此論文探討單層二維半導體的激子與電漿子之交互作用，藉由奈米金陣列的合成與研發，異質整合化學氣相沉積製程之單層二硫化鎢，實現室溫下觀察二維材料系統的強耦合效應。
　　過渡金屬二硫屬化合物具有強束縛能，能在室溫下觀察到穩定存在的多種激子，同時，奈米金屬因表面電漿共振所產生的電漿子，伴隨著電場侷限之效應，可有效調控過渡金屬二硫屬化合物的吸收與放光行為，將能量於空間中有效侷限在金屬周圍。當激子與電漿子的能量交換速率大於各自之衰退速率時，有機會產生極化子，其為一種兼具一半能量性質與一半物質性質之準粒子，可用於探討光與物質間的交互作用。
　　本研究選擇二硫化鎢代表單層二維半導體，由於二硫化鎢具有極高的自旋軌道耦合及激子束縛能(高達400-800 meV)，可避免熱干擾，有助於觀察單層二維晶體中關鍵議題。此外，化學法的奈米金製程，具有高品質且有助於發展大規模奈米金屬晶體陣列。本研究透過奈米晶體自組裝的研發，結合奈米金屬於材料尺度、幾何形貌、晶體結構及組成上的調控，實現具有多元光學調控能力的大型陣列。
　　藉由單層二硫化鎢及奈米金陣列結構的異質整合，透過陣列的設計調控其與單層二硫化鎢之交互作用，成功在室溫下觀察到單層二維晶體之激子與電漿子間的強耦合效應。此研究有助於深入研究二維材料在光與物質間的強交互作用，大規模奈米陣列的調控技術，將在後續研究及應用具有高度潛力。

　　　　In this thesis, interactions between excitons of the monolayer WS2 and plasmons of gold nanocrystal array are studied. With the development on the nanocrystal array and its hetero-integration with the monolayer, strong coupling of the two particles is successfully demonstrated at room temperature.
　　　　High exciton binding energy of the transition metal dichalcogenides is significant to explore exciton physics of the 2D lattices at room temperature. Plasmons, induced by localized surface plasmon resonance of noble metals, enable a confined electric filed around nanometals with better control of the dipole transitions with light, which enhance optical absorption, emission and novel properties of the monolayer. As the rate of energy exchange between exciton and plasmon is larger than the rate of dephasing, the energy exchange resulted in the strong coupling, forming a new hybrid state of half-light and half-matter, named polariton.
　　　　To study the interaction between exciton and plasmon, we combined monolayer WS2 with self-assembly nanocrystal array that are designed and fabricated with tunable parameters, including periodicity, size and geometry. Besides, we discussed the relationship between efficiency of nanoparticle and applied voltage, and provided the strategies to make nanocrystals into well-defined patterns. Further, we used the strategy to make various arrays of nanocrystal geometries. This research initiates a new route toward tunable light matter interaction of the monolayer 2D lattices with plasmonic nanocrystals array.

一、 緒論 9
二、 文獻回顧 11
2-1 二維晶體於異質系統下的光物質交互作用 (Light Matter Interaction of 2D lattice in hybrid system) 11
2-1-1 光物質交互作用 (Light-Matter Interaction) 11
2-1-2 柏塞爾效應 (Purcell Effect) 12
2-1-3 表面電漿共振特性 (Localized Surface Plasmon Resonances) 13
2-1-4 表面晶格共振 (Surface Lattice Resonances) 14
2-1-5 過渡金屬二硫屬化合物 (Transition Metal Dichalcogenides) 15
2-1-6 強耦合作用 (Strong Coupling) 16
2-2 金奈米晶體之性質(Properties of Gold Nanocrystals) 18
2-2-1 以晶核成長法調控晶體成長 (Controllable Nanocrystals by Seed-Mediated Method) 18
2-2-2 球型之奈米金( Gold Nanosphere) 19
2-2-3 柱狀之奈米金（Gold Nanorod） 20
2-3 奈米晶體陣列製程 (Fabrication of nanocrystal array) 21
2-3-1 奈米結構自組裝 (Self-Assembly of Nanostructure) 21
2-3-2 由上而下製程 (Top-Down Process) 23
2-3-3 定向自組裝 (Directed Assembly) 24
2-3-4 電泳沉積法 (Electrophoretic Deposition) 25
三、 實驗方法 27
3-1 實驗系統介紹 27
3-1-1 奈米材料合成 (Synthesis of Gold Nanocrystals) 28
3-1-1-1 球型奈米金 (Gold Nanosphere) 28
3-1-1-2 棒狀奈米金 (Gold Nanorod) 29
3-1-2 奈米陣列製作 (Fabrication of Nanoarray) 31
3-1-2-1 基板前置作業 31
3-1-2-2 奈米粒子自組裝 ( Self-assembly of Nanocrystals) 31
3-1-3 與過渡金屬二硫屬化合物結合 32
3-1-3-1 二硫化鎢製作 32
3-1-3-2 氧化鋁保護層 33
3-1-3-3 材料轉移 33
3-2 儀器介紹 34
3-2-1 紫外可見光光譜儀 (Ultraviolet-Visible Spectroscope, UV-Vis) 34
3-2-2 高解析熱場發射掃描式電子顯微鏡 (High-Resolution Field Emission Scanning Electron Microscope, SEM) 34
3-2-3 光學顯微鏡 (Optical Microscope, OM) 35
3-2-4 電子束蒸鍍 (E-gun Evaporator) 35
3-2-5 電子束微影系統 (E-Beam Lithography, EBL) 36
3-2-6 原子層沉積 (Atomic Layer Deposition, ALD) 36
四、 奈米晶體陣列與單層二硫化鎢之交互作用 38
4-1 奈米晶體製備與調控 38
4-1-1 球型奈米金 38
4-1-2 棒狀奈米金 43
4-2 奈米陣列自組裝 47
4-2-1 電泳沉積對奈米晶體自組裝之探討 47
4-2-2 應用 52
4-3 週期性排列與二硫化鎢之強耦合 52
五、 結論 58
六、 參考文獻 59

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