J, Zhou Y, Postill A.A novel technique for the deposition of aluminum-doped zinc oxide films[J].Thin Solid Films 2003,426:111
[25] Tominagaa K, Takaoa T, Fukushima A, etal.Amorphous ZnO-In2O3 transparent conductive films by simultaneous sputtering method of ZnO and In2O3 targets[J].Vacuum,2002,66:505
[26] Valenzuela M A,Jacobs J P,Bosch P,eta1.The influence of the preparation method on the surface structure of ZnA1204[J].Appl Cataly A,1997,148:315
[27] Minami T, Takeda Y, Takata S, etal.Preparation of transparent conducting In4Sn3O12 thin films by DC magnetron sputtering[J].Thin Solid Films,1997, 13:308-309
[28]姜燮昌,胡勇.ITO膜透明导电玻璃的应用前景及工业化生产[J].真空,1995,12:1～3
[29]张德恒.透明导电膜中光吸收边的移动[J].半导体杂志,1998,9:36
[30] Ma Honglei, Zhang Deheng. Large-scale fluorine-doped textured transparent conducting SnO2 films deposited by APCVD[J].Proceedings of SPIE-the International Society for Optical Engineering,1996,2897(6-7):104～112
[31] Shanthi S, Subramanian C, Ramasamy P. Growth and characterization of antimony doped tin oxide thin films[J].Journal of Crystal Growth,1999,197(4):858～864
[32]裴志亮,谭明辉,等.透明导电氧化物ZnO:A1(ZA0)薄膜的研究[J].金属学报,2000,1:72
[33] Alma M J,Cameron DC. Characterization of transparent conductive ITO thin films deposited on titanium dioxide film by a sol—gel process[J] .Surface and Coatings Technology,2001,6:776～780
[34] Annette Huhaker,Kenneth Jarrendahl. Electrical and optical properties of sputter deposited tin doped indium oxide thin films with silver additive[J].thin solid films,2001,392:305～310
[35] Minami Tadatsugu, Yamamoto Takashi. Transparent conducting zinc-co-doped ITO films prepared by magnetron sputtering[J].Thin Solid Films,2000,(9):189～194
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