光與物質間的交互作用會產生極化子是未來研究光子和光電器件中一個很重要的現象，透過共振腔內的電磁波和物質中偶極矩躍遷之間的同調能量交換可以形成一個新的極化系統，而Rabi 分裂通常會大於原本光與物質間交互作用所產生的線寬並且能在頻域中觀察到反交叉的現象。
本論文主要研究羅丹明6G (R6G)染料分子與銀奈米圓孔陣列的強耦合現象並且探討其在動量空間中的極化子物理。為了實現這個系統，我們首先透過時域有限差分(FDTD)來模擬近場下的分佈以證明金屬和介電質界面之間存在傳播的表面電漿子(SPP)。第二，將聚乙烯吡咯烷酮 (PVP)層(~90 nm)旋塗於銀奈米圓孔陣列表面，利用角度分辨量測系統測量不同週期的銀奈米圓孔陣列之色散關係，並且用耦合模態模型(Coupled mode modeling)來分析消光光譜。
在我們的研究結果中，角度分辨消光光譜顯示傳播的SPP去耦合成光子並且輻射到遠場。為了探討電漿子-激子-極化子(Plasmon-exciton polariton, PEP)，也就是光與物質間的相互作用，在銀奈米圓孔陣列表面塗覆R6G與高分子聚合物的基質去測量其角度分辨消光和螢光光譜。利用角度分辨的技術在此極化系統中觀察到強耦合現象和極化子。最後，我們還觀察到PEP所形成的極化子能帶和極化子能隙。

Controlling lightmatter interaction forms polariton states is a key factor of future photonic and optoelectronic devices. The polaritonic systems can be formed by strongly coherent energy exchange between electromagnetic modes and electronic transition states. Generally, Rabi splitting larger than line widths of the intrinsic light and matter states in strong coupling regime, and energy anti-crossing phenomenon will be observed in detuning spectra. Polaritons are half-light, half-matter bosonic quasiparticles and offer the possibilities to explore manybody physics including Bose-Einstein condensation (BEC), polariton laser and some practical polaritonic devices.
This work focus on the Rhodamine 6G (R6G) dye molecules coupled with the plasmonic silver nanohole arrays and probe polaritonic dispersions in momentum space. For more realizing this open system, we firstly simulated nearfield distributions by finite-different time domain (FDTD) to evidence propagating SPPs exist between interface of metal and dielectric medium. Secondly, polyvinylpyrrolidone (PVP) layer (~90 nm) covered on top of plasmonic silver nanohole arrays by spin-coating technique, measuring dispersions of the plasmonic silver nanohole arrays with different pitches by the angle-resolved extinction setup, and using coupled mode modeling to analyze these results. To discuss plasmon-exciton polaritons (e.g. light-matter interaction), R6G polymer matrix covered on plasmonic silver nanohole arrays, and measuring angle-resolved extinction and photoluminescence spectra. In this polaritonic system, strong coupling phenomena and polariton emission are observed by angular detuning, respectively. Furthermore, we also observed polariton band and gaps are formed by propagating plasmon-exciton polariton.

國 立 清 華 大 學
摘要 I
Abstract II
致謝 III
目錄 IV
圖目錄 VI
表目錄 X
第一章 緒論 1
1.1實驗簡介及動機 1
第二章 表面電漿 3
2.1 表面電漿極化子 3
2.2金屬電漿子材料的性質 5
2.3電漿子晶格(Plasmonic lattice) 7
2.3.1表面電漿子激發機制 7
2.3.2色散關係與週期結構 9
2.3.3 定義TM mode與TE mode 11
第三章 光與物質間的強耦合 13
3.1 量子發射器(Quantum emitters) 13
3.2 螢光染料分子―羅丹明6G (Rhodamine 6G，R6G) 14
3.3 光與物質的強耦合現象 15
第四章 理論與數據分析方法 18
4.1 兩個諧振子的運動方程 18
4.2耦合模態模型(Coupled mode modeling) 19
4.3 拉比分裂 "∝" "N" 20
第五章 實驗內容 23
5.1 樣品的製備 23
5.1.1基板的選擇 23
5.1.2 以熱蒸鍍法成長銀膜 23
5.1.3 使用聚焦離子束法(FIB)製作結構 25
5.1.4 原子層沉積系統(Atomic Layer Deposition, ALD)鍍保護層 26
5.1.5 調配羅丹明6G (Rhodamine 6G ，簡稱R6G)混合液 27
5.1.6 旋塗R6G混合液至樣品表面 28
5.2 角度分辨光學顯微術(Angle-resolved optical microscopy) 29
第六章 實驗結果與數據分析 30
6.1 不同濃度R6G的激子變化 30
6.2 FDTD 模擬銀奈米圓孔陣列 32
6.3 銀奈米圓孔陣列的光譜量測及分析 34
6.3.1 4×4的耦合模態理論 34
6.3.2 Square lattice 36
6.3.3 Square lattice的12×12 矩陣 37
6.3.4 Square lattice的色散關係圖 38
6.4 電漿激子極化子的色散曲線 40
6.4.1 PEP的色散曲線 40
6.4.2 降低晶格對稱性 42
6.4.3 Rectangular lattice 43
6.4.4 Rectangular lattice的4×4 矩陣 44
第七章 結論 46
第八章 參考文獻 47

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