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系統識別號 U0026-1601202018565900
論文名稱(中文) 鹵化有機鉛鈣鈦礦電子元件研究
論文名稱(英文) Research of Organolead Halide Perovskite Electronic Devices
校院名稱 成功大學
系所名稱(中) 電機工程學系
系所名稱(英) Department of Electrical Engineering
學年度 108
學期 1
出版年 108
研究生(中文) 吳炫達
研究生(英文) Hsuan-Ta Wu
學號 N28004012
學位類別 博士
語文別 英文
論文頁數 75頁
口試委員 指導教授-施權峰
召集委員-尤正祺
口試委員-陳文序
口試委員-許正興
口試委員-李偉民
口試委員-呂正傑
口試委員-陳逸謙
口試委員-黃正亮
中文關鍵字 有機鈣鈦礦  鈣鈦礦太陽電池  鈣鈦礦電阻式記憶體  缺陷 
英文關鍵字 Organic perovskite  Perovskite solar cells  Perovskite resistive random-access memory  Defects 
學科別分類
中文摘要 近十年來鹵化有機鉛鈣鈦礦應用於太陽電池上已從2009年的3.8%躍升至2019年的25.2%,其具有可調與良好的光電特性、多變但低溫非真空的製程手法與較差的水氧抗性,使其在學術與商業應用方面都具有研究的價值,本論文研究以鹵化有機鉛鈣鈦礦為主要材料的太陽電池與電阻式記憶體。
本研究同時摻雜水與鹵化鉀於鈣鈦礦前驅物碘化鉛溶液時,鈣鈦礦薄膜表面並無明顯變化,但在光電轉換效率上可增加開路電壓、短路電流與填充因子,使得效率提升。透過光致發光量測可看出純粹摻雜碘化鉀或氯化鉀可有效改善薄膜或界面中的非輻射復合缺陷,而從歐傑電子能譜縱深分析可以看到鉀訊號滲透至電洞傳輸層與電子傳輸層,與前述分析比較後可認定鉀離子對界面改善後增進了鈣鈦礦太陽電池的效率。本研究也摻雜碘化鉀於電阻式記憶體,適當的碘化鉀摻雜可使記憶體切換次數增加與保存特性穩定,過多的碘化鉀摻雜明顯使得薄膜產生孔洞並使得記憶體元件表現不佳,而光致發光與X光繞射分析一致可以看出碘化鉀摻雜主要增進鈣鈦礦薄膜的結晶度,X光電子能譜縱深分析則指出鉀離子主要作用於PEDOT:PSS/MAPbI3界面處,而缺陷減少可使電阻式記憶體內的通路不易永久性地斷路或短路。為使鈣鈦礦中缺陷更少,高指向性與大晶粒的鈣鈦礦薄膜是有可能的研究方向,本研究先以化學浴法沉積具空隙的硫化鉛晶粒,再與碘片一同加熱形成片狀晶粒的碘化鉛薄膜,最後與碘化甲基胺一起退火後得到高指向性與大晶粒的鈣鈦礦膜,與相似厚度的兩步法鈣鈦礦膜相比記憶體元件電阻開關比例稍高,但硫化鉛法的操作電流低了103倍,代表更低的功耗與更長的壽命。
綜上所述本研究以鹵化鉀摻雜與成長高指向性有機鹵化鉛鈣鈦礦薄膜修復了鈣鈦礦薄膜與其界面中的缺陷,使其在電子元件上有較佳的應用。
英文摘要 In the past ten years, the efficiency of organolead halide perovskite solar cells has jumped from 3.8% in 2009 to 25.2% in 2019. It has adjustable and good optoelectronic properties, variable but low temperature non-vacuum process and poor water-oxygen resistance. These properties make organolead halide perovskite of research value in both academic and commercial applications. This thesis studies solar cells and resistive memory made by organolead halide perovskite as the main material.
When water and potassium halide simultaneously doped in the perovskite precursor lead iodide solution of two-step method, there is no significant change in the surface of the perovskite film, but the photovoltaic conversion efficiency(PCE) increased caused by open-circuit voltage(VOC), short-circuit current(ISC) and fill factor(FF) increased. Through photoluminescence(PL) measurement, it can be seen that doping of only potassium iodide or potassium chloride can effectively improve the non-radiative recombination defects in the film or interface. From Auger electron spectroscopy(AES) depth analysis, it can be seen that the potassium signal penetrates into the hole transport layer and the electron transport layer. Compared with the above analysis, it can be confirmed that the potassium ion improves the efficiency of the perovskite solar cell after improving the interface. Potassium iodide was also doped in the perovskite resistive memory of ITO/PEDOT:PSS/MAPbI3/PMMA/Al structure. Appropriate potassium iodide doping can increase cycle endurance and retention time. Excessive potassium iodide doping made the film pores and damaged memory characteristics. It can be seen that the potassium iodide doping mainly enhances the crystallinity of the perovskite film from consistent PL and X-ray diffraction(XRD) analysis. X-ray photoelectron spectrum(XPS) depth analysis indicated that the potassium ions mainly act on the PEDOT:PSS/MAPbI3 interface, and the reduction in defects makes devices difficult to be permanently opened or shorted for the path in the resistive memory.
In order to make less defects in the perovskite film, high preferring orientation and large-grain perovskite film is a possible research direction. Three-step method was applied to make perovskite film. First, voided lead sulfide grains were deposited by chemical bath method. And then flaky lead iodide grains were formed after heating with the iodine sheet. Finally, after annealing with methylammonium iodide(MAI), a high preferring orientation and large-grain perovskite film was obtained. Comparing with perovskite film of similar thickness made by two-step method, the memory on/off ratio is slightly higher, but the operating current is 103 times lower by lead sulfide method. It represented lower power consumption and longer lifetime.
In summary, this study uses doped potassium halide and high preferring orientation organolead halide perovskite film to repair defects in the film and its interface of layers, making it a better application in electronic components.
論文目次 List of publications I
摘要 III
Abstract IV
致謝 VI
Contents VII
Table caption IX
Figure caption X
Chapter 1 Introduction 1
1-1 Organic perovskite 1
1-2 Perovskite solar cell 3
1-3 Process of organic perovskite film 5
1-4 Perovskite resistive memory 7
Chapter 2 Effect of co-doping water and potassium halide into perovskite solar cells 9
2-1 Preface 9
2-2 Experimental Section 11
2-3 Result and Discussion 13
2-4 Summary 22
2-5 Supporting Information 24
Chapter 3 Resistive memory properties of perovskite device doped with potassium iodide 32
3-1 Preface 32
3-2 Experimental Section 34
3-3 Result and Discussion 35
3-4 Summary 44
Chapter 4 PbS-buffered three-step growth method improve memory properties of perovskite device 45
4-1 Preface 45
4-2 Experimental Section 46
4-2-1 PbS-buffering process 47
4-2-2 Spin-coating process 47
4-2-3 Fabrication of RRAM device 48
4-2-4 Sample characterization 48
4-3 Result and Discussion 49
4-4 Summary 61
4-5 Supporting Information 62
Chapter 5 Conclusions 67
Reference 69
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