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系統識別號 U0026-2907201917124400
論文名稱(中文) 銅/氧化亞銅複合薄膜應用於先進鈣鈦礦太陽能電池及光偵測器之研究
論文名稱(英文) Cu/Cu2O composite films for novel perovskite solar cells and photodetectors
校院名稱 成功大學
系所名稱(中) 光電科學與工程學系
系所名稱(英) Department of Photonics
學年度 107
學期 2
出版年 108
研究生(中文) 陳宥駿
研究生(英文) You-Jyun Chen
學號 L78991186
學位類別 博士
語文別 英文
論文頁數 101頁
口試委員 指導教授-黃榮俊
召集委員-賴韋志
口試委員-陳昭宇
口試委員-傅耀賢
口試委員-曾百亨
中文關鍵字 鈣鈦礦  氧化亞銅  太陽能電池  光偵測器 
英文關鍵字 perovskite  Cu2O  solar cell  photodetector 
學科別分類
中文摘要 近年來,能源議題爭論不斷,從廢核到全民公投的「以核養綠」通過,人們漸漸意識到能源的重要性,再也不要“用愛發電”。根據台灣電力公司公布:107年台灣發電量結構以燃油+燃氣+燃煤超過80%的火力發電為主,核能11.4%為輔,其他再生、抽蓄、汽電能源還供給不到9%,說明了整體發電的形式依舊偏向對環境有負面的影響。隨著人們的環保意識抬頭,火力發電會造成空污問題,核能核廢料丟棄存放地點的設置已成為民意與政策互相角力辯論的議題,世界各國積極研發使用潔淨的再生能源,希望能以最積極的腳步減輕和解決傳統發電所產生的汙染問題,以綠色能源取代更多的燃煤、核能發電。綠能發電常見的有:太陽能、風力、水力以及生質能源發電,而太陽能又以鈣鈦礦太陽能電池在短短數年期間非常快速地成長,已由最初的3.8%提升至24.2%以上,被視為具有能與結晶矽太陽能電池競爭的潛力股。然而,由於鈣鈦礦本質上的缺陷,易受外在環境影響以及金屬電極的化學反應使得穩定性異常得差。
如何改善穩定性?首先想到的就是找出最佳化鈣鈦礦的組成工程,這方法雖然很有用卻也非常費工夫,然而目前文獻最佳化的鈣鈦礦組成的壽命仍舊難以與能存放50年以上的結晶Si抗衡。另一方面,將適當的載子傳輸層和電極結合到鈣鈦礦太陽能電池中也被認為是維持穩定性以及增加光電轉換效率的有效方法。
因此本論文研究無機電洞傳輸材料Cu/Cu2O對於鈣鈦礦太陽能電池的影響以期改善穩定性和增強光電轉換效率。經由霍爾量測確認在通氧量40%以上沉積出來的膜屬於p-type半導體,且電洞遷移率也比有機電洞傳輸材料大上許多,因此第一部分使用高氧壓環境下成長的p型Cu/Cu2O和有機材料Spiro-OMeTAD作為n-i-p異質結構鈣鈦礦太陽能電池中的組合式電洞傳輸層,以改善電洞提取能力,元件性能和元件穩定性。
第二部分調控Cu/Cu2O的厚度找出電性和透光度最佳平衡點,期望作為透明電極取代金屬電極。對於雙面透光的鈣鈦礦太陽能電池已經實現14.1% (從FTO照光)和9.37% (從Cu/Cu2O照光)的光電轉換效率,開啟雙面透光元件結合太陽能窗應用於建築物整合太陽光電系統中的可能性。
第三部分光偵測器更是嘗試直接取代有機電洞傳輸材料和金屬電極,把Cu/Cu2O作為載子傳輸電極使用。這邊工作表明,鈣鈦礦/(Cu/Cu2O)異質結構光偵測器可以被認為是雙面照明和柔性/可穿戴光電技術應用的有希望的候選者。
英文摘要 In recent year, the energy issues have been arguing endlessly. From the stop nuclear power generation to the vote through on nuclear energy by referendum. People are gradually realizing the importance of energy and never want to use “ love ” to generate electricity. According to the announcement of the Taiwan Power Company, the power generation structure of Taiwan in 107 year is mainly based on thermal power generation with fuel, gas, and coal burning of more than 80%. Nuclear energy is 11.4%, and other renewable, pumping, and steam energy sources are still less than 9%. This shows that the form of overall power generation still has a negative impact on the environment. As people's awareness of environmental protection rises, thermal power generation will cause air pollution problems and the setting storage sites of nuclear wastes have become a topic of debate between public opinion and policy. Countries around the world are actively developing and using clean renewable energy. We hope to reduce and solve the pollution problems caused by traditional power generation in the most positive way, and replace thermal and nuclear power with green energy. Green energy power generation is commonly found in solar, wind, hydro, and biomass energy generation. While perovskite-based solar cells has grown very rapidly in just a few years, which power conversion efficiency (PCE) has increased from the initial 3.8% to more than 24.2%, it is considered to have great potential and can compete with crystal Si-based solar cells. However, due to the inherent defects of the perovskite, it is susceptible to the external environment and the chemical reaction of the metal electrode makes the poor stability.
How to improve stability? The first way is to optimize the composition of the perovskite. Although this method is very useful, it is also very laborious. On the other hand, incorporating proper carrier transport layers and electrodes into perovskite-based solar cells is also considered as effective ways to maintain device stability as well as the efficiency of perovskite-based solar cells. Therefore, this study researches the effect of inorganic hole transport material Cu/Cu2O on perovskite solar cells to expect stability improved as well as the PCE increased.
The first part uses the ion beam sputtering system to deposit the Cu/Cu2O composite films by adjusting the ratio of argon and oxygen. To keep the organic hole transport material Spiro-OMeTAD on the perovskite, the organic material acts as a buffer layer so that the deposition of Cu/Cu2O does not damage the light absorbing layer perovskite. The mobilities of Cu/Cu2O are at least three orders of magnitude higher than the organic hole transport layers of Spiro-OMeTAD. In addition to helping the hole transport, it also isolates the organic material from direct contact with the external atmosphere and the metal electrode, effectively improving device efficiency and long-term stability.
The second part controlled the composition and thickness, the transmission and conductivity of the Cu/Cu2O composite electrode have been optimized for efficient perovskite solar cells. PCEs of 14.10% and 9.37% have been achieved for the bifacial-illuminated perovskite-based solar cell when the one sun AM1.5G illumination is incident from the fluorine-doped tin oxide (FTO) side and Cu/Cu2O side, respectively. This result opens up the possibility for a bifacial-illuminated devices in combination with a power-generating window in the building-integrated photovoltaics.
The third part of the photodetector is to use a Cu/Cu2O as the carrier transfer electrode to directly replace the organic hole transport material and the metal electrode. This work reveals that the perovskite/(Cu/Cu2O) heterojunction photodetector a promising candidate for applications in bifacial-illuminated and flexible/wearable optoelectronic technologies.
論文目次 中文摘要 I
Abstract III
誌謝 VI
Table of Contents VIII
List of Tables X
List of Figures XI
Chapter 1 Introduction 1
1.1 Sun 1
1.2 What is solar cells? 2
1.3 Perovskite-based solar cell 4
1.4 Motivation and objectives 9
Chapter 2 Related theory and model 14
2.1 Air mass 14
2.2 Current-Voltage characteristics 15
2.3 Photodetector characteristics 17
Chapter 3 Experimental methods 18
3.1 Ion beam sputtering system 18
3.2 Pulsed laser deposition 20
3.3 Fabrication processes 23
3.4 Characterization and Measurement 25
Chapter 4 Cu/Cu2O nanocomposite films as a p-type modified layer for efficient perovskite solar cells 29
4.1 Introduction 29
4.2 Characterizations of the Cu/Cu2O composite films 31
4.3 Devices 39
4.4 Stability Test 43
4.5 Discussion 44
Chapter 5 Cu/Cu2O nanocomposite as a p-type transparent-conductive-oxide for efficient bifacial-illuminated perovskite solar cells 45
5.1 Introduction 45
5.2 Room temperature (~ 30 °C) processed Cu/Cu2O films 48
5.3 Bifacial-Illuminated Devices 54
5.4 Stability Test 61
5.5 Conclusions 62
Chapter 6 Double-side operable perovskite photodetector using Cu/Cu2O as a hole transport electrode 64
6.1 Introduction 64
6.2 Results and discussion 67
6.3 Double-side operable photodetector 73
6.4 Conclusions 81
Chapter 7 Research that has not been done 83
7.1 PLD grows CIGS solar material 83
Chapter 8 Conclusions and Future works 87
8.1 Conclusions and challenges 87
References 91
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