本研究使用化學氣相沉積法(Chemical Vapor Deposition, CVD)生長的大面積的MoS2/sapphire基板，接著在基板上使用分子束磊晶(Molecular beam epitaxy, MBE)法成長氮化鎵薄膜，探討不同參數對氮化鎵化合物半導體的影響，目標成長出大面積且品質良好的氮化鎵薄膜。
實驗總共分為不同鎵鍍源溫度、有無緩衝層、有無退火、有無緩衝層或退火和預鎵或預氮等系列。磊晶薄膜時以反射式高能量電子繞射儀(Reflection High Energy Electron Diffraction，RHEED)可即時監控薄膜表面形貌的變化，原子力顯微鏡（Atomic Force Microscope，AFM）可測量薄膜表面粗糙度，場發射掃描式電子顯微鏡(Field Emission Scanning Electron Microscope，FE-SEM)可測量薄膜表面影像，拉曼光譜(Raman spectroscope)、光致發光螢光光譜(Photoluminescence spectroscope，PL)及X射線光電子能譜（X-ray photoelectron spectroscopy，XPS）可量測薄膜材料的光學特性與鍍膜品質。
最後結果顯示，提高鎵鍍源溫度，成長緩衝層、預鎵處理可強化氮化鎵薄膜的光學訊號、成長出明顯的六方晶結構。

In this study, we used chemical vapor deposition (CVD) to grow a large area MoS2 on 2-inch sapphire as substrate, and then GaN thin films were grown on MoS2/sapphire by plasma-assisted molecular beam epitaxy (PA-MBE). We try to investigate effects of deposition parameters on the properties of GaN films in order to have a large area and high quality GaN/MoS2 heterostructure thin films.
To optimize the quality of Ga thin films on MoS2 layers, the MBE growth was conducted at different temperatures of Ga cell, with low-temperature buffer layer, with annealing treatment, and the substrate with pre-gallium or pre-nitrogen treatments. During the growth, the Reflection High Energy Electron Diffraction (RHEED) can help us to monitor the surface condition of samples. After the growth, Atomic Force Microscope (AFM), Field Emission Scanning Electron Microscope (FE-SEM), Raman spectroscope, Photoluminescence spectroscope (PL) and X-ray photoelectron spectroscopy (XPS) were applied to analyze the morphology, structure and quality of GaN thin films.
In summary, higher gallium-cell temperature, buffer layer and pre-gallium treatment on the substrate were better for the MBE growth that enhanced the optical properties of GaN thin films on CVD MoS2 layers.

第一章 諸論 1
1.1 前言 1
1.2 氮化鎵介紹 2
1.3 二維材料介紹 3
(1) 石墨烯 3
(2) 二硫化鉬 4
1.4 文獻回顧 5
1.5 研究動機 13
第二章 儀器介紹與原理 15
2.1 電漿輔助式分子束磊晶系統　(Plasma-Assisted Molecular Beam Epitaxy, PA-MBE) 15
2.1.1 真空腔體與汞浦裝置 16
2.1.2 材料源與磊晶裝置 17
2.1.3 附屬裝置 18
2.2 反射式高能量電子繞射儀 (Reflection High Energy Electron Diffraction, RHEED) 20
2.3 高解析 X 光繞射儀 (High Resolution X-ray Diffraction, HRXRD) 22
2.4 場發射掃描式電子顯微鏡 (Field Emission Scanning Electron Microscopy, FE-SEM) 24
2.5 原子力顯微鏡 (Atomic force microscopy, AFM) 27
2.6 拉曼光譜 (Raman spectroscopy) 29
2.7 光致發光螢光光譜(Photoluminescence spectroscopy, PL) 31
2.8 X 射線光電子能譜(X-ray photoelectron spectroscopy,XPS) 33
第三章 實驗流程與方法 35
3.1 鎵鍍源流量的測量 35
3.2 二硫化鉬基板製作 38
3.3 基板清洗 39
3.4 開始磊晶 40
第四章 實驗結果與討論 43
4.1 不同鎵鍍源溫度對氮化鎵成膜品質的影響 43
4.1.1 實驗結果與討論 44
4.1.2 不同鎵鍍源溫度對磊晶氮化鎵之結論 53
4.2 有無緩衝層對氮化鎵成膜品質的影響 54
4.2.1 實驗結果與討論 55
4.2.2 有無緩衝層磊晶氮化鎵之結論 63
4.3 有無退火對氮化鎵成膜品質的影響 64
4.3.1 實驗結果與討論 64
4.3.2 有無退火磊晶氮化鎵之結論 73
4.4 有無緩衝層和退火對氮化鎵成膜品質的影響 74
4.4.1 實驗結果與討論 74
4.4.2 有無緩衝層和退火磊晶氮化鎵之結論 82
4.5 預鎵或預氮對氮化鎵成膜品質的影響 83
4.5.1 實驗結果與討論 83
4.5.2 預鎵和預氮磊晶氮化鎵之結論 91
第五章 結論 93
第六章 未來工作 95
參考資料 97
附錄 103

[1] F.A. Ponce, D.P. Bour, Nitride-based semiconductors for blue and green light-emitting devices, Nature (1997) 386:351–359.
[2] H.C. Wang, M.C. Chen, Y.S. Lin, Optimal silicon doping layers of quantum barriers in the growth sequence forming soft confinement potential of eight-period In0.2Ga0.8N/GaN quantum wells of blue LEDs, Nanoscale Res Lett (2017) 12.
[3] X. Zhou, T. Lu, Y. Zhu, Surface morphology evolution mechanisms of InGaN/GaN multiple quantum wells with mixture N2/H2-grown GaN barrier, Nanoscale Res Lett (2017) 12.
[4] S. Nakamura, M. Senoh, S. Nagahama, InGaN-based multiquantum-well-structure laser diodes, Jpn J Appl Phys (1996) 35 L74–L76.
[5] A.J. Tzou, K.N. Chu, L.F. Lin, AlN surface passivation of GaN-based high electron mobility transistors by plasma-enhanced atomic layer deposition, Nanoscale Res Lett (2017) 12
[6] F. Li, S.H. Lee, J.H. You, T.W. Kim, K.H. Lee, J.Y. Lee, T.W. Kang, UV photovoltaic cells fabricated utilizing GaN nanorod/Si heterostructures, Journal of Crystal Growth, 312(16) (2010) 2320-2323.
[7] S.J. Pearton, J.C. Zolper, R.J. Shul, F. Ren, GaN: Processing, defects, and devices, Journal of applied physics, 86(1) (1999) 1-78.

[8] Q.H. Wang, K. Kalantar-Zadeh, A. Kis, J.N. Coleman, M.S. Strano, Nat. Nanotechnol. 7, 699 (2012).
[9] K.S. Novoselov, A.K. Geim, S.V. Morozov, D. Jiang, Y. Zhang,S.V. Dubonos, I.V. Grigorieva, A.A. Firsov, Science (2004) 306,666.
[10] K.S. Novoselov, A.K. Geim, S.V. Morozov, D. Jiang,M.I. Katsnelson, I.V. Grigorieva, S.V. Dubonos, A.A. Firsov, Nature (2005) 438, 197.
[11] https://zh.wikipedia.org/wiki/%E6%B0%AE%E5%8C%96%E9%8E%B5#/media/File:Wurtzite_polyhedra.png
[12] 陳宗廷，在GaN上以電漿輔助分子束磊晶成長之高銦組成氮化銦鎵/氮化鎵量子井特性研究，國立中山大學物理研究所 碩士論文，民國102 年8 月
[13] B. Radisavljevic, A. Radenovic, J. Brivio, etal., Single-layer MoS2 transistors, Nature Nano technology (2011) 6:147~150.
[14] J.N. Coleman, M. Lotya, A. ONeill, Two-dimensional nanosheets produced by liquid exfoliationoflayered materials, Science(2011) 331:568~571.
[15] C. Lee, Measurement of the Elastic Properties and Intrinsic Strength of MonolayerGraphene,.Science (2008) 321(5887):385.
[16] N.D. Mermint, Phys. Rev. (1968) 176, 250.
[17] Y. Peng, Z. Meng, C. Zhong, J. Lu, W. Yu, Y. Jia, Y. Qian, Chem. Lett. (2001) 30, 772.



[18] S.Z. Butler, S.M. Hollen, L. Cao, Y. Cui, J.A. Gupta, H.R. Gutierrez, T.F. Heinz, S.S. Hong, J. Huang, A.F. Ismach, E. Johnston-Halperin, M. Kuno, V. V. Plashnitsa, R.D. Robinson,R.S. Ruoff, S. Salahuddin, J. Shan, L. Shi, M.G. Spencer, M. Terrones, W. Wind, J.E. Goldberger, ACS Nano (2013) 7, 2898.
[19] A. Kuc, N. Zibouche, T. Heine, Influence of quantum confinement on the electronic structure of the transition metal sulfide TS2, Physical Review B (2011) 83: 245213 ~ 245216.
[20] A. Yamada, K.P. Ho, T. Maruyama, K. Akimoto, Molecular beam epitaxy of GaN on a substrate of MoS2 layered compound, Institute of Materials Science (1999).
[21] Priti Gupta, Layered transition metal dichalcogenides: promising near-lattice- matched substrates for GaN growth, Scientific Reports, (2016).
[22] Malleswararao Tangi, Pawan Mishra, Tien Khee Ng, Determination of band offsets at GaN/single-layer MoS2 heterojunction, Applied Physics Letters 109, 032104 (2016).
[23] Yasuyuki Watanabe, Masatoshi Sano, Japanese Journal of Applied Physics logo Low-Temperature Growth of GaN Epitaxial Layers with Buffer Layers by Reactive Close-Spaced Method, Jpn. J. Appl. Phys (2003) 42 38.
[24] Xu.Zhao Chai, Dong Zhou, Bin Liu, Effect of High-Temperature Annealing on Yellow and Blue Luminescence of Undoped GaN, Chinese Physics Letters (2015)


[25] 劉耕辰，極化效應對可撓性氮化銦鎵發光二極體光電特性影響之研究，國立中興大學精密工程研究所 碩士論文，民國104 年1 月。
[26] 郭鴻毅，應用於垂直結構氮化鎵系列發光二極體製備之基板工程，國立成功大學微電子工程研究所 碩士論文，民國97年 年7 月。

Chapter 2
[27] A.Y. Cho, J.R. Arthur Jr, .Molecular beam epitaxy, Solid State Chem (1975) 10: 157–192.
[28] J. Osaka, M. Senthil Kumar, H. Toyoda, T. Ishijima, H. Sugai, T. Mizutani, Role of atomic nitrogen during GaN growth by plasma-assisted molecular beam epitaxy revealed by appearance mass spectrometry, Applied physics letters, 90(17),172114.
[29] J. M. Myoung, O. Gluschenkov, K. Kim, S. Kim, Growth kinetics of GaN and effects of flux ratio on the properties of GaN films grown by plasma-assisted molecular beam epitaxy,Journal of Vacuum Science & Technology A: Vacuum,Surfaces, and Films, 17(5), 3019-3028.
[30] M. D. Szata, Analysis of RHEED pattern from semiconductor surfaces, Materials chemistry and physics, 81(2), 257-259.
[31] http://www.reocities.com/CapeCanaveral/5702/Fe_Si.html
[32] S. Andrieu, P. Fréchard, What information can be obtained by RHEED applied on polycrystalline films, Surface science, 360(1-3), 289-296.
[33] http://www.academia.edu/16183346/MLE2101_Lab_Report
[34] http://www.ou.edu/research/electron/bmz5364/resolutn.html
[35] 羅聖全，科學基礎研究之重要利器_掃描式電子顯微鏡，科學研習，2013 年 5 月，No. 52-5。
[36] http://www.wunan.com.tw/www2/download/preview/5E57.PDF
[37] http://www.mdu.edu.tw/~yinyu/contributions/SEM-EDS%20readouts.pdf
[38] https://zh.wikipedia.org/wiki/%E6%89%AB%E6%8F%8F%E7%94%B5%E5%AD%90 %E6%98%BE%E5%BE%AE%E9%95%9C
[39] 李其紘，原子力顯微鏡的基本介紹，科學研習，2013 年5 月，No. 52-5。
[40] http://www.coretechint.com/technical_info-xps.php?lang=2
[41] Retrieved March 13th, 2017, from URL
[42] https://zh.wikipedia.org/wiki/%E6%8B%89%E6%9B%BC%E5%85%89%E8%AD%9C%E5%AD%B8
[43] http://labguide.com.tw/user/w016267551/uploads/1246937317.pdf
[44] http://www.teo.com.tw/brand.asp?lv=0&id=70
[45] http://www.ym.edu.tw/biophotonics-ultrasound-lab/research/yensen_2.htm
[46] http://www.tnu.edu.tw/ee/upimages/file/Std-97/1004/%E5%B0%88%E9%A1%8C%E4%BB%8B%E7%B4%B9/A_3.htm
[47] http://www.tnu.edu.tw/ee/upimages/file/Std-97/1004/%E5%B0%88%E9%A1%8C%E4%BB%8B%E7%B4%B9/A_3.htm
Chapter 4
[48] Sunwoon Kima, Jeongtak Oha, Joongseo Kanga, Dongjoon Kima, Jonghak Wona, Je Won Kima, Hyung-Koun Cho, Two-step growth of high quality GaN using V/III ratio variation in the initial growth stage, Journal of Crystal Growth 262 (2004) 7–13.
[49] A. Michael, Reshchikova, Hadis Morkoç, Luminescence properties of defects in GaN, Journal of Applied Physics 97, 061301 (2005).
[50] Dharanipal Doppalapudi, Theodore D. Moustakas, Chapter 2 - Epitaxial growth and structure of III-V nitride thin films, Handbook of Thin Films Volume 4, 2002, Pages 57-115.
[51] Monu Mishra, Abhiram Gundimeda, Shibin Krishna, Neha Aggarwal, Wet chemical etching induced stress relaxed nanostructures on polar & non-polar epitaxial GaN films, Physical Chemistry Chemical Physics (2017).
[52] Wei Li,Aizhen Li, Post growth thermal annealing of GaN grown by RF plasma MBE, Journal of Crystal Growth Volumes 227–228 (2001) Pages 415-419
[53] Chai Xu-Zhao, Effect of High-Temperature Annealing on Yellow and Blue Luminescence of Undoped GaN, Chinese Phys. Lett. (2015) 32 097804.
[54] Dongsheng Li, M. Sumiya, S. Fuke, Selective etching of GaN polar surface in potassium hydroxide solution studied by x-ray photoelectron spectroscopy, Journal of Applied Physics 90, 4219 (2001).
[55] M, A, Mastro, Influence of polarity on GaN thermal stability, Journal of Crystal Growth Volume 274, Issues 1–2, 15 (2005) Pages 38-46.