臺灣博碩士論文加值系統

　　發光二極體被視為未來主要的照明光源，高功率發光二極體於技術上屢有突破，但現階段發光效率的不足，使發光二極體無法取代傳統光源作為照明燈源的主流，故發光二極體發光效率的提升，是目前技術發展的重點之一。過去的研究指出，將奈米線應用於發光二極體的結構製作，能有效提升其發光強度；而在各式成長奈米線的方法中，以水熱法製備之奈米線具有高品質順向成長與製程簡易的優點，故本論文將採用此法成長氧化鋅奈米線，並以射頻濺鍍法沉積N型氧化鋅鋁薄膜，P型材料則選用氧化鋅與氮化鎵，藉以製備氧化鋅奈米線發光二極體，進行其特性之研究。
　在奈米線的部份，藉由水熱法成功製備氧化鋅奈米線，直徑34 nm-200 nm，長度1 um-2 um，密度4 NWs/um2-68.23 NWs/um2。EDS分析顯示氧化鋅奈米線的鋅、氧比接近50 % : 50 %。XRD分析僅於34度存在繞射峰值，亦即於(002)面有較強之繞射訊號。PL顯示奈米線的發光峰值位於378 nm，並具有微弱之可見光放射。從HRTEM可觀察到，奈米線內部的晶格結構良好，晶格條紋間距為0.2629 nm，証實奈米線為C軸取向成長。
　　N型氧化鋅鋁薄膜部份，其最佳電阻率為3×10^(-3) Ω-cm，載子濃度為1.72×10^21 cm^(-3)，載子遷移率為0.0715 cm2/V-s，於可見光波段的平均穿透率大於80 %，於波長450 nm之最佳穿透率為87 %，於波長380 nm之最佳穿透率為77 %。
　　P型氧化鋅部份，分別使用氧化鋅及純鋅靶材，嘗試藉由製程氣體氧/氬比例的控制，用以製備P型氧化鋅，但目前薄膜均呈現N型半導體電性。未來將使用摻雜P2O5之氧化鋅靶材，繼續P型氧化鋅薄膜之試驗。
　　發光二極體部份，目前已於P型氮化鎵(鎂摻雜，載子濃度約為10^17 cm^(-3))薄膜上，成功製備氧化鋅奈米線/N型氧化鋅鋁薄膜結構，並完成發光二極體之晶粒製作，其尺寸為300 um×300 um。在約大於15 V的操作電壓下，以長工作距離顯微鏡可觀察到，發光二極體晶粒的部份區域放射出藍光，且發光強度隨外加電壓而增加。發光二極體之I-V曲線顯示其串聯電阻相當大，未來將以快速熱退火進行後處理，以期提升其性能，並檢測發光頻譜等特性。

Light emitting diode (LED) is considered as the major next-generation luminescence technology, but nowadays insufficient light efficiency of high power LED limits its application for illumination lighting. Some research group have developed nanowrie-inserted LED structure, and the EL intensity shows that the novel LED structure can improve light efficiency effectively. ZnO nanowires grown
by hydrothermal method have excellent properties such as single crystal, vertical alignment, broad area growth and simple process. Thus in this study hydrothermal method is adopted to fabricate ZnO nanowires, N-type material of LED is aluminum-doped ZnO film (AZO) deposited by RF sputtering, and P-type materials are ZnO and Mg-doped GaN film. Finally, the characteristics of N-type AZO/ZnO
nanowire/P-type ZnO or P-type GaN structure LED will be studied.

The ZnO nanowries grown by hydrothermal method are 34 nm-200 nm in diameter, 1 um-2 um in length, and 4 NWs/um2-68.23 NWs/um2 in density. EDS shows the atomic percentage of Zn and O is closed to 50 % : 50 %. XRD peak locates at 34° and shows (002) preferred crystallinity. PL indicates the luminescence peak of nanowries appears at 378 nm, and weak visible emission is observed. HRTEM image shows good crystal structure, and the spacing of lattice fringe is
0.2629 nm.

For AZO film, the optimal resistivity is 3×10^(-3) Ω-cm, carrier concentration is 1.72×10^21 cm^(-3) and mobility is 0.0715 cm2/V-s. The average transmittance of visible light is above 80 %, the optimal transmittance at 450 nm is 87 %, and the optimal transmittance at 380 nm is 77 %.

ZnO and pure zinc targets are used to deposit P-type ZnO by O2/Ar flow controlling, but unfortunately all fabricated samples still show N-type properties. P2O5-doped ZnO target will be used to fabricated P-type ZnO film continuously.

For LED study, ZnO nanowrie/N-type AZO film have been fabricated on Mg-doped P-GaN film (carrier concentration is about 1017 cm-3), the size of LED die is 300 μm × 300 μm. Blue emission is observed from partial area of LED die through long-distance microscope when forward-bias is above 15-20 V, and voltage raise leads to increasing of light intensity. In the next step, current-voltage relation and
electroluminescence (EL) spectrum will be examined.

摘要 ................................. I
總目錄 ................................ V
圖目錄 ................................ VIII
表目錄 ................................ XVIII


第一章 序論 ........................... 1
1.1 前言 ............................. 1
1.2 發光二極體之簡介 .................. 5
1.2.1 發光二極體之原理 .............. 5
1.2.2 發光二極體之發光效率 ........... 7
1.2.3 同質與異質結構發光二極體 ....... 9
1.3 氧化鋅材料 ........................ 18
1.3.1 氧化鋅之材料特性 .............. 18
1.3.2 氧化鋅之發光機制 .............. 18
1.4 量子侷限效應 ...................... 25

第二章 文獻回顧 ....................... 33
2.1 氧化鋅奈米線/奈米柱之製備 .......... 33
2.1.1 VLS與VS成長機制 .............. 33
2.1.2 氣相沉積法 ................... 36
2.1.3 有機金屬化學氣相沉積法 ......... 38
2.1.4 電漿輔助化學氣相沉積法 ......... 40
2.1.5 脈衝雷射蒸鍍法 ................ 41
2.1.6 電化學沉積法 .................. 41
2.1.7 聲化學法 ..................... 44
2.1.8 水熱法 ....................... 45
2.2 氧化鋅奈米線/奈米柱發光二極體之製作 .. 83
2.2.1 有機金屬化學氣相沉積法 ......... 83
2.2.2 化學氣相沉積法 ................ 86
2.2.3 氣相傳輸法 .................... 87
2.2.4 電化學沉積法 .................. 87
2.2.5 水熱法 ....................... 89
2.3 研究動機與目的 .................... 114

第三章 實驗設計與規劃 .................. 115
3.1 元件設計 ......................... 115
3.1.1 發光二極體結構設計 ............ 115
3.1.2 光罩設計 ..................... 117
3.2 實驗規劃與製程 .................... 121
3.2.1 氧化鋅奈米線之製備 ............ 121
3.2.2 同質結構氧化鋅奈米線發光二極體之製作 . 122
3.2.3 異質結構氧化鋅奈米線發光二極體之製作 . 124
3.3 實驗設備 ......................... 132

第四章 實驗結果與探討 .................. 142
4.1 氧化鋅奈米線 ...................... 142
4.1.1 溶液濃度對氧化鋅奈米線之影響 .... 142
4.1.2 反應時間對氧化鋅奈米線形貌之影響 . 155
4.1.3 X光繞射分析 ................... 161
4.1.4 光激發光螢光頻譜分析 ........... 166
4.1.5 穿透式電子顯微鏡分析 ........... 169
4.2 氧化鋅鋁薄膜 ...................... 171
4.2.1 靶材距離對氧化鋅鋁薄膜電阻值之影響 .. 171
4.2.2 氣體流量對氧化鋅鋁薄膜電阻值之影響 .. 172
4.2.3 濺鍍功率對氧化鋅鋁薄膜電阻值之影響 .. 173
4.2.4 快速熱退火對氧化鋅鋁電阻值之影響 .... 173
4.2.5 濺鍍參數對氧化鋅鋁薄膜穿透率之影響 .. 174
4.3 P型氧化鋅薄膜 ......................... 184
4.4 氧化鋅奈米線異質結構發光二極體之製作 ..... 187

第五章 結論與未來展望 ...................... 194
5.1 結論 ................................. 194
5.2 未來展望 ............................. 196

參考文獻 .................................. 197

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