本篇論文研究應用於真空蒸鍍銫基鈣鈦礦主動層之元素組成與製備方式對元件表現的影響。
第一章，簡介太陽能電池的發展歷史，並回顧染料敏化太陽能電池、有機太陽能電池與鈣鈦礦太陽能電池的發展過程與現況。
第二章，概述鈣鈦礦太陽能電池之工作原理、光電特性、元件結構、特性分析、元件製備與量測。
第三章，我們以真空共蒸鍍製程作來製備鈣鈦礦主動層，透過調變銫基鉛鈣鈦礦的元素組成，觀察其對於元件表現之影響。CsPbI2Br參雜少量CsCl時，最佳元件表現為短路電流密度14.6 mA/cm2，開路電壓1.13 V，填充因子0.75，元件光電轉換效率12.2%。CsPbI2Br參雜少量ZnI2時，最佳元件表現為短路電流密度15.1 mA /cm2，開路電壓1.14 V，填充因子0.71，元件光電轉換效率12.2%。參雜CsCl與ZnI2均對CsPbI2Br元件表現無顯著提升。以CsPbI2.5Br0.5作為主動層時，最佳元件表現為短路電流密度16.2 mA/cm2，開路電壓1.15 V，填充因子0.61，元件光電轉換效率11.3%。以CsPbBr3作為主動層時，在反結構元件中有最佳表現，其短路電流密度為5.96 mA/cm2，開路電壓為1.01 V，填充因子為0.55，元件光電轉換效率為3.3%。
第四章，我們選用CsBr與SnI2為前驅物，藉由真空共蒸鍍製程製備CsSnI2Br，搭配4,4′-Cyclohexylidenebis[N,N-bis(4-methylphenyl)benzenamine] (TAPC) 與 4,4′,4′′-Tris[2-naphthyl(phenyl)amino] triphenylamine (2T-NATA) 作為電洞傳輸材料，探討其對於元件表現之影響。其中，以2T-NATA作為電洞傳輸層時元件有最佳表現，短路電流密度為8.32 mA/cm2，開路電壓為0.4 V，填充因子為0.4，元件光電轉換效率為1.36%。
第五章，我們以交替型真空蒸鍍製程製備CsPbI2Br，探討相同厚度下，不同層數之CsBr與PbI2薄膜特性與其對於元件表現的影響。其中以類磊晶之660-pair CsPbI2Br有最佳元件表現，在優化C60電子傳輸層厚度後，最佳元件之短路電流密度為15.6 mA/cm2，開路電壓為1.13 V，填充因子為0.74，能量轉換效率達13%。該元件在有封裝且存放於氮氣環境的狀態下，經90天後仍保有原先96%之效率，具有優異的元件穩定度。我們也以螢光燈做為量測光源，量測不同室內光強度下的元件表現，元件於1000 lux時擁有達33.9%的轉換效率。

In this thesis, we studied the vacuum deposited Cs-based perovskite active layers for solar cell applications.
In the first part of this thesis, we briefly reviewed the development of photovoltaics, dye-sensitized solar cells, organic solar cells and perovskite solar cells.
In the second part of thesis, we explicated the operation principle and characteristics of perovskite solar cells, followed by details of device structures, materials analyses, device fabrication and characteristics measurements.
In the third part of thesis, we prepared cesium-based lead perovskites by vacuum co-evaporation process with different element compositions. The device doped with CsCl in CsPbI2Br active layer exhibited highest power conversion efficiency (PCE) of 12.2%, with a short-circuit current density (Jsc) of 14.6 mA/cm2, an open-circuit voltage (VOC) of 1.13 V, and a fill factor (F.F.) of 0.75. And the device doped with ZnI2 in CsPbI2Br active layer exhibited highest PCE of 12.2%, with a Jsc of 15.1 mA/cm2, a VOC of 1.14 V, and a F.F. of 0.71. There were no obvious improvements by doping CsCl and ZnI2 in the CsPbI2Br thin film. The highest device PCE of CsPbI2.5Br0.5 was 11.3%, with a Jsc of 16.2 mA/cm2, a VOC of 1.15 V, and a F.F. of 0.61. When CsPbBr3 was used as an active layer, the n-i-p inverted structure device exhibited highest PCE of 3.3%, with a Jsc of 5.96 mA/cm2, a VOC of 1.01 V, and a F.F. of 0.55.
In the fourth part of thesis, we selected CsBr and SnI2 as precursors and fabricated CsSnI2Br thin film by vacuum co-evaporation deposition. By optimizing the hole transporting materials, the device using 2T-NATA as a hole transporting layer delivered the highest PCE of 1.36%, with a Jsc of 8.32 mA/cm2, a VOC of 0.4 V, and a F.F. of 0.4.
In the fifth part of thesis, we used alternative deposition method to fabricate CsPbI2Br thin film and evaluated the effect of CsBr and PbI2 pair number on the device performance. The 660-pair CsPbI2Br solar cell with a 15-nm C60 electron transporting layer showed the highest PCE of 13.0%, with an VOC, JSC, and F.F. of 1.13 V, 15.6 mA.cm−2, and 0.74, respectively. The encapsulated device maintained 96% of its efficiency after 90 days. Furthermore, the use of these devices for environmental light energy harvesting was validated by a PCE of 33.9% under 1000 lux fluorescent light illumination.

摘要 I
Abstract III
致謝 V
目錄 VI
圖目錄 IX
表目錄 XIII
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 3
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 染料敏化太陽能電池發展 5
1-4 有機薄膜太陽能電池發展 5
1-5 鈣鈦礦太陽能電池發展 6
1-6 論文結構 10
Chapter 2 鈣鈦礦太陽能電池之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 鈣鈦礦太陽能電池之工作原理 13
2-4 鈣鈦礦太陽能電池之光電特性 13
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) 14
2-4.3 短路電流密度 (short circuit current density, JSC) 14
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.) 15
2-5 鈣鈦礦太陽能電池之元件結構 16
2-6 鈣鈦礦太陽能電池之特性分析、製備與量測 17
2-6.1 材料的光物理性質量測 17
2-6.2 元件製備 18
2-6.3 元件量測 19
Chapter 3 真空蒸鍍銫基鉛鈣鈦礦作為主動層於光伏元件之應用 20
3-1 銫基鈣鈦礦太陽能電池簡介與發展 20
3-2 CsPbI2Br參雜金屬鹵化物之元件製備 22
3-2.1 CsPbI2Br標準元件製備 22
3-2.2 CsPbI2Br參雜CsCl之元件製備 25
3-2.3 CsPbI2Br參雜ZnI2之元件製備 29
3-3 CsPbI2.5Br0.5元件製備 34
3-4 CsPbBr3薄膜製備與分析 38
3-5 CsPbBr3元件製備 43
3-5.1 CsPbBr3正結構元件製備 43
3-5.2 CsPbBr3反結構元件製備 47
3-6 不同元素組成之銫基鉛鈣鈦礦元件表現之比較 50
3-7 結論 52
Chapter 4 真空蒸鍍銫基錫鈣鈦礦作為主動層於光伏元件之應用 54
4-1 錫鈣鈦礦太陽能電池簡介與發展 54
4-2 CsSnI2Br薄膜製備與分析 56
4-3 CsSnI2Br元件製備 59
4-4 結論 67
Chapter 5 交替型真空蒸鍍製程應用於銫基鈣鈦礦太陽能電池 68
5-1 交替型真空蒸鍍製程簡介 68
5-2 不同層數之CsPbI2Br薄膜製備 70
5-3 不同層數之CsPbI2Br元件製備 75
5-3.1 4-pair CsPbI2Br 75
5-3.2 50-pair CsPbI2Br 78
5-3.3 660-pair CsPbI2Br 81
5-3.4 1560-pair CsPbI2Br 84
5-3.5 不同層數CsPbI2Br元件表現之比較 87
5-4 不同層數之CsPbI2Br薄膜分析 90
5-4.1 GIWAXS分析 90
5-4.2 SEM、EDS和AFM分析 92
5-5 類磊晶CsPbI2Br元件優化與量測 97
5-5.1 調變類磊晶CsPbI2Br元件之電子傳輸層厚度 97
5-5.2 室內光、穩定性量測 99
5-6 結論 104
Chapter 6 結論與未來展望 106
參考文獻 108

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