從18世紀工業革命以來，隨著人類科技發展及石化燃料的逐漸枯竭，能源議題備受重視，各界也積極投入發展替代性能源。在眾多太陽能電池中，鈣鈦礦太陽能電池在近五六年以非常快的速度串起，光電轉換效率由3 %線性提升到了超過20 %，引起了許多研究的興趣。
本研究針對鈣鈦礦太陽能電池進行低溫製程研究，特別著墨於低壓鄰近蒸鍍法(LPPET)，期盼藉由達到節省生產能源及兼容可撓性基板應用的方法，並改良製程技術以增進元件之光電轉換效率，進一步達成產業化的目標。
氧化鋅由於具有良好的電子傳輸能力及光穿透率，在高分子太陽能電池中廣被使用。本研究首先以溶液製程成長氧化鋅薄膜，並使用簡單的二步驟製程，在氧化鋅基板上成長CH3NH3PbI3，且利用調變二步驟製程的濃度參數、氧化鋅層的架構來提升元件效率。並修正了實驗室標準製程中ZnO溶液的濃度可使鈣鈦礦層成長較佳，成功將元件轉換效率提升至13.44 %。
由於鈣鈦礦的生長過程中非常容易受環境中水氧的影響，再加上鈣鈦礦層的形成若太快會導致晶粒小且雜亂，使介面接觸不好影響載子傳輸。因此我們利用溶液製程搭配低壓鄰近蒸鍍法(LPPET)，加上傳統熱蒸鍍機蒸鍍PbI2來製備順置結構鈣鈦礦太陽能電池。這樣的製程具有的優勢包括較慢速的方式來成長鈣鈦礦層，以形成較佳結晶，此外改善了倒置結構中的磁滯現象和ZnO熱穩定性不佳的問題。並透過嘗試(side方式)許多不同LPPET的參數，找到最佳元件光電轉換效率為11.29 %，及非常不錯的短路電流18.38 mA/cm2。
為改善低壓鄰近蒸鍍法不易使底層PbI2反應完全，且容易使表層MAI蒸鍍過量的現象，我們提出一個溶液製程搭配低壓鄰近蒸鍍法的應用，即製作MAI/ PbI2/MAI之三明治結構，使MAI和PbI2能夠反應完全，得到高品質的鈣鈦礦層。
接著更進一步優化低壓鄰近蒸鍍法的製程，在先前的元件結構中的電子傳輸修飾層PEI更換為BCP，此中介層能相當有效阻擋電洞，使電子更順利的傳輸。此外也將LPPET side的方式改用top方式來鍍製，增進了鈣鈦礦層的結晶。最重要的是，我們在三明治結構中加入了退火之步驟，尤其是PbI2之退火。大大地提升鈣鈦礦層的結晶性和緻密性。得到品質極佳的鈣鈦礦層，元件之光電轉換效率最高為15.52 %；Jsc為23.91 mA/cm2，及其他優異的電性。

Due to the development of technology and gradual depletion of fossil fuels, the energy issue has received wide attention in this century. Solar energy is one of the best choices. Among many types of solar cells, perovskite solar cells suddenly appear on the horizon and the power conversion efficiency has been improved from 3 % to over 20 % in just 6 years. This makes many scholars who originally study in polymer and dye-sensitized solar cells start doing research about perovskite PVs.
Halide perovskites have recently emerged as promising materials because of low-cost and high-efficiency. In this study, we develop a new method, Low Pressure Proximity Evaporation Technique (LPPET), combined with Solution Process (SP) to fabricate planar sandwich-like perovskite thin films. We also optimize the methods to improve the power conversion efficiency of the devices.
Zinc oxide is widely used in polymer solar cells because of its good electron conductivity and high light transmittance. As a results, we first applied solution processed zinc oxide based on inverted-structure and a simple two-step solution process to fabricate perovskite PV cells. We modified the concentration of CH3NH3I solution to improve the efficiency. We analyzed the effect of interface morphology between perovskite and ZnO and finally, gained a PCE of 13.44 %.
Because two-step process is very susceptible to the atmosphere and the formation of perovskite is too quick that causes perovskite grains small and messy, we developed a new method, called Low Pressure Proximity Evaporation Technique (LPPET) to fabricate perovskite layer. At first, we investigate two layered perovskite devices. In order to achieve complete formation of the bottom PbI2 and avoid the excess deposition of MAI on surface, we bring up an idea of using solution process along with LPPET to form a sandwich structure of MAI/PbI2/MAI. However, due to poor thermal stability of the perovskite layer, we found the LPPET process is different to be exercised on ZnO substrate. With appropriate LPPET parameters, we got a PCE of 11.29 % and a very good short-circuit current density of 18.38 mA/cm2.
After that, we optimized LPPET process on traditional-structure perovskite PV devices. We found that the annealing step of sandwich-like perovskite layer is the most important factors to get best quality devices. The best crystallization and structure of perovskite could be obtained at 160℃, 35 minutes PbI2 annealing. Consequently, with adequate parameters of LPPET, we achieved efficiency of 15.52 % and large Jsc, 23.91 mA/cm2, also others good electric properties. For a low temperature process under whole atmosphere or under vacuum condition, this is a breakthrough of the perovskite solar cells and mass production.

目錄
論文審定書 ............................................................................................................................................. I
誌謝 ........................................................................................................................................................ II
中文摘要 .............................................................................................................................................. III
ABSTRACT ........................................................................................................................................ IV
目錄 ........................................................................................................................................................ V
第壹章 緒論 ........................................................................................................................................... 1
1.1 研究背景 .......................................................................................................................................... 1
1.1.1 科學與人類文明 ....................................................................................................................... 1
1.1.2 全世界能源與太陽能使用發展 ............................................................................................... 2
1.2 文獻回顧簡述 .................................................................................................................................. 4
1.2.1 太陽能電池之發現與演進歷程 ............................................................................................... 4
1.2.2 鈣鈦礦太陽能電池之崛貣與發展歷程 ................................................................................... 9
1.3 研究目的 ........................................................................................................................................ 13
第貳章 實驗原理簡介 .......................................................................................................................... 14
2.1 太陽能電池之基本原理 ................................................................................................................. 14
2.1.1 P-N接面 ................................................................................................................................. 14
2.1.2 光伏效應 ................................................................................................................................ 15
2.1.3 重要性能表徵 ......................................................................................................................... 16
2.2簡介鈣鈦礦太陽能電池 .................................................................................................................. 20
2.2.1鈣鈦礦太陽能電池之物理 ...................................................................................................... 20
2.2.2 鈣鈦礦太陽能電池之材料應用 ............................................................................................. 25
2.3製程技術簡述與文獻回顧 .............................................................................................................. 27
2.3.1 一步驟溶液製程法 (ONE-STEP SOLUTION PROCESS) ............................................................ 27
2.3.2 一步驟溶液製程法進化：溶劑及介面工程 (SOLVENT ENGINEEERING) .............................. 28
2.3.3 二步驟溶液製程法 (TWO-STEP SOLUTION PROCESS, TSP) .................................................... 29
2.3.4 二步驟溶液製程法進化：介面擴散法 (INTERDIFFUSION) ................................................... 30
2.3.5 二步驟溶液製程法進化：蒸汽輔助溶液製程 (VASP) ....................................................... 32
2.3.6 二步驟溶液製程法進化：熱蒸鍍法 (THERMAL EVAPORATION) ......................................... 32
2.3.7 二步驟溶液製程法進化：低壓鄰近蒸鍍法 (LPPET) ......................................................... 33
vi
第叁章 實驗設備與流程簡介 .............................................................................................................. 35
3.1 製程設備 ........................................................................................................................................ 35
3.1.1 手套箱 .................................................................................................................................... 35
3.1.2 旋轉塗布機與加熱盤 ............................................................................................................. 36
3.1.3 熱蒸鍍機 ................................................................................................................................ 36
3.1.4 低壓鄰近蒸鍍法 (LPPET) ..................................................................................................... 37
3.2 量測設備 ........................................................................................................................................ 38
3.2.1 太陽能模擬器 ......................................................................................................................... 38
3.2.2 X光繞射儀 (XRD) ................................................................................................................. 39
3.2.3 場發射掃描式電子顯微鏡 (FE-SEM) ................................................................................... 40
3.2.4 外部量子效應 (EQE) ............................................................................................................. 41
3.3 實驗流程 ........................................................................................................................................ 42
3.3.1 基板清洗與表面處理 ............................................................................................................. 42
3.3.2 電(子/洞)傳輸層旋塗 ............................................................................................................. 42
3.3.3 鈣鈦礦層製作 ......................................................................................................................... 43
3.3.4 電(洞/子)傳輸層旋塗 ............................................................................................................. 43
3.3.5 蒸鍍電極 ................................................................................................................................ 43
第肆章 以二步驟溶液製程法製備倒置結構鈣鈦礦太陽能電池 ....................................................... 44
4.1 研究動機 ........................................................................................................................................ 44
4.2 實驗設計 ........................................................................................................................................ 45
4.2.1 藥品配置 ................................................................................................................................ 46
4.2.2 元件製程 ................................................................................................................................ 49
4.3 結果與討論 .................................................................................................................................... 50
4.3.1 低成本電洞傳輸層應用於二步驟溶液製程之元件特性比較.............................................. 50
4.3.2 不同濃度的氧化鋅溶液元件比較 ......................................................................................... 52
4.3.3 使用不同基板之元件比較 ..................................................................................................... 54
4.4 小結 ................................................................................................................................................ 55
第伍章 以低壓鄰近蒸鍍法製備順置結構鈣鈦礦太陽能電池........................................................... 57
5.1 研究動機 ........................................................................................................................................ 57
5.2 實驗設計 ........................................................................................................................................ 57
5.2.1 藥品配置 ................................................................................................................................ 58
5.2.2 元件製程 ................................................................................................................................ 59
vii
5.3 結果與討論 .................................................................................................................................... 62
5.3.1 雙層結構之鈣鈦礦太陽能電池 ............................................................................................. 62
5.3.2 三明治鈣鈦礦結構中的碘化鉛膜厚效應 ............................................................................. 63
5.3.3 低壓鄰近蒸鍍法之溫度與時間效應 ..................................................................................... 66
5.3.4 使用不同前驅物(MAI, MACL)之元件晶體結構特性比較 .................................................. 68
5.4 小結 ................................................................................................................................................ 68
第陸章 溶液製程結合低壓鄰近蒸鍍法之優化與元件特性表現分析 ............................................... 69
6.1 研究動機 ........................................................................................................................................ 69
6.2 實驗設計 ........................................................................................................................................ 69
6.2.1 藥品配置 ................................................................................................................................ 70
6.2.2 元件製程 ................................................................................................................................ 71
6.3 結果與討論 .................................................................................................................................... 74
6.3.1製程優化後之溫度與時間效應 .............................................................................................. 75
6.3.2低壓鄰近蒸鍍法之不同蒸鍍方式之元件特性比較 .............................................................. 84
6.4 小結 ................................................................................................................................................ 85
第柒章 結論與未來展望 ...................................................................................................................... 86
7.1 結論 ................................................................................................................................................ 86
7.2 未來展望 ........................................................................................................................................ 87
第捌章 附錄 ......................................................................................................................................... 89
8.1三明治結構中PBI2的退火效應 ..................................................................................................... 89
8.2三明治結構中PBI2的厚度效應 ..................................................................................................... 92
REFERENCES .................................................................................................................................... 94

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