在本論文中，我們透過預濺鍍過渡金屬再硫化方式成長出大面積的二硫化鉬薄膜，且經由控制濺鍍金屬時間，可以於準確控制10 層以下二硫化鉬薄膜之層數。對於較厚的鉬金屬膜，經硫化後雖可成長出層數大於 10 層之二硫化鉬薄膜，但在薄膜下方則包覆著鉬氧化物。此結果說明了，在硫化的過程中，兩種成長機制將同時發生，其一為平面二硫化鉬薄膜的成長，其二為鉬氧化物因高溫在表面的移動。此外，經過依序濺鍍過渡金屬鉬和鎢且依序硫化的方式，可以成功的製備出二硫化鉬/二硫化鎢二維晶體異質結構薄膜，轉印此二維晶體異質結構薄膜至預成長 300 奈米二氧化矽的矽基板上，透過此方式，即可製作出背閘極場效電晶體，其元件特性更勝於二硫化鉬背閘極場效電晶體。此結果表明了，二維晶體異質結構的堆疊可以克服了單一二維晶體先天上的限制並且仍然保有著二維晶體的優點，為一種具有前瞻性的材料。此外在此論文中，我們亦完成了二硫化鉬與二硫化鎢的的原子層蝕刻，對於二硫化鎢/二硫化鉬異質結構薄膜，透過重複的氧電漿蝕刻並進行再硫化之方式，可以達到上方二硫化鎢之選擇性蝕刻。另外透過重複原子層蝕刻之技術來製備二硫化鎢/二硫化鉬異質結構電晶體，可以使得源/汲電極直接接觸到二硫化鉬通道，此結果表明，二維晶體異質結構的等效選擇性蝕刻可以通過重複原子層蝕刻技術來實現，這是二維晶體異質結構元件製作上極為重要的一步。

In this thesis, we have demonstrated that large-area molybdenum disulfide (MoS2) can be prepared by sulfurizing the pre-deposited transition metal films. Good layer number controllability up to 10 layers of the MoS2 film is also achieved by controlling the sputtering times of the pre-deposited transition metal films. For the sample with thicker Mo films, although MoS2 films with the layer number larger than 10 can be obtained, clusters of multi-layer 2D crystals covering Mo oxides are obtained for the sample. The results suggest that two growth mechanisms of planar MoS2 formation and Mo oxide segregation would take place simultaneously during the sulfurization procedure. After sequential transition metal deposition and sulfurization procedures of Mo and tungsten (W), MoS2/WS2 2D crystal hetero-structures can be established. After transferring the hetero-structure film to a 300 nm SiO2/Si substrate, a bottom-gate transistor with enhanced field-effect mobility is obtained. The results have revealed that the establishment of different hetero-structures is a promising approach to overcome the limit of individual 2D crystals and still maintain their advantage. The atomic layer etchings of MoS2 and WS2 are demonstrated in this paper. By repeated oxygen plasma etchings and a final re-sulfurization procedure, multi-layer WS2 can be selectively etched off from the WS2/MoS2 hetero-structure. A WS2/MoS2 hetero-structure transistor is fabricated with source/drain electrodes contacted directly to the MoS2 channel by using the repeated atomic layer etching technique. The results have revealed that the equivalent selective etching effect for two-dimensional crystal hetero-structures can be achieved by repeating the atomic layer etching procedure, which is an important step for the device fabrication of 2D crystal hetero-structures.

摘要 I
Abstract II
目錄 IV
圖目錄 VII
第一章 緒論 1
1-1 二硫化鉬晶體結構與性質 1
1-2 二硫化鉬之拉曼光譜 2
1-3 二硫化鉬之光激螢光光譜 2
1-4 二硫化鉬薄膜之製備方式 3
1-4-1 機械剝離法 3
1-4-2 電化學分離法 4
1-4-3 化學氣相沉積法 4
1-5 本論文研究方向與大綱 5
第二章 實驗儀器介紹 12
2-1 薄膜成長系統 12
2-1-1 過渡金屬射頻濺鍍系統 12
2-1-2 過渡金屬硫化系統 14
2-2 薄膜分析系統 14
2-2-1 拉曼光譜儀 15
2-2-2 光激發螢光光譜儀 15
2-2-3 X光光電子能譜儀 16
2-2-4 紫外光光電子能譜儀 16
2-2-5 穿透式電子顯微鏡 17
2-3 電晶體製程儀器 17
2-3-1 反應式離子蝕刻系統 RIE (Reactive-Ion Etching) System 17
2-3-2 原子層沉積系統 ALD (Atomic Layer Deposition) System 18
2-3-3 氧電漿蝕刻系統 19
第三章 二硫化鉬和二硫化鉬/二硫化鎢異質結構薄膜成長及特性 26
3-1二硫化鉬薄膜成長 26
3-1-1 基板選擇與前處理 26
3-1-2 鉬金屬沉積 27
3-1-3 鉬金屬硫化 27
3-2 不同濺鍍時間對二硫化鉬薄膜特性 28
3-2-1 透過拉曼光譜分析不同濺鍍金屬時間之二硫化鉬薄膜 28
3-2-2 透過光激螢光光譜分析不同濺鍍金屬時間之二硫化鉬薄膜 29
3-2-3 透過穿透式電子顯微鏡分析不同濺鍍金屬時間二硫化鉬薄膜 29
3-2-4 多層二硫化鉬薄膜元素分析 30
3-2-5 二硫化鉬成長模型探討 30
3-3 二硫化鎢/二硫化鉬異質結構薄膜製備及特性 31
3-3-1 二硫化鎢/二硫化鉬異質結構薄膜樣品製備 31
3-3-2 二硫化鎢/二硫化鉬異質結構薄膜之拉曼光譜分析 31
3-3-3 二硫化鎢/二硫化鉬異質結構薄膜之光激螢光光譜分析 32
3-3-4 二硫化鉬/二硫化鎢異質結構之紫外光光電子能譜儀分析 32
3-3-5 二硫化鉬/二硫化鎢異質結構之穿透式電子顯微鏡分析 33
3-4 小結 33
第四章 二硫化鉬/二硫化鎢異質結構之電晶體特性 46
4-1 背閘極場效電晶體之製備 46
4-1-1 於基板上定義源極與汲極 46
4-1-2 薄膜轉印至源極與汲極基板 47
4-1-3 定義場效電晶體通道 48
4-2 上閘極場效電晶體製備 48
4-2-1 上Alignment Key 49
4-2-2 定義場效電晶體通道 49
4-2-3 定義源極與汲極 50
4-2-4 氧化層沉積 50
4-2-5 定義上閘極 50
4-3 二硫化鉬場效電晶體特性 51
4-3-1 單層二硫化鉬背閘極場效電晶體 51
4-3-2 三層二硫化鉬背閘極場效電晶體 52
4-3-2 三層二硫化鉬上閘極場效電晶體 52
4-4 二硫化鉬/二硫化鎢異質結構場效電晶體特性 54
4-4-1 二硫化鉬/二硫化鎢異質結構背閘極場效電晶體特性 55
4-4-2 二硫化鉬/二硫化鎢異質結構上閘極場效電晶體特性 55
第五章 利用氧電漿對於過渡金屬二硫化物異質結構進行等效選擇性蝕刻及其電晶體元件特性 67
5-1 利用氧電漿進行二硫化鉬之原子層蝕刻 67
5-1-1 二硫化鉬之原子層蝕刻拉曼光譜分析 68
5-1-2 二硫化鉬之原子層蝕刻光激螢光光譜分析 68
5-1-3 二硫化鉬之原子層蝕刻X光電子能譜分析 69
5-1-4 二硫化鉬之原子層蝕刻穿透式電子顯微鏡橫切面分析 70
5-1-5 二硫化鉬原子層蝕刻後之背閘極場效電晶體特性 70
5-2 利用氧電漿進行二硫化鉬/二硫化鎢單異質結構之等效選擇性蝕刻 71
5-2-1單異質結構之選擇性蝕刻拉曼光譜分析 71
5-2-2單異質結構之等效選擇性蝕刻光激螢光光譜分析 72
5-2-3單異質結構之選擇性蝕刻穿透式電子顯微鏡剖面分析 72
5-2-4單異質結構進行等效選擇性蝕刻之兩端點元件 73
第六章 總結 84
參考文獻 86

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