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研究生： 黃楷翔
Huang, Kai-Hsiang
論文名稱： 熱處理及溶液加工法合成調控雙銨基碳鏈陽離子之低維度鹵化物鈣鈦礦
Solvent Engineering of Low­-dimensional Halide Perovskite with Alkyldiammonium Cation via Heat Treatment
指導教授： 陳昭宇
Chen, Peter
學位類別： 碩士
Master
系所名稱： 理學院 - 光電科學與工程學系
Department of Photonics
論文出版年： 2021
畢業學年度： 109
語文別： 英文
論文頁數： 130
中文關鍵詞： 低維度 、Dion-Jacobson 相 、碳鏈 、乙二胺 、預熱 、鹵化物鈣鈦礦 、添加劑
外文關鍵詞： low-dimension, Dion-Jacobson phase, alkyl chain, ethylenediammonium, hot-casting, halide perovskite, additive
相關次數： 點閱：141  下載：0 
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    • 近年來，許多團隊致力於改善鈣鈦礦材料裡所發現的瓶頸，穩定性及元件表現為其中最大的兩個研究方向。三維結構會因親水性材料而與環境中水份相結合，產生令結構不穩定的非鈣鈦礦相，故以大尺寸陽離子置入結構中的二維鈣鈦礦，其層狀結構能因其中具疏水性的銨基，抵禦水分的破壞並使穩定性提升。但是，純二維結構因量子阱結構能隙過大，若製成太陽能元件，則會使電流密度大幅下降。由二、三維結構所合併的低維度鈣鈦礦，提高了無機層裡的八面體比例，能夠使載子傳輸更佳，而加入大尺寸陽離子的作用，能使低維度鈣鈦礦的結構有相當程度的疏水性。
    本研究探討具雙銨基的乙二胺及 FA0.9Cs0.1PbI3 三維鈣鈦礦之間的關係，以二/三維不同比例的鈣鈦礦，並利用旋塗前、旋塗後的熱處理來控制基板溫度，旨在研究不同的熱處理對於低維度鈣鈦礦的成長機制之影響。經低維度材料的吸收和放光特性，發現二維 EDAPbI4 的比例會隨著預熱基板溫度的提升而逐漸變少，三維比例的效應會更為明顯，說明量子阱的寬化。但是，從晶格繞射瞭解到二維結構僅是比例變低，仍然存在在薄膜裡，生長在薄膜更內層的位置，顯現低維度結構由薄膜表面開始往下成長，疏水性也因預熱溫度提升而變佳。鈣鈦礦結晶的方面，預熱溫度過高會使溶劑蒸發速度過快，成核初期速度過快，使晶體成長方向提早定型，最終薄膜觀察到成長無方向，且形貌也變得極不平整。然而，FACl 添加劑的加入，除了能改善薄膜的表面形貌，也能使結晶性提升、晶體方向性更單一，對於 DJ 相的低維度鈣鈦礦研究是不可或缺的要素。

    Recently, many researchers have made attempts to address the bottlenecks in fabrica­tion of perovskite materials, of which stability and device performance are two of the main objectives. Three-dimensional structures, whose hydrophilic composition consorts with the moisture, generate unstable non-­perovskite phases. Therefore, large-­size organic cations are intercalated within the structure to resist moisture based on their hydrophobic ammonium end. This helps promote the stability of perovskite, and has gain increasing recognition. However, the quantum well in 2D structures has a large band gap, which proves a great disadvantage for separating the electron­-hole pair owing to the strong binding force. As such, quasi­-2D perovskite, which raises the number of inorganic slabs that charge carriers transport through, is introduced. Along with the formation involving large cations, hydrophobic properties are procured.
    In this work, we investigated the incorporation of a large organic cation with double ammonium ends, ethylenediammonium (EDA2+), into the lead triiodide perovskite structure of FA0.9Cs0.1PbI3. With this combination, heat treatments including both hot-­casting method and post­-annealing were implemented. By applying various temperatures before and after the spin­-coating, we aimed to understand how heating affects the crystallisation of the lat­tice structure. Nevertheless, the 2D structure was still retained in thin film, only to be found growing more inwards. The engagement of FACl as additive not only ameliorated the mor­phology, but also upgraded crystallinity and lattice orientation. Its introduction served well for Dion­-Jacobson phase perovskite materials and could be an indispensable reference for future endeavours in this field.

    摘要 i Abstract ii Acknowledgements iv Table of Contents vi List of Tables viii List of Figures ix Chapter 1. Introduction 1 1.1. Overture 1 1.2. Mechanism in Solar Cells 4 1.2.1. Shockley­-Queisser Limit 4 1.2.2. Working Principle of a Solar Cell 6 1.3. Parameters for the Efficiency of Solar Cells 8 1.3.1.  Short-circuit current density (Jsc) and open-­circuit voltage (Voc) 10 1.3.2.  Fill factor 12 1.3.3.  Power conversion efficiency 13 1.3.4.  Quantum efficiency 14 1.4. Types of Solar Cells 16 1.4.1. First generation solar cells 16 1.4.2. Second generation solar cells 18 1.4.3. Third generation solar cells 19 1.5. Research Objective 26 Chapter 2. Literature Review 29 2.1. Three­-dimensional Perovskite Structure 29 2.1.1. A-­site cation 30 2.1.2. B­-site cation 39 2.1.3. X­-site anion 43 2.2. Low-­dimensional Perovskite 47 2.2.1. Ruddlesden­-Popper phase 50 2.2.2. Dion­-Jacobson phase 55 2.2.3. Trap state 61 2.3. Mechanism for Nucleation 62 Chapter 3. Experimental Section 64 3.1. Apparatuses and Materials 64 3.2. Experimental Design 65 3.3. Film Fabrication 67 3.3.1. Substrate 67 3.3.2. Mesoporous layer 67 3.3.3. Three­-dimensional thin film 67 3.3.4. Low­-dimensional thin film 68 3.4. Characterisation Method 69 3.4.1. X-­ray diffraction (XRD) 69 3.4.2. Grazing­-incidence wide­-angle X-­ray scattering (GIWAXS) 70 3.4.3. Scanning electron microscope (SEM) 71 3.4.4. Photoluminescence (PL) 72 3.4.5. UV­-vis absorption 73 3.4.6. Fourier­-transform infrared spectrometer (FTIR spectrometer) 74 3.4.7. Contact angle meter 75 3.4.8. Near-­edge X­ray Absorption Fine Structure (NEXAFS) 76 Chapter 4. Results and discussion 79 4.1. Film characterisation 79 4.1.1. Identification 80 4.1.2. Orientation 97 4.1.3. Optical properties 100 4.1.4. Morphology 104 4.2. Effect of Additives 109 4.2.1. Identification 110 4.2.2. Orientation 114 4.2.3. Morphology 114 Chapter 5. Conclusion 116 Chapter 6. Future Work 118 References 119

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