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研究生:沈忠雄
研究生(外文):Jung-hsiung Shen
論文名稱:導電透明氧化鋅與銦錫氧化物薄膜之低溫製備與光電性質研究
論文名稱(外文):Low Temperature Preparation and Optoelectronic Properties of ZnO and ITO Transparent Conducting Thin Films
指導教授:甘德新
指導教授(外文):Dershin Gan
學位類別:博士
校院名稱:國立中山大學
系所名稱:材料與光電科學學系研究所
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:2010
畢業學年度:98
語文別:英文
論文頁數:88
中文關鍵詞:薄膜離子束濺鍍銦錫氧化物氧化鋅
外文關鍵詞:Thin filmsZnOIon beam sputteringITO
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本論文在研究導電透明銦錫氧化物(ITO)與氧化鋅(ZnO)薄膜之低溫製備,微結構,及其光電性質。首先,使用離子束濺鍍法於低溫製備高穿透率、低電阻之ZnO薄膜於玻璃基材上,藉由控制離子束電壓與電流,可於150 oC的基材溫度下製備出穿透率、電阻率、載子遷移率分別為85-90%、2.95 x 10-3 Ω-cm與21.41 cm2/Vs的氧化鋅薄膜,且厚度低於200 nm。對其微結構與光電性質之關係將進一步分析討論。
然後於200 oC以及400 oC下,於氯化鈉單晶(001)面,分別製備出表面為 與 的ZnO奈米薄膜。使用光致螢光光譜儀分析 面得知在其發光光譜上僅有一在能帶邊緣的發光峰;而在 面上則同時出現能帶邊緣的發光峰與一寬化的可見光峰,其可能機制將加以討論。ZnO與NaCl之間的晶向關係與其界面亦將加以分析討論。
其次使用離子束濺鍍法於室溫下製備高穿透率、低電阻率之ITO薄膜於玻璃基材上,探討在沉積過程中通氣方式、氧流量、離子束電壓、電流等對薄膜結晶性、穿透率與導電性之影響。製備出電阻率約10-4 Ω-cm、穿透率為85-90%之導電透明ITO層,並利用霍爾量測法量測其載子遷移率與載子濃度,並探討對電阻率之影響。
然後於200 oC下製備ITO薄膜於玻璃基材上,探討氧流量對微結構與光電性質之影響。發現於低氧流量的沉積條件下,薄膜表面有ITO鬚晶產生,其頂部為銦金屬,其晶向關係為(010)In//(110)ITO與(001)In// (001)ITO。該鬚晶乃以銦金屬做為晶種並藉由氣體-液體-固體成長機制而形成。隨著氧流量的增加,ITO薄膜結晶性隨之降低直至轉變為非晶相結構為止。高穿透率(~90%)與低電阻率(6 x 10-4 Ω-cm)之ITO薄膜可在中等程度的氧流量下製得。
The purposes of this thesis are to prepare ZnO and tin-doped In2O3 (ITO) films at low temperature and study their microstructure and optoelectronic properties. Low-temperature growth of undoped ZnO films with high transparency and low electrical resistance was prepared by ion beam sputtering. After systematic testing, a sheet resistivity as low as 2.95 x 10-3 Ω-cm was obtained at a substrate temperature of 150 oC, ion source voltage of 850 V, and ion beam current of 30 mA. The transmittance of the ZnO films was in the range of 85-90%. Hall measurements showed that a high mobility of 21.41 cm2/Vs was obtained for films less than 200 nm thick. The related microstructures and physical properties were measured and discussed.
ZnO nanofilm of (2-1-10) and (01-11) surfaces were prepared on NaCl (001) surface at 200 oC and 400 oC to produce nearly pure (2-1-10) and (01-11) textures respectively and the orientation relationships were determined and the interface discussed. By dissolving the NaCl substrate, the ZnO (2-1-10) and (01-11) surfaces several cm2 in area, which may have some useful applications, can be easily prepared. The photoluminescence spectrum from the (2-1-10) surface showed only a near-band-edge UV emission peak while the (01-11) surface showed a near band-edge UV emission and a broad green emission.
Low-temperature preparation of transparent conducting electrode is essential for flexible optoelectronic devices. ITO films of high transparency and low electrical resistance were prepared at room temperature with a radio-frequency ion beam sputtering system. Specimens with a low sheet resistivity of 10-4 Ω-cm and a high visible-light transmittance of 85-90% were obtained. Hall measurement was used to measure the mobility and carrier concentrations and the effects on resistivity were discussed.
ITO films were deposited on glass substrates at 200 oC at various oxygen flow rates. At low oxygen flow rate the film surface has ITO whiskers with metallic In tips and a crystallographic relationship of (010)In//(110)ITO and (001)In//(001)ITO is present between them. The In tips act as the seeds for the growth of ITO whiskers by a vapor-liquid-solid growth mechanism.
As the oxygen flow rate increases, the crystallinity of the ITO film decreases till an amorphous phase is formed. The microstructure, resistivity and transmittance of the films were studied as a function of oxygen flow rate. Thin films of high transmittance (~90%) and low resistivity (6 x 10-4 Ω-cm) were prepared at an intermediate oxygen flow rates.
論文摘要內容(中).................................................................I
Abstract.................................................................................III
Contents................................................................................V
List of Figures.................................................................................VII
List of Tables....................................................................................X

Chapter 1...............................................................................1
Low-temperature preparation of undoped ZnO films with high transparency and conductivity by ion beam deposition
1.1Introduction......................................................................1
1.2Experimental procedure...............................................2
1.3Results and discussion............................................................................3
1.4Conclusion......................................................................8

Chapter2.............................................................................15
Oriented growth of ZnO nanofilms on NaCl (001) by ion beam sputtering
2.1Introduction...................................................................15
2.2Experimental procedure.............................................18
2.3Results and discussion.............................................18
2.3.1Low-temperature growth of the ZnO nanofilm...18
2.3.2Structure, interface, and luminescence of the ZnO nanofilm.....................................................................20
2.3.2.1SAED analysis.......................................................21
2.3.2.2Formation of the (01-11) surface.......................21
2.3.2.3The (01-11)ZnO /(001)NaCl interface...............24
2.3.2.4Luminescence.......................................................25
2.4Conclusion....................................................................26

Chapter3.............................................................................40
Room-temperature preparation of high transparency and low resistivity ITO films by ion beam sputtering
3.1Introduction...................................................................40
3.2Experimental procedure.............................................41
3.3Results and discussion.............................................42
3.3.1Oxygen flow into the chamber................................42
3.3.1.1Effect of oxygen flow rate......................................42
3.3.1.2Effect of ion beam voltage...................................42
3.3.2Oxygen flow into the ion beam...............................43
3.3.2.1Effect of oxygen flow..............................................43
3.3.2.2Effect of ion beam current....................................45
3.4Conclusion....................................................................47

Chapter4.............................................................................52
Microstructures and properties of ITO films prepared by ion beam sputtering at low temperature
4.1Introduction...................................................................52
4.2Experiment procedure............................................................................53
4.3Results and discussion.............................................54
4.3.1XRD analysis.............................................................54
4.3.2SEM analysis.............................................................55
4.3.3TEM analysis.............................................................56
4.3.4Optoelectronic properties.......................................57
4.4Conclusion....................................................................59

References.........................................................................67
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