鹵化有機金屬鈣鈦礦因具有相當優異的光吸收係數、載子壽命、電子與電動遷移率等特性，而受到了學術界的矚目，開始被應用於太陽能電池中，作為高效吸光層材料。但截至目前為止，幾乎所有的鈣鈦礦太陽能電池中的鈣鈦礦材料皆屬多晶薄膜，其晶界容易導致載子的再結合，是影響其光電轉換效率與元件穩定性的瓶頸之一。相較於多晶薄膜，單晶鈣鈦礦因晶界與表面缺陷相當稀少，因此具有更優異的光電性質與穩定性，若能以其作為光吸收層將有機會獲得更高的光電轉換效率。
但目前研究最廣泛的鈣鈦礦MAPbI3由於陽離子MA+平均半徑值較小而導致晶體成為不穩定的扭曲結構，水氣等外在因子容易造成晶體結構的瓦解。因此為了同時解決多晶MAPbI3晶界導致載子再結合和MAPbI3材料不穩定的問題，本研究利用升溫析晶法在溶液中合成出不同FA+((NH2)2CH+)/MA+比例的單晶混合陽離子鈣鈦礦FAXMA(1-X)PbI3，並利用多種儀器進行性質分析，我們發現當單晶FAXMA(1-X)PbI3對於濕度有較好的穩定性，代表其更適合做為長效鈣鈦礦太陽能電池中的吸光材料。
另外，溶液中合成出的單晶鈣鈦礦因為厚度的因素限制了其應用光伏元件的發展性，為了取得單晶鈣鈦礦薄片，本研究另設計出可以簡易合成厚度為0.17mm單晶MAPbI3 wafer的培養槽。並結合FAXMA(1-X)PbI3前驅液與wafer培養槽，合成單晶FAXMA(1-X)PbI3 wafer並量測其電性，並與MAPbI3做比較。

The organic-inorganic hybrid perovskites have been receiving considerable attention in various optoelectronic applications due to its superior characteristics including high absorption coefficient, direct bandgap, long carrier lifetime, and high hole and electron mobility. However, current perovskite solar cells are all based on polycrystalline perovskite thin films, which contain plenty of grain boundaries and surface defects, rendering noticeable carrier loss and device instability. It was reported that single crystalline perovskite possesses superior optoelectronic properties and stability due to less grain boundaries and surface defects.
However, the widely explored MAPbI3 is still unstable due to its distorted crystal structure caused by small MA+ ions. It was found that the crystal structure is weak against moisture. Herein we added formamidinium ions (FA+) ions in the MA+ incubation solution and successfully synthesized MAXFA(1-X)PbI3 single crystal by means of inverse temperature crystallization. We examined the mixed cation single crystals by several instruments and found they possess better stability under high humidity.
In addition, the applications on MSCs are limited by the thickness of crystals. Herein, we designed a incubating tank to synthesize large area MAPbI3 wafer with 0.17mm in thickness. We also synthesized MAXFA(1-X)PbI3 wafer and measured its electrical properties comparing to MAPbI3.

第一章 緒論 1
1-1前言 1
第二章 文獻回顧 5
2-1鈣鈦礦太陽能電池 5
2-1-1鈣鈦礦 5
2-1-2鈣鈦礦太陽能電池結構與發展 6
2-2 單晶鈣鈦礦 7
2-2-1單晶鈣鈦礦和多晶薄膜性質差異 7
2-2-2 合成方法 12
2-2-3 升溫析晶法合成MAPbI3的反應機制 17
2-3混合陽離子鈣鈦礦 19
2-3-1 環境對MAPbI3的影響 19
2-3-2 混合陽離子鈣鈦礦FAXMA(1-X)PbI3的性質 21
2-4 單晶鈣鈦礦薄片 27
2-5 研究動機 33
第三章 實驗方法與儀器分析 34
3-1設備與儀器 34
3-2儀器與分析原理 35
3-2-1 X光繞射光譜儀(X-ray diffraction) 35
3-2-2 熱重量分析儀（Thermogravimetric analyzer） 36
3-2-3紫外光/可見光光譜儀（Ultraviolet-visible spectroscopy） 37
3-2-4 光激發螢光(Photoluminescence) 38
3-2-5 動態光散射儀(Dynamic light scattering) 39
3-2-6 空間電荷限制電流(space charge limit current, SCLC) 40
3-2-7 I-V特性曲線（I-V curve） 41
3-2-8 掃描電子顯微鏡（Scanning electron microscopy，SEM） 44
3-4 藥品與材料 45
3-5 甲基碘化銨的合成方法 45
3-5-1 甲基碘化銨合成 45
3-5-2 甲基碘化銨純化 46
3-6 單晶鈣鈦礦的合成方法 46
3-6-1 合成單晶MAPbI3方法 46
3-6-2 合成單晶FAPbI3方法 47
3-6-3 合成單晶FAXMA(1-X)PbI3方法 47
3-7 單晶鈣鈦礦濕度測試環境的製造 48
3-8 合成單晶MAPbI3薄片之長晶槽設計 48
3-8-1合成單晶FA0.6MA0.4PbI3薄片方法 49
3-9 測試鈣鈦礦前驅物在狹縫中擴散速率的裝置設計 50
3-10 單晶MAPbI3元件設計 50
第四章 結果與探討 52
4-1 升溫析晶法長晶機制之探討 52
4-2 混合陽離子FAXMA(1-X)PbI3鈣鈦礦的性質分析 55
4-2-1 結構分析 55
4-2-2 光學分析 56
4-2-3 熱穩定性 57
4-2-4 對水穩定性 58
4-3 單晶鈣鈦礦薄片 62
4-3-1 單晶MAPbI3 薄片的合成 62
4-3-2 單晶FA0.6MA0.4PbI3薄片的合成 63
4-3-3 單晶鈣鈦礦薄片的XRD分析 65
4-3-4 量測單晶鈣鈦礦薄片的電性 66
4-3-5 單晶MAPbI3太陽能電池的量測 70
第五章 結論 72
第六章 參考文獻 74

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