直接成長二維材料:從成長控制、材料鑑定及免轉移製程之元件應用

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研究生：	陳雨澤 Chen, Yu Ze
論文名稱：	直接成長二維材料:從成長控制、材料鑑定及免轉移製程之元件應用 Direct Growth of 2D Materials: From Controllable Growth to Material Characterizations and Transfer-Free Device Applications
指導教授：	闕郁倫 Chueh, Yu Lun
口試委員:	戴念華 Tai, Nyan Hwa 邱博文 Chiu, Po Wen 張文豪 Chang, Wen Hao 蘇清源 Su, Ching Yuan 林麗瓊 Lin, Li Chyong 陳貴賢 Chen, Kuei Hsien
學位類別：	博士 Doctor
系所名稱：	工學院 - 材料科學工程學系 Materials Science and Engineering
論文出版年：	2016
畢業學年度：	104
語文別：	英文
論文頁數：	187
中文關鍵詞：	直接成長、二維材料、免轉移
外文關鍵詞：	direct growth, 2D materials, transfer-free
相關次數：	點閱：3 下載：0
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自從2004年科學家成功於石墨剝離出一個原子層厚度的碳膜，其優異的表現激發了科學家的熱情以及好奇。由於石墨烯在各方面，如:光、電、熱，都表現出驚人的表現，因此石墨烯被視為極具高發展潛力的材料。由於化學氣相沉積法在銅片上製備出大面積單層石墨烯的成功，推向市場的目標又更進一步。然而，為了後續的應用，轉移石墨烯於目標基板的步驟是不可避免的，這卻也造成石墨烯品質的犧牲。因此，為了解決此問題，我們發展出以銅蒸氣輔助，直接於目標基板上沉積石墨烯的技術，以及提出新的成長機制。
取代ITO並應用於透明導電膜，一直是石墨烯受到高度矚目的原因之一。但是，石墨烯的導電率仍然無法跟ITO匹敵。我們成功結合金屬網絡與石墨烯，不僅大幅提升導電率，並且由於石墨烯的保護，提高了此複合材料在嚴峻條件下的操作穩定度。
雖然石墨烯被寄予厚望，但天生零能隙的電子結構，阻礙了場發效電晶體的應用。因此，同樣具備層狀結構的過渡金屬二硫化物吸引了大家的目光，更令人興趣的是它天生的電子能隙。傳統上，常用化學氣相沉積法於爐管製備材料，但其製程時間長、高熱預算。本論文中，我們利用先進儀器，如:雷射、微波系統，實現了直接成長少層於任一基板，並且具備快速、低熱預算的優點。另一特點，除了平行基板的堆疊方向的過渡金屬二硫化物，受到大家的注目外，近年來，不論是理論計算或是實驗數據，皆指出具備垂直結構的過渡金屬二硫化物，在電化學的應用上具有高度潛力。本論文中，我們成功以微波系統，在短時間內(3分鐘)，製備出垂直結構的過渡金屬二硫化物，並且製備感測器，經由實驗數據，證明出應用於電化學上的潛力。

Since 2004, scientists successfully exfoliated one-atomic layer carbon layer from graphite, namely graphene, this incredible material had been triggered our passion and enthusiasm until now. Owing to the fabulous properties of various aspects such as optical, electrical, thermal, graphene is highly expected a potential material in all respects. Monolayer and large area of graphene on Cu via chemical vapor deposition (CVD) process make a notable step toward pushing graphene into market. However, the inevitable transfer process badly sacrificed the quality of graphene, hindering the following application. To address this issue, we successfully develop a direct deposition of graphene by means of gaseous catalytic species, Cu vapor, as well as established the mechanism from the view point of Cu vapor.
Transparent conducting film is the main target of using graphene for replacing conventional ITO. Nevertheless, the conductivity was still far behind ITO by far. We combined metal meshes with covering graphene, not only improving conductivity as good as ITO but also enhancing the stability in harsh environment by graphene shielding.
Thanks to the great development of graphene, transition metal dichalcogenide was also attracted everyone’s attention due to the similar layer structure and its nature band gap property. Differencing with conventional CVD process via furnace, we firstly exploited advanced technique, such as laser, microwave system, to aim for fast and low temperature growth. Moreover, we fabricated the vertical structure of MoS2 with exposing edges via microwave system, and further proved its highly active property in which benefited the application of electrochemistry field.

Abstract in Chinese    i
Abstract    ii
Acknowledgements    iii
Chapter  1    Rise of two dimensional materials: graphene, single layer of transition metal dichalcogenide    1
1 Graphene    1
1.1 Transparent Conductive Materials    2
1.2 The manufacturing process of graphene    4
1.2.1 Mechanical Exfoliation    4
1.2.2 Intercalation by metal particles    5
1.2.3 Exfoliation by immersing in the organic solution    7
1.2.4 Reduction of Graphene oxide    7
1.2.5 Thermo-decomposition of SiC into graphene    9
1.2.6 Chemical vapor deposition    9
2    Transition Metal Dichalcogenides (TMDs)    11
2.1 The atomic structure of TMDs    11
2.2 Single layer of TMDs    13
2.3 The practical application based on TMDs    18
2.3.1 Lubricants    18
2.3.2 Hydrodesulfurization catalysts    20
2.3.3 Li-ion batteries    22
2.3.4 Hydrogen evolution reaction    25
2.4 The manufacturing process of few- and mono- layer of TMDs    29
2.4.1 Mechanical Exfoliation    29
2.4.2 Lithium-based intercalation    30
2.4.3 Plasma-thinning process and Laser-thinning process    31
2.4.4 Thermolysis of WSe2    34
2.4.5 Direct deposition of MoS2 by pulsed laser deposition (PLD)    35
2.4.6 Synthesis of monolayer TMDs by chemical vapor deposition (CVD)    36
3 Motivations    39
Chapter  2     The role of Cu vapor on the synthesis of graphene grew on Cu foils    41
1    Methods    41
1.1    Aging quartz tube with condensed Cu vapor    41
1.2    Growing graphene on Cu foils for evaporation test    43
2    Results and Discussion    44
2.1    The proof of Cu vapor existed during the graphene growing    44
2.2    Dual role of Cu vapor played during the formation of graphene    48
2.3    Mechanism    53
2.4    Directly growing graphene on oxide substrate (gas phase)    55
3    Conclusion    57
Chapter     3 Direct transformation of amorphous carbon Film into  graphene/graphite on onsulators via Cu mediation engineering and its application on all-Carbon based device    58
1    Methods    58
1.1    Transformation of amorphous carbon to graphene    58
1.2 Fabrication of electrical devices made of carbon materials.    58
2    Results and Discussion    59
2.1    The influence of Cu vapor on the phase transformation from amorphous to crystalline during annealing    59
2.2    The thickness control of resulting graphene/graphite by pre-deposited amorphous carbon    62
2.3    X-ray photoemission spectroscopy analysis in depth    67
2.4    Large area, patternable graphene and electrical performance    71
2.5    Demonstration of all carbon-based devices    74
2.6    Mechanism    76
3 Conclusion    80
Chapter     4  Low temperature growth of graphene on glass by carbon-enclosed chemical vapor deposition process and its application as transparent electrode in the harsh environment    81
1    Methods    81
1.1    Chemical vapor deposition (CE-CVD)    81
1.2    Fabrications of graphene Field-Effect Transistors    81
1.3    Fabrications of metal mesh shielded with graphene    82
2    Results and Discussion    83
2.1    The schematics of low temperature CE-CVD process for the growth of monolayer graphene with high quality    83
2.2    The quality and coverage of resulting graphene w/ and w/o underlying graphite plate    86
2.3    The electrical performance    94
2.4    Mechanism and its availability of coating NWs    95
2.5    Synthesis of graphene on a ultrathin metal grid deposited directly on commercial optical glass    99
2.6    Anti-oxidation and Anti-corrosion tests    104
3 Conclusions    109
Chapter    5  Ultrafast and low temperature synthesis of highly crystalline and patternable few-layers tungsten diselenide by laser irradiation assisted-selenization process    110
1    Methods    110
1.1    Sample preparation and Laser-irradiation    110
2    Results and Discussion    111
2.1    The schematics of formation of WSe2 via laser irradiation assisted-selenization    111
2.2    Material characterization: optical contrast, Raman spectra and mapping, photoluminescence spectrum    114
2.3    Cross-sectional TEM image of few layers of WSe2    117
2.4    Evolution of WSe2 from amorphous to crystalline and growth window    119
2.5    X-ray photoemission spectroscopy    123
2.6    Patternable WSe2    125
2.7    One step synthesis of WSe2-FET devices    128
2.8    Synthesis of MoSe2 via LIAS    130
3    Conclusion    132
Chapter 6     Low temperature and ultrafast synthesis of patternable few-layers transition metal dichacogenides with controllable stacking alignment by microwave-assisted selenization process    133
1    Methods    133
1.1    Sample preparation and Microwave assisted-selenization process.    133
1.2    Characterizations.    133
2    Results and Discussion    135
2.1    The schematics of formation of WSe2 via microwave- assisted-selenization    135
2.2    XPS analysis of Raman mapping of WSe2 and MoSe2    138
2.3    Growth window for the reduction of WO3 film to few-layers WSe2    141
2.4    Patternability of WSe2    143
2.5    Formation of vertical MoS2 via microwave treatment and possible mechanism    148
2.6    Vertical Structure WSe2-Based Gas Sensor    153
2.7    Conclusions    155
Chapter     7 Future Work    156
References    163
 

                                

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