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研究生:劉瑞文
研究生(外文):Jui-wen Liu
論文名稱:以射頻磁控濺鍍法製備鍶銅氧化物透明導電膜之性質研究
論文名稱(外文):Investigation on Properties of Transparent Conductive Strontium Copper Oxide Film by RF Magnetron Sputtering System
指導教授:李世欽李世欽引用關係
指導教授(外文):Shih-chin Lee
學位類別:博士
校院名稱:國立成功大學
系所名稱:材料科學及工程學系碩博士班
學門:工程學門
學類:材料工程學類
論文種類:學術論文
論文出版年:2008
畢業學年度:96
語文別:中文
論文頁數:135
中文關鍵詞:光電性質透明導電膜退火鍶銅氧濺鍍摻雜p型
外文關鍵詞:Post-annealingTransparent conducting oxide (TCO) filmsstrontium copper oxideOptoelectronic propertiesSputteringp-type
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  • 被引用被引用:3
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本研究的主要目的,在於利用磁控濺鍍法製備氧化銅鍶(strontium copper oxide, SCO)薄膜,並針對薄膜之結構、導電性質與光學性質進行研究。SCO薄膜先以不同的濺鍍參數進行濺鍍製程。濺鍍氣氛主要以氬氣與氧氣用不同的流量比混合。濺鍍完成後,再將薄膜置於氧氣氣氛下,以不同的退火溫度進行退火處理。根據低掠角薄膜X光繞射儀分析後的結果顯示,在4x10-1 Pa工作壓力下,當氧氣流量增加至10 sccm以上,可沉積出SrCu2O2導電相,並以氧氣流量20 sccm下沉積出的薄膜性質最佳,此時的電阻率、載子濃度與載子遷移率分別為6.64x10-2 Ω·cm、2.89x1021 cm-3及0.092 cm2 V-1s-1。其中薄膜的載子濃度與載子遷移率均隨氧氣的流量變化。載子濃度隨氧氣流量增加而增加,但載子遷移率則呈現相反的變化趨勢。薄膜之光學穿透率在29%~41%之間變化,並隨著氧氣流量增加而增加。
後半段之研究選擇在實驗中光學穿透率與電阻率最低的初鍍膜,在壓力1.01×10-5 Pa的純氧氣中進行退火製程,嘗試藉由結晶性的改善以增加載子遷移率。退火溫度分別為100℃、200℃、350℃、450℃,時間為三小時。實驗結果顯示適當的退火溫度可降低薄膜電阻率。隨著退火溫度上升,當退火溫度升高至350℃時,電阻率可降低至1.63x10-2 Ω·cm,此時的薄膜之載子濃度與載子遷移率分別為1.21x1021 cm-3與4.0x10-5 m2V-1S-1。其中,光學穿透率隨退火溫度的增加而有小幅度的增加,550 nm處的穿透率到達58.2%。研究中並發現當退火溫度上升到450℃時,會導致SrCu2O2導電相消失,使薄膜電阻率大幅上升。以霍爾效應分析量測對初鍍膜與退火處理後的薄膜進行分析,結果顯示兩者均為p型的半導體透明導電膜。
The main purpose of this study is to investigate the feasibility of depositing the strontium copper oxide (SCO) films by the radio frequency magnetron sputtering system. Structural, electrical and optical properties of these films were studied. The SCO films were first deposited with different combinations of Ar and O2 gas on glass substrates at room temperature, and then annealed in O2 atmosphere at different annealing temperature. Grazing incidence angle x-ray diffraction (GIAXRD) analysis showed that SrCu2O2 structure was achieved when oxygen flow was raised above 10 sccm, while the total working pressure was kept at 4.0x10-1 Pa. Both carrier density and resistivity of the film varied with oxygen partial pressure. The optimum optoelectrical properties appeared on the films deposited under pure O2 atmosphere. The carrier density of the films was increased as increasing of oxygen flow rate, but the variation in carrier mobility shown an opposite trend. The carrier density and resistivity of the film prepared with 20 sccm oxygen flow were 2.89x1021 cm-3 and 6.64x10-2 Ω·cm, respectively. The carrier mobility was 0.092 cm2 V-1s-1 and the Hall coefficient measured at room temperature indicated that the conduction was p-type. The optical transmittance in the visible range 550 nm was 29%~41%.
Then, the as-deposited films with the best optoelectrical properties were chosen to annealed at different temperatures ranging from 100℃ to 450℃ in an oxygen atmosphere controlled at 1.01×105 Pa. Results showed that the resistivity decreased as the annealing temperature raised from 100℃ to 350℃, and then increased when annealed at 450℃. Carrier density of an annealed film increased to 1.21x1021 cm-3 as the annealing temperature increased. Results also showed that the resistivity of a SCO film was correlated to the carrier mobility; the highest carrier mobility observed by annealing a SCO film at 350℃ was 4.0x10-5 m2V-1S-1. The optical transmittance of an annealed SCO film in the visible range at 550 nm fell between 52.6% and 58.2%. The Hall coefficient measured at room temperature indicated the nature of the as-deposited and annealed films were both p-type.
摘要 I
Abstract III
誌謝 V
總目錄 VII
圖目錄 XI
表目錄 XIV
第一章 序論 1
1-1 前言 1
1-2 研究動機與目的 7
第二章 理論基礎與文獻回顧 9
2-1 薄膜成核成長理論 9
2-2 透明導電氧化物膜 17
2-2-1 n型透明導電氧化物材料 17
2-3 p型透明導電氧化物材料 21
2-4 CMVB法 23
2-5 Delafossite結構與非Delafossite結構之p型TCO材料 26
2-5-1 Delafossite結構的p型TCO材料 26
2-5-2 非Delafossite結構的p型TCO材料 33
2-6 氧化銅鍶相關文獻與薄膜製備方法 36
2-6-1 SrCu2O2之結晶構造 36
2-6-2 SrCu2O2薄膜製備法整理 36
2-7 氧化銅鍶之光電性質 42
2-7-1 電學性質 42
2-7-2 光學性質 44
第三章 實驗方法與步驟 49
3-1 實驗流程 49
3-2 實驗材料 50
3-3 鍍膜製程 50
3-3-1 實驗系統說明 50
3-3-2 鍍膜參數及步驟 54
3-3-3 鍍層退火處理 55
3-4 鍍膜性質分析 56
3-4-1 膜厚與成長速率之量測 56
3-4-2 結構分析 58
3-4-2.1 XRD分析 58
3-4-3 電性量測 59
3-4-4 表面形態及粗糙度分析 65
3-4-5 光學性質量測 65
第四章 結果與討論 66
4-1 製程參數對鍍層性質之研究 66
4-1-1 製程參數對沉積速率之研究 66
4-1-1.1 濺鍍氣氛與沉積速率 69
4-1-1.2 濺鍍功率與沉積速率 70
4-1-1.3 工作壓力與沉積速率 70
4-1-2 製程參數與薄膜結構的探討 74
4-1-2.1 濺鍍氣氛與薄膜結構 74
4-1-2.2 濺鍍功率與薄膜結構 75
4-1-2.3 工作壓力與薄膜結構 76
4-1-3 薄膜電性與濺鍍氣氛之探討 81
4-1-3.1 四點探針與霍爾效應 83
4-1-4 濺鍍氣氛與薄膜光學性質 87
4-1-4.1 光學穿透率 87
4-1-4.2 光學反射率 89
4-1-4.3 濺鍍氣氛與光學能隙的計算 94
4-1-5 表面形態之觀察 98
4-1-6 薄膜成分分析 103
4-2 退火處理對鍍層性質影響之研究 105
4-2-1 退火溫度與薄膜結構 105
4-2-2 退火溫度與薄膜導電性質 107
4-2-3 退火溫度與薄膜光學性質 113
4-2-4 退火溫度與表面形態 119
第五章 結論 122
參考文獻 125
附錄(自述) 135
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