本篇論文研究應用於有機金屬鈣鈦礦太陽能電池之電荷傳輸層，與作為主動層應用於光伏元件之無含鉛材料之開發及探討。
第一章中，簡介太陽能電池之發展歷程，並回顧有機太陽能電池、染料敏化太陽能電池與有機金屬鈣鈦礦太陽能電池過去至今發展進程與現況。
第二章中，概述有機金屬鈣鈦礦太陽能電池之運作原理及光電特性，並接著介紹元件結構、元件製備與元件量測。
第三章中，我嘗試以代換、搭配或摻雜之方法製備應用於正、反結構元件中之載子傳輸層來改善以濕式製程與真空製程製備之鈣鈦礦太陽能電池效率。其中以優化之Ca與C60搭配作為反結構元件之電子傳輸層，成功應用於真空製程中，開發出具高再現性與高效率之全真空製程鈣鈦礦太陽能電池，經優化之最佳元件其短路電流密度(JSC) 為23.7 mA/cm2，開路電壓(VOC) 為1.04 V，填充因子(F.F.) 為0.70，能量轉換效率(PCE) 達17.2%。
第四章中，我使用真空製程製備包含鈣鈦礦與非鈣鈦礦結構之鉍基材料，並初步量測其基本性質。接著將鉍基材料作為光伏主動層分別應用於正、反結構元件之中，依能階位置選擇不同載子傳輸層搭配，並比較對元件表現之影響。目前優化厚度與退火條件之最佳鉍基鈣鈦礦太陽能元件其JSC為0.35 mA/cm2，VOC為0.74 V，F.F.為0.27，PCE為0.07%。
第五章中，我分別以真空製程與濕式製程嘗試製備錫基鈣鈦礦薄膜，並對其進行基本性質量測、元素分析與表面形貌分析。使用真空製程得以製備高覆蓋率，表面形貌均勻之錫基鈣鈦礦薄膜，經優化反應與前驅物厚度條件，最佳元件其JSC為5.12 mA/cm2，VOC為0.55 V，F.F.為0.39，PCE達1.09%。

In this thesis, I studied the charge carrier transporting layers of the organometallic perovskite solar cells and the photovoltaics with lead-free active layers.
In the first chapter, I briefly reviewed the development of modern photovoltaics including organic solar cells, dye-sensitized solar cells and organometallic perovskite solar cells.
In the second chapter, the operation principle and photovoltaic characteristics of organometallic perovskite solar cells were described. Then, the structures of the devices, device fabrication methods and device characteristics measurement were comprehensively introduced.
In the third chapter, to improve the power conversion efficiency of the solution-processed and vacuum deposited organometallic perovskite solar cells, I optimized the properties of charge carrier transporting layers used in the normal or inverted device structures through material composition tuning, device layer structure design and condutive doping. With optimized Ca/C60 bi-layer structure as electron transporting layers, I successfully developed highly efficient and highly reproducible vacuum deposited organometallic perovskite solar cells. The best device power conversion efficiency was as high as 17.2%, with a short circuit current density (JSC) of 23.7 mA/cm2, an open circuit voltage (VOC) of 1.04 V, and a fill factor (F.F.) of 0.70.
In the fourth chapter, I prepared bismuth-based materials with perovskite or non-perovskite crystal structure by the vacuum deposition and proceeded various characteristics measurements. I fabricated the devices with the normal and inverted structures by utilizing these bismuth-based materials. I also chosed charge carrier transporting layers with proper energy levels to pair with these bismuth-based solar-active layers. With the optimized active layer thicknesses and annealing conditions, the best device power conversion efficiency of the bismuth-based perovskite solar cell was 0.07%, with a JSC of 0.35 mA/cm2, VOC of 0.74 V, and F.F. of 0.27.
In the last chapter, I prepared tin-based perovskite thin films by solution process and sequential vacuum deposition and investigate their characteristics including material compositions and thin-film morphologies. By using the sequential vacuum deposition and optimizing the process conditions, homogeneous and smooth tin-based perovskite thin films could be obtained. The best device power conversion efficiency was 1.09%, with a JSC of 5.12 mA/cm2, VOC of 0.55 V, and F.F. of 0.39.

目錄
摘要 I
Abstract II
目錄 V
圖目錄 IX
表目錄 XV
Chapter 1　序論 1
1-1　前言 1
1-2　太陽能電池發展簡介 2
1-2.1　第一代太陽能電池 2
1-2.2　第二代太陽能電池 3
1-2.3　第三代太陽能電池 4
1-3有機太陽能電池發展 4
1-4染料敏化太陽能電池發展 5
1-5有機金屬鈣鈦礦太陽能電池發展 6
1-6論文結構 9
Chapter 2　有機太陽能電池工作原理與特性量測 11
2-1　簡介 11
2-2　太陽光光譜 11
2-3　太陽能電池工作原理 12
2-4　有機金屬鈣鈦礦太陽能電池之光電特性 12
2-4.1　能量轉換效率 (power conversion efficiency, PCE) 13
2-4.2　開路電壓 (open circuit voltage, VOC) 13
2-4.3　短路電流密度 (short circuit current density, JSC) 13
2-4.4　填充因子 (fill factor, F.F.) 14
2-4.5　外部量子效率 (external quantum efficiency, E.Q.E.) 14
2-5　有機金屬鈣鈦礦太陽能電池元件之結構 15
2-5.1　依載子傳遞方向分類 15
2-5.2　依元件型態分類 15
2-6　有機金屬鈣鈦礦太陽能電池之分析、元件量測與製備 15
2-6.1 有機材料之純化 15
2-6.2　材料之光物理性質量測 15
2-6.3　元件製備 17
2-6.4　元件量測 18
Chapter3應用於鈣鈦礦太陽能電池之載子傳輸層 22
3-1鈣鈦礦太陽能電池傳輸層簡介與發展 22
3-1.1正結構元件之電洞傳輸層 22
3-1.2正結構元件之電子傳輸層 24
3-1.3反結構元件之電洞傳輸層 26
3-1.3反結構元件之電子傳輸層 29
3-2濕式鈣鈦礦太陽能電池之傳輸層 31
3-2.1搭配不同型號PEDOT:PSS之應用 31
3-2.2搭配不同富勒烯與其衍生物之應用 32
3-2.3導電摻雜對電子傳輸層之改質應用 34
3-3真空蒸鍍製程鈣鈦礦太陽能電池傳輸層 36
3-3.1正結構元件之開發 36
3-3.2反結構元件之開發 37
3-3.3調變電子傳輸層應用於反結構元件 38
3-3.4調變反結構元件之PbI2厚度 39
3-3.5調增鈣鈦礦薄膜厚度 40
3-4結論 42
Chapter4 鉍化物作為主動層於光伏元件之應用 65
4-1簡介與發展 65
4-1.1鈣鈦礦結構吸光材料 65
4-1.2雙重鈣鈦礦結構吸光材料 66
4-1.3非鈣鈦礦結構吸光材料 67
4-2以真空製程製備鉍化物主動層薄膜 67
4-2.1有機鉍鈣鈦礦薄膜 67
4-2.2無機鉍鈣鈦礦薄膜 69
4-2.3非鈣鈦礦材料薄膜 69
4-3鉍化物主動層於光伏元件之應用 70
4-3.1有機鉍鈣鈦礦光伏元件 70
4-3.2無機鉍鈣鈦礦光伏元件 72
4-3.3非鈣鈦礦主動層光伏元件 74
4-4結論 76
Chapter5 錫鈣鈦礦作為主動層於光伏元件之應用 96
5-1簡介與發展 96
5-2錫鈣鈦礦薄膜製備 98
5-3兩階段製程錫鈣鈦礦薄膜於元件之應用 100
5-3.1調變鈣鈦礦反應溫度與厚度 100
5-3.2錫鈣鈦礦薄膜分析 101
5-3.3還原劑之摻雜 102
5-4由濕式製程碘化錫反應之錫鈣鈦礦 105
5-4.1錫鈣鈦礦薄膜之製備 105
5-4.2由濕式製程碘化錫反應之錫鈣鈦礦元件 106
5-5結論 108
Chapter 6　未來展望 125
參考文獻 126

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