本文旨在探索最適合Ⅰ-Ⅱ-Ⅳ-Ⅵ族薄膜太陽能電池的熱處理程序，並透過雙重離子取代來提升薄膜太陽能電池的轉換效率。此外並結合材料模擬及元件實作探討Ⅰ-Ⅱ-Ⅳ-Ⅵ族化合物半導體薄膜太陽能電池的光電性質以及硒化機制。在材料模擬方面，本文使用CASTEP/Materials Studio模擬軟體預測雙重離子取代法對材料性質的影響。至於在實作方面，採用非真空直接升溫合成法來制備Ⅰ-Ⅱ-Ⅳ-Ⅵ族太陽能電池中的硫化銅鋅錫(Cu2ZnSnS4,CZTS)或是雙重離子取代法中陽離子取代的硫化銅銀鋅錫((AgxCu1-x)2ZnSnS4,ACZTS)前驅物(precursor)，透過旋轉塗佈製備生胚薄膜。再使用加壓硒化製程以及加壓預燒結製程等快速熱退火製程對生胚薄膜進行硒化熱處理。研究結果發現，透過雙重離子取代法以及在加壓硒化製程前先行施以加壓預燒結製程可使吸收層薄膜的霍爾電性獲得顯著的改善。雖然由於薄膜太陽能電池中窗口層的微結構不佳並同時在窗口層與上電極之間形成了低品質的異質接面，進而劣化元件的光電轉換效率，不過仍然清楚證明了可以透過兩階段快速熱退火製程以及雙重離子取代使元件的光電轉換效率由0.034%顯著的提升至0.724%。
除了透過多種熱處理方法及雙重離子取代法優化薄膜太陽能電池的轉換效率外，經實驗發現當CZTS薄膜經過加壓硒化製程後，其薄膜微結構將會由原本的單層結構轉變成大晶粒層在上、細晶層在下的雙層結構。本文成功提出了加壓硒化製程的反應機制，整個反應依序為CZTSSe再結晶、液相燒結最後為固相燒結。相信透過硒化機制的探討能提升未來對CZTSSe大晶粒微結構及緻密度的掌控性。

In this study, the photoelectric conversion efficiency of the I-II-IV-VI thin film solar cell (TFSC) was effectively promoted not only through the optimization of the heat treatment process but also through the double ions substitution method. The CASTEP/Material Studio simulation software was used to predict the double ions substitution effect on the electric properties of the ACZTSSe. The direct heating up method was used to synthesize the CZTS or ACZTS precursor, followed by spin coating to fabricate the green thin film. Next, the different rapid thermal annealing methods such as the pressure-assisted selenization process and the pressure-assisted pre-sintering process were used to optimize the selenization process. Finally, the photoelectric conversion efficiency of the TFSC prepared by using the optimized heat treatment and double ions substitution method was measured by the Solar Simulator. The results show that the electrical properties of the absorber can be significantly improved through the double ions substitution method and two-step rapid thermal annealing process. However, due to the poor microstructure of the window layer (ITO) in the TFSC and the low-quality heterojunction between the window layer and the upper electrode, the photoelectric conversion efficiency of the TFSC has deteriorated. However, the conversion efficiency of the TFSC was significantly promoted from 0.034% to 0.724% by the optimization of the heat treatment method and double ions substitution method. In addition, this study also successfully proposed the reaction mechanism of the pressurized selenization process. The entire reaction was CZTSSe recrystallization, liquid phase sintering and finally solid-phase sintering.

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