臺灣博碩士論文加值系統

本論文是利用有機金屬氣相磊晶以選擇性佈植和選擇性再成長技術(regrowth)成長氮化鎵發光二極體。於再成長時磊晶層會先成長在非佈植區域而不是佈植區域，這主要是因為經過離子佈植後，佈植區與非佈植區之間產生了晶格差異，造成在佈植區和非佈植區上磊晶層的成長速率不同而導致選擇性成長。從元件製作的角度來看，此一技術可以省去一道乾式蝕刻製程，除此之外還可以因選擇性成長技術自然形成特定方向的晶格斜面，增加發光二極體發光效率。
在實驗結果方面，經由穿透式電子顯微鏡分析，證實再成長的磊晶層，不管是在佈植區或非佈植區上方皆為單晶，推測可能導致佈植區上方成長的起始點的原因有兩個:第一個為多重量子井中的Well層，即氮化銦鎵，第二個為 LED結構當中作為電子阻擋層(Electron Blocking Layer, EBL)的氮化鋁鎵（p-AlGaN）。
前述推論可由當結構是氮化鎵紫外光檢測器(無鋁、無銦)時，在佈植區上方並沒有再成長氮化鎵，由這個事實加以佐證，當我們結構為發光二極體時，再成長時佈植區會有氮化鎵材料成長上去，進而導致LED結構不是正常的p-n接面，影響後續發光二極體光電特性，而在無鋁、無銦的氮化鎵紫外光檢測器上就不會有這種問題發生。

In this thesis, ion implantation technique was applied to create selective-area and periodic patterns on GaN templates for the sequent growth of GaN-based LEDs. Selective-area growth (SAG) phenomenon of GaN epitaxial layers on the implanted GaN template(IGT) was attributed to the initial nucleation of GaN on the implantation-free regions rather than on the Si-implanted regions. That is, the GaN growth rate on the implanted regions was markedly lower than that on the implantation-free regions. The discrepancy in the growth rate was due to the different lattice constants between the implantation-free and the Si-implanted regions. In principle, the proposed approach could achieve oblique sidewall facets in the periphery of GaN-based LEDs for the improvement of light-extraction efficiency(LEE). In contrast to previous reports, the mask layer, such as SiO2, in this design was not necessary for achieving SAG of epitaxial layers on an n-GaN template layer. In addition, this approach has other advantages, including its simple processing and low cost due to the cut out of dry etching procedure. The detailed processing procedures and related results, including the electrical and optical properties of the fabricated LEDs, are discussed in following pparagraphes.

摘要 Ⅰ
ABSTRACT Ⅱ
致謝 Ⅲ
目錄 Ⅳ
表目錄 Ⅷ
圖目錄 Ⅸ
第一章 序論 1
1.1前言 1
1.2研究動機與目的 3
第二章 基礎理論、製程設備與量測儀器 6
2.1 發光二極體(Light Emitting Diodes, LEDs) 6
2.1.1 發光二極體(Light Emitting Diodes, LEDs)原理 6
2.1.2 光萃取效率(Light Extraction Efficiency, LEE)原理 7
2.1.3 傳輸線模型理論(Transmission Line Model, TLM) 9
2.2 離子佈植(Ion-implanted) 12
2.3 製程設備簡介 14
2.3.1 有機金屬氣相磊晶(Metal Organic Vapor Phase Epitaxy, MOVPE) 14
2.3.2 黃光微影(Photo lithography) 14
2.3.3 電子束蒸鍍機(Electron beam evaporator) 15
2.2.4 感應耦合式電漿 (Inductive Coupled Plasma, ICP) 15
2.2.4電漿輔助化學氣相沉積(Plasma Enhanced Chemical VaporDeposition, PECVD) 16
2.3.6 高溫爐管(Furnace) 16
2.4 量測儀器簡介 16
2.4.1 光輸出功率(Light Output Power, LOP)量測 16
2.4.2 電流與電壓(Current-Voltage, I-V)量測 17
2.4.3 掃描式電子顯微鏡(Scanning Electron Microscopy, SEM) 17
2.4.4高解析場發射掃描穿透式電子顯微鏡(High-Resolution Transmission Electron Microscopy, HR-TEM) 17
2.4.5微光顯微鏡(Emission microscope, EMMI) 18
第三章 實驗方法與製程步驟 19
3.1 選擇性佈植與再成長應用於氮化鎵發光二極體 19
3.1.1 選擇性佈植於n型氮化鎵製作 19
3.1.2 選擇性再成長氮化鎵發光二極體磊晶層 21
3.2選擇性佈植與再成長應用於氮化鎵發光二極體製程 22
3.2.1 透明導電薄膜層(TCL)製程 22
3.2.2 熱處理(Thermal Annealing)製程 24
3.2.3 金屬電極層製程 24
3.3 標準氮化鎵發光二極體製程 26
3.3.1高台蝕刻(Mesa etching)製程 26
3.3.2透明導電薄膜層(TCL)製程 28
3.3.3 熱處理(Thermal Annealing)製程 29
3.3.4 金屬電極層製程 30
3.2 選擇性佈植與再成長應用於無鋁(Al-free)氮化鎵發光二極體製程 32
3.4.1 透明導電薄膜層(TCL)製程 32
3.4.2 熱處理(Thermal Annealing)製程 33
3.4.3 金屬電極層製程 34
3.5 標準無鋁(Al-free)氮化鎵發光二極體製程 36
3.5.1高台蝕刻(Mesa etching)製程 36
3.5.2透明導電薄膜層(TCL)製程 37
3.5.3 熱處理(Thermal Annealing)製程 39
3.5.4 金屬電極層製程 39
第四章 實驗結果與討論 41
4.1 選擇性佈植和再成長氮化鎵發光二極體分析 41
4.2 選擇性佈植與選擇性再成長氮化鎵發光二極體光電分析 43
4.2.1 TLM量測 43
4.2.2 電壓-電流量測 43
4.2.3 微光顯微鏡量測 44
4.2.4 光輸出功率量測 44
4.3 選擇性佈植和再成長無鋁氮化鎵發光二極體分析 45
4.4 選擇性佈植和再成長無鋁氮化鎵發光二極體光電分析 47
4.4.1 TLM量測 47
4.4.2 電壓-電流量測 47
4.4.3 微光顯微鏡量測 48
4.4.3 光輸出功率量測 48
4.5 選擇性佈植和再成長氮化鎵紫外光檢測器 48
第五章 結論 49
參考文獻 86

1.S. Nakamura, T. Mukai, and M. Senoh, “Candelaclass highbrightness InGaN/AlGaN doubleheterostructure bluelight emitting diodes,” Appl. Phys. Lett. 64, 1687 (1994)
2.S. Nakamura and G. Fasol, “The Blue Laser Diodes”, Springer (1997)
3.Shuji Nakamura, Masayuki Senoh, Naruhito Iwasa, Shin-ichi Nagahama, Takao Yamada, Takashi Mukai, “Superbright Green InGaN Single-Quantum- Well-Structure Light-Emitting Diodes,” Jpn. J. Appl. Phys. 34, L1332 (1995)
4.S. J. Chang, W. C. Lai, Y. K. Su, J. F. Chen, C. H. Liu, and U. H. Liaw, “AlGaN/GaN Modulation-Doped Field-Effect Transistors with An Mg-doped Carrier Confinement Layer,” IEEE J. Sel. Top. Quantum Electron. 8, 278 (2002)
5.E. F. Schubert and J. K. Kim, Science 308, 1274 (2005)
6.施敏，半導體元件物理與製作技術第二版，國立交通大學出版社，2002出版。
7.J. Wu, W. Walukiewicz, K. M. Yu, J. W. Ager, E. E. Haller, H. Lu, W. J. Schaff, Y. Saito, and Y. Nanishi, “Unusual properties of the fundamental band gap of InN,” Appl. Phys. Lett. 80, 3967 (2002)
8.J. Wu, W. Walukiewicz, K. M. Yu, J. W. Ager, E. E. Haller, Hai Lu, and William J. Schaff, “Small band gap bowing in In1-xGaxN alloys,” Appl. Phys. Lett. 80, 4741 (2002)
9.E. F. Schubert, “Light-Emitting Diodes,” Cambridge University Press (2006)
10.W. C Johnson, J. B. Parsons, and M. C. Crew, “Nitrogen Compounds of Gallium. III,” J. Phys. Chem. 36, 2561 (1932)
11.H. Amano, N. Sawaki, I. Akasaki, and Y. Toyoda, “Metalorganic vapor phase epitaxial growth of a high quality GaN film using an AlN buffer layer,” Appl. Phys. Lett. 48, 353 (1986)
12.S. Nakamura, “GaN Growth Using GaN Buffer Layer,” Jpn. J. Appl. Phys. 30, L1705 (1991)
13.H. Amano, M. Kito, K. Hiramatsu, and I. Akasaki, “P-Type Conduction in Mg-Doped GaN Treated with Low-Energy Electron Beam Irradiation,” Jpn. J. Appl. Phys. 28, L2112 (1989)
14.S. Nakamura, N. Iwasa, M. Senoh, T. Mukai, “Hole Compensation Mechanism of P-Type GaN Films,” Jpn. J. Appl. Phys. 31, 1258 (1992)
 
15.S. Nakamura, T. Mukai, and M. Senoh, “Candela-class high-brightness InGaN/AlGaN double-heterostructure blue-emitting diodess,” Appl. Phys. Lett. 64, 1687 (1994)
16.A. Watanabea, T. Takeuchib, K. Hirosawab, H. Amanob, K. Hiramatsu, I. Akasakib, “The growth of single crystalline GaN on a Si substrate using AlN as an intermediate layer,” Elsevier, 128(1), 391 (1993)
17.V. K. Lazarov, J. Zimmerman, S. H. Cheung, L. Li, M. Weinert, and M. Gajdardziska-Josifovska, “Selected growth of cubic and hexagonal GaN epitaxial films on polar MgO (111) , ” Phys. Rev. Lett. 94, 216101 (2005)
18.E. S. Hellman, Z. L. Weber, and D. Buchanan, “Epitaxial growth and orientation of GaN on (100) gamma-LiAlO2,” MRS Internet J. Nitride Semicond. Res., 2, 30 (1997)
19.F. Hamdani, A. Botchkarev, W. Kim, H. Morkoc, M. Yeadon, J. M. Gibson, S.-C. Y. Tsen, David J. Smith, D. C. Reynolds, D. C. Look, K. Evans, C. W. Litton, W. C. Mitchel, and P. Hemenger, “Optical properties of GaN grown on ZnO by reactive molecular beam epitaxy,” Appl. Phys. Lett. 70, 467 (1997)
20.Kuramata, A. Horino, Kazuhiko; Domen, Kay; Shinohara, Kouji; Tanahashi, T. “High‐quality GaN epitaxial layer grown by metalorganic vapor phase epitaxy on (111) MgAl2O4 substrate,” Appl. Phys. Lett. 67, 2521 (1995)
21.郭浩中，賴芳儀，郭守義，LED 原理與應用，五南圖書，九十八年出版。
22.Fitzgerald, E.A. Watson, G.P.; Proano, R.E.; Ast, D.G.; Kirchner, P.D.; Pettit, G.D.; Woodall, J.M. “Nucleation mechanisms and the elimination of misfit dislocations at mismatched interfaces by reduction in growth area,” J. Appl. Phys. 65, 2220 (1989)
23.Schubert, E. F.; Hunt, N. E. J. “15000 hrs stable operation of resonant cavity light emitting diodes,” Appl. Phys. 66, 319 (1998)
24.K. Tadatomo, H. Okagawa, Y. Ohuchi, T. Tsunekawa, T. Jyouichi, Y. Imada, M. Kato, H. Kudo, T. Taguchi, “High Output Power InGaN Ultraviolet Light-Emitting Diodes Fabricated on Patterned Substrates Using Metalorganic Vapor Phase Epitaxy,” physica status solidi, 188(1), 12 (2001)
25.Shota Kitamura, Kazumasa Hiramatsu, Nobuhiko Sawaki, “Fabrication of GaN Hexagonal Pyramids on Dot-Patterned GaN/Sapphire Substrates via Selective Metalorganic Vapor Phase Epitaxy,” Jpn. J. Appl. Phys. 34, L1184 (1995).
26.Lee, Y. J.; Hwang, J. M.; Hsu, T. C.; Hsieh, M. H.; Jou, M. J.; Lee, B. J.; Lu, T. C.; Kuo, H. C.; Wang, S. C. “Enhancing the Output Power of GaN-Based LEDs Grown on Wet-Etched Patterned Sapphire Substrates,” IEEE Photonics Technology Letters, 18(10), 1152 (2006)
 
27.T. Fujii, Y. Gao, R. Sharma, E. L. Hu, S. P. DenBaars, and S. Nakamura, “Increase in the extraction efficiency of GaN-based light-emitting diodes via surface roughening,” Appl. Phys. Lett. 84, 855, 2004.
28.Jinn-Kong Sheu, Y. S. Lu, Min-Lum Lee, W. C. Lai, C. H. Kuo, and Chun-Ju Tun, “Enhanced efficiency of GaN-based light-emitting diodes with periodic textured Ga-doped ZnO transparent contact layer,” Appl. Phys. Lett. 90, 263511 (2007)
29.M. R. Krames, M. Ochiai-Holcomb, G. E. Hofler, C. Carter-Coman, E. I. Chen,I.-H. Tan, P. Grillot, N. F. Gardner, H. C. Chui, J.-W. Huang, S. A. Stockman, F. A. Kish, M. G. Craford, ” High-power truncated-inverted-pyramid (AlxGa1-x)0.5In0.5P/GaP light-emitting diodes exhibiting≫ 50% external quantum efficiency,” Appl. Phys. Lett. 75, 2365 (1999)
30.郭桓卲，利用選擇性成長及側壁蝕刻方式增加氮化鎵系列藍光發光二極體光輸出功率之研究，國立成功大學光電科學與工程研究所，碩士論文 (2010)。
31.Jinn-Kong Sheu, Kuo-Hua Chang, Shang-Ju Tu, Ming-Lun Lee, Chih-Ciao Yang, Che-Kang Hsu, and Wei-Chih Lai, “InGaN light-emitting diodes with oblique sidewall facets formed by selective growth on SiO2 patterned GaN film,” Optics Express, 18(S4), A562 (2010)
32.郭浩中，賴芳儀，郭守義，LED原理與應用，五南圖書，九十八年出版。
33.陳盈宏，利用空隙陣列結合圖案化基板改善氮化鎵發光二極體之光電特性，國立成功大學光電科學與工程研究所，碩士論文(2011)。
34.S. J. Chang, C. S. Chang, Y.K. Su, P. T. Chen, Y. R. Wu, K. H. Huang, and T. P. Chen, “AlGaInP yellow-green light-emitting diodes with a tensile strain barrier cladding layer,” IEEE Photon. Technol. Lett. 9(9), 1199 (1997)
35.高國峯，GaN-LED 晶片結構對光萃取效率影響的研究，國立中央大學光電科學研究所，碩士論文(2005)。
36.馬景時，氮化鎵藍色發光二極體透明電極之製作與研究，國立中央大學光電科學研究所，碩士論文(2001)
37.K. V. Vassilevski, M. G. Rastegaeva, A. I. Babanin, I. P. Nikitina, and V.A.Dmitriev, “Fabrication of GaN mesa structures,” MRS Internet J. Nitride Semicond. Res. 1,38(1996)
38.陸大成，段樹坤，金屬有機化合物氣相外延基礎及應用(簡體)，科學出版社，(2009)
39.杜尚儒，透明導電膜沉積於矽基板之異質接面太陽能電池研究，南台科技大學光電工程研究所，碩士論文(2008)。
40.Hong Xiao，半導體製程技術導論第二版第二刷，學銘圖書有限公司，2003出版。
41.葉育翔，選擇性成長方法應用於倒置型p-i-n偵測器成長在p-GaN之研究，南台科技大學光電工程研究所，碩士論文(2011)。
42.張詠翕，以聚焦離子束製程的AlGaN/GaN量子結構之研究，國立中山大學物理學系研究所，碩士論文(2009)。
43.楊亞諭，光致電化學氧化與壓印技術於氮化物發光二極體之研究，國立成功大學光電科學與工程研究所，碩士論文(2009)。
44.國立成功大學微奈米科技研究中心網頁
45.黃順源，高亮度發光二極體之研製，南台科技大學光電工程研究所，碩士論文(2010)。
46.杜尚儒，離子佈植技術應用於氮化鎵系列發光二極體，成功大學光電科學與工程學系，博士論文(2012)。
47.http://www.srim.org/SRIM/SRIMINTRO.htm
48.馮天璟，磁控濺鍍銦錫氧化物於P型氮化鎵之歐姆接觸與光電特性分析，成功大學光電科學與工程學系，碩士論文(2012)。
49.J. K. Sheu, Y. K. Su, G. C. Chi, P. L. Koh, M. J. Jou, C. M. Chang, C. C. Liu, and W. C. Hung, “High-transparency Ni/Au ohmic contact to p-type GaN,” Appl. Phys. Lett. 74, 2340 (1999)
50.K. Kiruma, T. Haga, and M. Miyazaki, “Surface migration and reaction mechanism during selective growth of GaAs and AlAs by metalorganic chemical vapor deposition,” J. Cryst. Growth, 102(4), 717 (1990)
51.張國華，局部再成長方法應用於有機金屬氣相磊晶成長氮化鎵系列光電元件之研究，國立成功大學光電科學與工程研究所，博士論文(2010)。
52.Wai Kin CHim, “Semiconductor Device and Failure Analysis using photon Emission Microscopy,” WILEY(2000)