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標題: | 黃銅礦結構薄膜太陽電池光吸收層與緩衝層材料之製備與特性分析 Preparation and Characterization of Chalcopyrite-based Films Used in the Absorber Layers and Buffer Layers of Thin-film Solar Cells |
作者: | Shin-Hom Lin 林信宏 |
指導教授: | 呂宗昕(Chung-Hsin Lu) |
關鍵字: | 黃銅礦,銅銦鎵硒,吸收層,薄膜,太陽電池, chalcopyrite,CIGS,absorber,thin film,solar cells, |
出版年 : | 2014 |
學位: | 博士 |
摘要: | 本論文針對黃銅礦結構太陽電池緩衝層材料及光吸收層材料進行製備與特性分析。利用塗佈法結合硒化製程製備黃銅礦結構之ZnIn2Se4薄膜,並做為替代型緩衝層薄膜應用於Cu(In,Ga)Se2太陽電池。為改善薄膜之晶粒成長與光電特性,利用鉍成份來添加進入濺鍍法製備之Cu(In,Ga)Se2薄膜中。並為提昇吸收層薄膜之表面能隙及減少硒缺陷,使用硫成份來導入吸收層薄膜Cu(In,Ga)(Se,S)2之表面以提昇其薄膜之光電特性。為進一步提昇光電特性與減少薄膜內部缺陷,Cu(In,Ga)(Se,S)2薄膜將以改質式硒硫化反應來製備,並針對於本研究中所製備之太陽光電元件特性與理想因子分析之影響進行探討
論文第一部份使用塗佈法結合硒化法成功製備黃銅礦結構之ZnIn2Se4薄膜。隨增加硒化反應溫度,所製備得之ZnIn2Se4薄膜的緻密程度與導電特性可以被增加。並利用ZnIn2Se4薄膜作為緩衝層結合Cu(In,Ga)(Se,S)2薄膜製作太陽光電元件,可有效產生光電流。以塗佈法結合硒化法成功製備之ZnIn2Se4薄膜,可製作為替代式緩衝層薄膜於CIGS太陽電池之應用中。 本論文之第二部份中,為提昇Cu(In,Ga)Se2太陽電池之光電特性,開發利用鉍添加入濺鍍法製備Cu(In,Ga)Se2薄膜之中。添加入鉍於硒化過程中可形成銅鉍硒化合物與前驅膜產生液相燒結,並可提昇整體薄膜之晶粒成長與緻密程度。於鉍添加之Cu(In,Ga)Se2薄膜可提昇鎵離子擴散並改善晶粒成長特性,其所製備Cu(In,Ga)Se2太陽電池之光電轉化效率可有效提升。 於第三部份中,以硒化法結合後硫化法製備Cu(In,Ga)(Se,S)2薄膜。於硒化法結合硫化法後,可於吸收層薄膜表面形成高硫含量之Cu(In,Ga)(Se,S)2薄膜,並提昇吸收層與緩衝層接面的能隙。並於螢光光譜分析中指出經由後硫化反應之適化控制可有效減少薄膜表面之硒缺陷。經由後硫化反應處理後,Cu(In,Ga)(Se,S)2太陽電池之開環電壓、填充因子及轉化效率可進一步提昇。 於論文之第四部份,以改良式硒硫化製程製備Cu(In,Ga)(Se,S)2薄膜並進行分析研究。於此改良式硒硫化製程反應後,薄膜中之鎵離子擴散可被提昇並其薄膜中之電子電洞再結合可被有效抑制。於本部份中所製備之Cu(In,Ga)(Se,S)2薄膜之光電轉化效率、開環電壓及填充因子可被有效增加。在最後部份中,在以鉍成份添加進入改質式硒硫化製程製備之Cu(In,Ga)(Se,S)2薄膜中,其薄膜所組成之太陽光電元件效率進一步提昇。本研究成功開發黃銅礦緩衝層薄膜之與製備具有高效率之Cu(In,Ga)(Se,S)2太陽電池,可用於提昇黃銅礦結構之太陽電池特性與發展應用。 The chalcopyrite-based buffer and absorber layers were prepared for the application of Cu(In,Ga)Se2-based solar cells in this thesis. Zinc indium selenide films with a defective chalcopyrite structure were fabricated via a spin coating route for the alternative buffer layers used in Cu(In,Ga)Se2-based solar cells. The bismuth species were added into sputtering-derived Cu(In,Ga)Se2 films to improve the grain growth and the photovoltaic properties of the obtained films. Additionally, the sulfur species were incorporated into Cu(In,Ga)Se2 films for increasing the band gap and reducing the defects of selenium near the surface region of absorber films. For further increasing the photovoltaic characteristics and eliminating the defects of solar cells, Cu(In,Ga)(Se,S)2 films were prepared via the modified selenization and sulfurization process. The photovoltaic performance and diode analysis of the fabricated solar cells were investigated. Defective chalcopyrite-based ZnIn2Se4 films were successfully synthesized via a spin coating process with a sequential selenization treatment. With elevating the selenziation temperature, the densification and electric properties of the prepared ZnIn2Se4 films were significantly increased. The photocurrent was generated from the Cu(In,Ga)Se2 films combined with the spin-coated ZnIn2Se4 films. ZnIn2Se4 layers prepared via the spin coating process were presented to be an effective approach for the alternative buffer layers used in Cu(In,Ga)Se2 solar cells. In the second section, for increasing the photovoltaic properties of Cu(In,Ga)Se2 films, bismuth species were utilized to add into sputtering-derived Cu(In,Ga)Se2 films. The liquid-phase sintering was yielded by copper bismuth selenide compound to facilitate the grain growth and densification of obtained Cu(In,Ga)Se2 films. The conversion efficiency of the bismuth-doped Cu(In,Ga)Se2 solar cells was effective increased owing to the improvement of the gallium distribution and the grain growth resulted from the bismuth-ion doping. In the third section, the preparation for Cu(In,Ga)(Se,S)2 films incorporated with sulfur species via a sulfurization treatment after selenization process was investigated. The Cu(In,Ga)(Se,S)2 layers with sulfur-rich content were formed near the surface region of absorber films to increase the band gap at the interface of absorber/buffer layers. The photoluminescence spectra indicated that the selenium vacancies near the surface region of the obtained Cu(In,Ga)(Se,S)2 films were significantly reduced with the well-controlled duration of sulfurization. The conversion efficiency of the resulting Cu(In,Ga)(Se,S)2 solar cells were further increased owing to the improvement of open circuit voltage and fill factor. In the four section, Cu(In,Ga)(Se,S)2 films were prepared using the modified chalcogenization process. After the reaction of the modified chalcogenization method, the gallium distribution of the prepared Cu(In,Ga)(Se,S)2 films could be improved and the recombination of electron and hole in obtained absorber films was further suppressed. The conversion efficiency of the fabricated solar cells using the Cu(In,Ga)(Se,S)2 films derived from the modified chalcogenization process was improved. Moreover, the photovoltaic performance of the bismuth-doped Cu(In,Ga)(Se,S)2 absorber films with via the modified chalcogenization method was further improved by the well controlling of doping with bismuth and sulfur species. This thesis developed the new preparation process for the alternative buffer layers and fabricating highly-efficient Cu(In,Ga)(Se,S)2 solar cells used in the field of CIGS-based photovoltaic technology. |
URI: | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/18518 |
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