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http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/91984完整後設資料紀錄
| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 莊嘉揚 | zh_TW |
| dc.contributor.advisor | Jia-Yiang Juang | en |
| dc.contributor.author | 吳承洋 | zh_TW |
| dc.contributor.author | Cheng-Yang Wu | en |
| dc.date.accessioned | 2024-02-27T16:22:49Z | - |
| dc.date.available | 2024-02-28 | - |
| dc.date.copyright | 2022-09-07 | - |
| dc.date.issued | 2022 | - |
| dc.date.submitted | 2002-01-01 | - |
| dc.identifier.citation | [1] K. Ellmer, "Past achievements and future challenges in the development of optically transparent electrodes," Nature Photonics, Review Article vol. 6, p. 809, 11/30/online 2012.
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Castro-Hermosa et al., "Efficient fully blade-coated perovskite solar cells in air with nanometer-thick bathocuproine buffer layer," Nano Research, vol. 14, no. 4, pp. 1034-1042, 2021/04/01 2021. [121] 邱立擎, "噴射式大氣電漿系統鍍製霧度導電薄膜應用於鈣鈦礦太陽能電池前電極," 碩士論文, 機械工程學研究所, 國立臺灣大學, 台北市, 2022. | - |
| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/91984 | - |
| dc.description.abstract | 具有紋理表面的透明導電氧化物(Transparent conductive oxide, TCO)薄膜通常具有高霧度的特性，能使光產生散射與漫射，增加光的路徑長，有望提高太陽能電池的光電轉換效率。而沉積具有紋理表面的TCO通常需要額外的製程步驟，例如蝕刻和塗佈奈米顆粒，這些步驟會使製程複雜化，成本也隨之增加。本研究使用噴射式大氣電漿系統(Atmospheric pressure plasma jet, APPJ)搭配共摻雜法(Co-doping)一步驟鍍製出高霧度鎵和鋯共摻雜氧化鋅(GZO:Zr)透明電極於5 × 5 cm^2之玻璃基板上，相較於文獻中使用的複雜製程，APPJ系統不需在真空環境下操作，過程中也不需要更換機台以及製程參數，基板溫度也較低(180℃)，既省時又省成本。最佳參數之GZO:Zr (2 at%)薄膜具有高霧度(34.8%)、低電阻率(7.88 × 10^-4 Ω-cm) 和出色的品質參數(Figure fo merit, F.O.M, 8.22 × 10^3 Ω^-1)。本研究發現當2 at% Zr摻雜到 GZO 薄膜中時，霧度從7.19%提升到34.8% (+ 384%)，此霧度的提升可歸因於薄膜表面粗糙度的增加。本研究進行了電子顯微鏡（Scanning electron microscopy, SEM）和原子力顯微鏡（Atomic force microscopy, AFM）來探討薄膜的表面形態。SEM圖像顯示，將Zr摻雜到GZO薄膜中會使薄膜表面產生球狀顆粒。AFM結果表明，這些顆粒會使薄膜之均方根粗糙度顯著增加，從而增加了霧度。此外，鮮少研究針對共摻雜薄膜之化學組成進行探討，因此本研究也透過能量散佈X光光譜儀(Energy-dispersive X-ray spectroscopy, EDS)及X光光電子能譜儀（X-ray photoelectron spectroscopy, XPS）分析共摻雜對薄膜化學組成的影響，EDS結果顯示，粒徑大小較小的球狀顆粒之鋯含量較基材的含量高；而XPS及XRD皆有量測到ZrO2的訊號，再搭配霍爾量測的結果可推測，2 at% Zr之摻雜濃度可能就已超過氧化鋅薄膜之摻雜極限，多數的鋯都是以氧化鋯團簇之形式出現在薄膜中，只有少數的鋯有參與摻雜。綜合上述量測分析，我們推論共摻雜薄膜表面出現球狀顆粒的原因為：反應物過多時會因為解離不完全而預先在空中成核，並被薄膜表面所吸附。
為了驗證高霧度薄膜是否適用於提高鈣鈦礦太陽能電池之光電轉換效率，本研究進一步將GZO及GZO:Zr (2 at%)薄膜組成鈣鈦礦太陽能電池，結果顯示雖然GZO:Zr (2 at%)有良好的光電性質及接近35%的高霧度，但組成之太陽能電池光電轉換效率卻較低，這可能是因為旋轉塗佈法(Spin coating)容易受到底層材料的表面形貌影響，GZO:Zr (2 at%)之表面粗糙度太大將影響旋轉塗佈之均勻性，導致鈣鈦礦層長晶時內部產生缺陷造成元件開路電壓下降，也會使各層間的接觸電阻提升而提高串聯電阻，此外，因為鈣鈦礦太陽能電池之總厚度(不包含透明電極)不超過200 nm，過高的表面粗糙度會使電極刺穿電池造成短路，導致並聯電阻過低使光電轉換效率變低。因此GZO:Zr (2 at%)並不適用於厚度較薄，且製程以旋轉塗佈法為主的鈣鈦礦太陽能電池，更適合應用於製程不受表面粗糙度影響，或總厚度較厚之電池元件，例如矽基太陽能電池。 | zh_TW |
| dc.description.abstract | Transparent conductive oxides (TCOs) with textured surfaces often have high haze factors. High haze factors enable light to be scattered, leading to longer optical path lengths, promising to enhance solar cells' power conversion efficiency. Deposition of TCOs with textured surfaces often requires additional process steps, such as etching and coating nanoparticles. However, those steps take substantial effort and time, making the process inefficient and complicated to handle. Here, we demonstrate a one-step fabrication process to deposit high haze gallium and zirconium co-doped zinc oxides (GZO:Zr) prepared by atmospheric pressure plasma jet (APPJ) on 5 × 5 cm^2 glasses. GZO:Zr (2 at%) films achieve a high haze (34.8%), a low resistivity (7.88 × 10^-4 Ω cm), and a great Figure of merit (F.O.M, 8.22 × 10^−3 Ω^−1). When 2 at% Zr is doped into GZO films, the haze factor increases from 7.19% to 34.8% (+ 384%). Such an increase in haze may be attributed to the increased surface roughness. We conducted SEM and AFM to investigate the surface morphology of films. SEM images show that doping Zr into GZO thin films creates spherical particles on the film surface. AFM results show that these particles significantly increase the root-mean-square roughness from 18.4 to 122 nm after 2% Zr is doped, thus increasing the haze factor. This study proposes a novel and convenient way to enhance the haze factor of the TCO layer and discover some new phenomena of co-doping TCO thin films. Our vacuum-free method does not need a change of materials or machines/tooling during the process and is suitable for industrial-scale mass production.
In addition, to know the chemical composition of the spherical particles on the surface of GZO:Zr thin film, we conducted EDS and XPS to analyze it. EDS results show that Zr mainly gathers on the smaller spherical particles. XPS and XRD results show the existence of ZrO2 in co-doped films. Combined with the results of Hall measurement, we conclude that 2 at% Zr doping concentration is already too high in our experiment. The excessive reactant would nucleate in the gas phase and then be absorbed on the film surface, hence the spherical particles. In order to verify whether high haze GZO:Zr thin film would enhance the power conversion efficiency of solar cells, we use GZO and GZO:Zr (2 at%) as the electrodes to fabricate perovskite solar cells. The results show that using GZO:Zr (2 at%) as a front electrode would have lower PCE. This is because the large surface roughness affects the spin coating process significantly. The spherical particles might affect the contact of layers and hinder the crystallization of the perovskite layer. Besides, the spherical particles might contact the perovskite layer to cause shunting. Therefore, GZO:Zr (2 at%) might be more suitable for thicker solar cells or processes that would not be affected by the roughness of electrodes, such as silicon solar cells. | en |
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| dc.description.provenance | Made available in DSpace on 2024-02-27T16:22:49Z (GMT). No. of bitstreams: 0 | en |
| dc.description.tableofcontents | 目錄
誌謝 I 中文摘要 III ABSTRACT V 目錄 VIII 圖目錄 XI 表目錄 XV 符號表 XVI Chapter 1 緒論 1 1.1 透明導電薄膜概論 1 1.2 研究動機與目的 2 Chapter 2 文獻回顧與理論基礎 5 2.1 文獻回顧 5 2.1.1 共摻雜 5 2.1.2 高霧度透明電極 7 2.2 GZO薄膜結構與光電特性 11 2.2.1 GZO薄膜材料之結構特性 11 2.2.2 GZO薄膜材料之光電特性 12 2.3 薄膜沉積理論 13 2.4 常見薄膜沉積方法 15 2.4.1 蒸鍍法(Evaporation) 15 2.4.2 濺鍍法(Sputtering) 16 2.4.3 脈衝雷射沉積(Pulsed laser deposition, PLD) 17 2.4.4 分子束磊晶(Molecular beam epitaxy, MBE) 18 2.4.5 化學氣相沉積(Chemical vapor deposition, CVD) 19 2.4.6 噴霧熱裂解法(Spray pyrolysis) 20 2.4.7 溶膠-凝膠法(Sol gel) 20 2.4.8 原子層沉積(Atomic layer deposition, ALD) 20 2.4.9 大氣電漿(Atmosphere pressure plasma) 21 2.5 電漿原理 26 2.5.1 離子化碰撞 26 2.5.2 激發–鬆弛碰撞 27 2.5.3 分解碰撞 27 Chapter 3 實驗方法與儀器設備 29 3.1 實驗流程 29 3.2 系統架設 29 3.3 噴射式大氣電漿系統細部架設及參數設定 33 3.3.1 基板與前驅物 33 3.3.2 氣體供應系統 34 3.3.3 電力供應系統 35 3.3.4 加熱系統 36 3.3.5 移動平台系統 37 3.3.6 電漿噴嘴 38 3.4 薄膜性質檢測儀器 40 3.4.1 膜厚測定儀 40 3.4.2 片電阻量測 40 3.4.3 霍爾量測 42 3.4.4 薄膜光學性質分析 44 3.4.5 表面形貌分析 45 3.4.6 表面粗糙度分析 46 3.4.7 晶體結構分析 47 3.4.8 能量散佈X光光譜儀分析 48 3.4.9 縱深元素分析 49 3.4.10 X光光電子能譜儀分析 50 3.5 鈣鈦礦太陽能電池之製備方法 51 Chapter 4 結果與討論 52 4.1 高霧度透明導電薄膜製備 52 4.1.1 膜厚分析 52 4.1.2 表面形貌分析 53 4.1.3 表面粗糙度分析 56 4.1.4 晶體結構分析 57 4.1.5 光學性質分析 64 4.1.6 電學性質分析 66 4.1.7 最佳鋯摻雜濃度選擇 67 4.1.8 能量散佈X光光譜分析 69 4.1.9 縱深元素分析 75 4.1.10 X光光電子能譜分析 79 4.1.11 樣本比較與展示 85 4.2 高霧度透明導電薄膜應用於鈣鈦礦太陽能電池 87 Chapter 5 結論與未來展望 90 5.1 結論 90 5.2 未來展望 92 參考文獻 93 著作目錄 108 附錄 109 圖目錄 圖 1.1 高霧度電極對入射光造成之影響示意圖[29] 4 圖 2.1 三種氧化鋅之結構。由左至右分別為：立方岩鹽礦、立方閃鋅礦及六方纖鋅礦[54] 11 圖 2.2 多晶薄膜沉積機制[62] 14 圖 2.3 電子束蒸鍍法示意圖[65] 16 圖 2.4 磁控濺鍍架構示意圖[66] 17 圖 2.5 脈衝雷射沉積系統架構圖[69] 18 圖 2.6 分子束磊晶系統架構圖[70] 19 圖 2.7 噴霧熱解法之系統架構示意圖[72] 20 圖 2.8 原子層沉積法原理示意圖[77] 21 圖 2.9 利用噴射式大氣電漿於SiOx基板上鍍製GZO薄膜示意圖[43] 22 圖 2.10 電漿火炬示意圖[82] 23 圖 2.11 電暈放電示意圖[93] 25 圖 2.12 介電質屏蔽放電示意圖[98] 25 圖 2.13 離子化碰撞之示意圖[99] 28 圖 2.14 激發碰撞示意圖 (a) 碰撞前 (b) 碰撞後[99] 28 圖 2.15 鬆弛碰撞示意圖 (a) 碰撞前 (b) 碰撞後[99] 28 圖 2.16 分解碰撞示意圖[99] 28 圖 3.1 高霧度透明電極實驗流程圖 29 圖 3.2 (上圖)大氣電漿薄膜鍍製系統之架構，(下圖)電將噴嘴柵狀掃描之掃描路徑示意圖 30 圖 3.3 噴射式大氣電漿系統腔體外部件 31 圖 3.4 噴射式大氣電漿系統腔體內之部件 32 圖 3.5 前驅瓶及振盪片系統示意圖 34 圖 3.6 供氣系統流程圖 35 圖 3.7 電力供應系統流程圖 36 圖 3.8 加熱系統示意圖 (a)加熱吸盤 (b)電漿噴嘴加熱棒[87] 37 圖 3.9 移動平台操作系統 37 圖 3.10 電漿噴嘴內部構造圖[87] 39 圖 3.11 表面輪廓儀(DektakXT) 40 圖 3.12 四點探針量測系統(Sadhu Design Model：EM4P)及多功能電錶(Agilent 3440A) 41 圖 3.13 四點探針原理示意圖[101] 42 圖 3.14 霍爾量測儀(Ecopia HMS-3000) 43 圖 3.15 霍爾效應原理示意圖(以n型半導體為例) 43 圖 3.16 載台晶片(HMS-3000) 44 圖 3.17 UV-Vis-NIR 光譜分析儀[102] 45 圖 3.18 高解析場發射掃描式電子顯微鏡 (JeoL JSM-7800F Prime) [103] 46 圖 3.19 原子力顯微鏡 (Bruker MultiMode 8) [87] 47 圖 3.20 D8 DISCOVER SSS多功能高功率X光繞射儀[104] 48 圖 3.21 高解析場發射掃描式電子顯微鏡 (JeoL JSM-7800F Prime) [103] 49 圖 3.22 二次離子質譜儀 (TOF-SIMS IV) [105] 50 圖 3.23 化學電子能譜儀(PHI 5000 Versa Probe) [106] 51 圖 4.1 鋯摻雜濃度與膜厚之關係[109] 53 圖 4.2 不同鋯摻雜濃度之薄膜之SEM上視圖 (a) GZO (b) GZO:Zr (2 at%) (c) GZO:Zr (4 at%) (d) GZO:Zr (6 at%) (比例尺：2 μm) 55 圖 4.3不同鋯摻雜濃度之薄膜之表面顆粒平均粒徑大小 55 圖 4.4不同鋯摻雜濃度之薄膜之表面顆粒數量 56 圖 4.5 不同鋯摻雜濃度之薄膜之表面顆粒覆蓋率 56 圖 4.6 不同鋯摻雜濃度之薄膜的AFM圖像以及平方平均值表面粗糙度 (a) GZO (b) GZO:Zr (2 at%) (c) GZO:Zr (4 at%) (d) GZO:Zr (6 at%) [109] 57 圖 4.7 不同鋯摻雜濃度之薄膜XRD峰譜圖 61 圖 4.8 (1 0 0)、(0 0 2)、(1 0 1)、(1 0 3)峰之面積比[109] 62 圖 4.9 t-ZrO2 (1 0 1)繞射峰之面積比例 63 圖 4.10 不同鋯摻雜濃度之薄膜之(0 0 2)繞射峰半高寬及晶粒大小 63 圖 4.11 不同鋯摻雜濃度之薄膜之殘餘應力 64 圖 4.12 不同鋯摻雜量之薄膜之總穿透度 65 圖 4.13不同鋯摻雜量之薄膜之鏡面穿透度 65 圖 4.14 不同鋯摻雜量之薄膜之霧度 66 圖 4.15 不同鋯摻雜濃度之薄膜的載子濃度、霍爾遷移率及電阻率[109] 67 圖 4.16 不同鋯摻雜濃度之薄膜之F.O.M及霧度[109] 68 圖 4.17 GZO之SEM圖(上)與X-射線能譜儀素像(下) (比例尺：1 μm) 70 圖 4.18 GZO:Zr (2 at%)之SEM圖(上)與X-射線能譜儀素像(下) (比例尺：1 μm) 71 圖 4.19 GZO:Zr (4 at%)之SEM圖(上)與X-射線能譜儀素像(下) (比例尺：1 μm) 72 圖 4.20 GZO:Zr (6 at%)之SEM圖(上)與X-射線能譜儀素像(下) (比例尺：1 μm) 73 圖 4.21 GZO:Zr (2 at%)之SEM圖與框選的9個區域 (比例尺：1 μm) 74 圖 4.22 不同鋯摻雜濃度之薄膜的矽元素縱深分布圖 76 圖 4.23 不同鋯摻雜濃度之薄膜的碳元素縱深分布圖 76 圖 4.24 不同鋯摻雜濃度之薄膜的鋅元素縱深分布圖 77 圖 4.25 不同鋯摻雜濃度之薄膜的鎵元素縱深分布圖 77 圖 4.26 不同鋯摻雜濃度之薄膜的鋯元素縱深分布圖 78 圖 4.27 GZO XPS全頻掃描圖譜 81 圖 4.28 不同鋯摻雜濃度之薄膜的Ga2p元素鍵結比例比較 (a) GZO (b) GZO:Zr (2 at%) (c) GZO:Zr (4 at%) (d) GZO:Zr (6 at%) 82 圖 4.29 不同鋯摻雜濃度之薄膜的O1s元素鍵結比例比較 (a) GZO (b) GZO:Zr (2 at%) (c) GZO:Zr (4 at%) (d) GZO:Zr (6 at%) 83 圖 4.30 不同鋯摻雜濃度之薄膜的Zr3d元素化學電子能譜圖 (a) GZO (b) GZO:Zr (2 at%) (c) GZO:Zr (4 at%) (d) GZO:Zr (6 at%) 84 圖 4.31 本研究與高霧度透明電極之性能比較圖 85 圖 4.32 可見光源下樣本之比較圖[109] 86 圖 4.33 GZO與GZO:Zr (2 at%)組成之鈣鈦礦太陽能電池之光電轉換效率盒狀圖 88 圖 4.34 GZO與GZO:Zr (2 at%)之表面輪廓儀量測結果 89 表目錄 表 2.1 共摻雜薄膜之歷年文獻統整 7 表 2.2 高霧度透明導電薄膜之歷年文獻統整 10 表 3.1 碳酸鈉鹼性光學玻璃組成成分表 33 表 3.2 碳酸鈉鹼性光學玻璃機械性質表 34 表 4.1 不同鋯摻雜濃度之前驅物的密度(ρp)、霧滴直徑(ddroplet)以及平均膜厚(tavg) [109] 53 表 4.2 不同鋯摻雜濃度之薄膜之t-ZrO2 (1 0 1)繞射峰位置 62 表 4.3 不同鋯摻雜濃度之薄膜之穿透度、片電阻、F.O.M及霧度[109] 68 表 4.4 GZO:Zr (2 at%)之SEM圖中框選的9個區域之元素含量 74 表 4.5 不同鋯摻雜濃度之薄膜的Ga2p元素鍵結比例比較 82 表 4.6 不同鋯摻雜濃度之薄膜的O1s元素鍵結比例比較 83 表 4.7 不同鋯摻雜濃度之薄膜的Zr3d5/2及Zr3d3/2束縛能位置及曲面下總面積 84 表 4.8 以GZO、GZO:Zr (2 at%)為電極之太陽能電池之開路電壓(VOC)、短路電流(JSC)、填充因子(FF)、串聯電阻(Rs)、並聯電阻(Rsh)及光電轉換效率(PCE) 88 | - |
| dc.language.iso | zh_TW | - |
| dc.subject | 共摻雜 | zh_TW |
| dc.subject | 鎵與鋯共摻雜氧化鋅 | zh_TW |
| dc.subject | 高霧度透明電極 | zh_TW |
| dc.subject | 光散射 | zh_TW |
| dc.subject | 鈣鈦礦 | zh_TW |
| dc.subject | 太陽能電池 | zh_TW |
| dc.subject | 大氣電漿 | zh_TW |
| dc.subject | 鎵摻雜氧化鋅 | zh_TW |
| dc.subject | Light scattering | en |
| dc.subject | High haze electrode | en |
| dc.subject | Gallium and Zirconium co-doped Zinc Oxide (GZO) | en |
| dc.subject | Gallium doped Zinc Oxide (GZO) | en |
| dc.subject | co-doping | en |
| dc.subject | Perovskite solar cell | en |
| dc.subject | Atmosphere pressure plasma jet (APPJ) | en |
| dc.title | 利用噴射式大氣電漿系統製備高霧度鎵與鋯共摻雜氧化鋅透明導電薄膜 | zh_TW |
| dc.title | High Haze Ga and Zr Co-doped Zinc Oxide Transparent Electrodes Prepared by Atmospheric Pressure Plasma Jet | en |
| dc.type | Thesis | - |
| dc.date.schoolyear | 111-1 | - |
| dc.description.degree | 碩士 | - |
| dc.contributor.oralexamcommittee | 林明澤;許麗;李志偉 | zh_TW |
| dc.contributor.oralexamcommittee | Ming-Tzer Lin;Li Xu;Jyh-Wei Lee | en |
| dc.subject.keyword | 大氣電漿,共摻雜,鎵摻雜氧化鋅,鎵與鋯共摻雜氧化鋅,高霧度透明電極,光散射,鈣鈦礦,太陽能電池, | zh_TW |
| dc.subject.keyword | Atmosphere pressure plasma jet (APPJ),co-doping,Gallium doped Zinc Oxide (GZO),Gallium and Zirconium co-doped Zinc Oxide (GZO),High haze electrode,Light scattering,Perovskite solar cell, | en |
| dc.relation.page | 109 | - |
| dc.identifier.doi | 10.6342/NTU202203026 | - |
| dc.rights.note | 未授權 | - |
| dc.date.accepted | 2022-09-01 | - |
| dc.contributor.author-college | 工學院 | - |
| dc.contributor.author-dept | 機械工程學系 | - |
| 顯示於系所單位： | 機械工程學系 | |
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