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    题名: 電漿子極化子能源裝置製程方法的開發;Development of fabrication methods for making plasmon polariton energy devices
    作者: 陳品宏;Chen, Pin-Hung
    贡献者: 物理學系
    关键词: 脈衝雷射沉積;金奈米顆粒;強耦合;玻璃基板;Pulsed Laser Deposition;Gold Nanoparticles;Strong Coupling;Glass Substrate
    日期: 2025-07-28
    上传时间: 2025-10-17 11:56:28 (UTC+8)
    出版者: 國立中央大學
    摘要: 這份研究主要是透過脈衝雷射沉積法與金屬跟金屬氧化物靶材;金,銀,二氧化鈦,氧化鎳,獨立發展製備金奈米顆粒/二氧化鈦/鈦/金/鈦/矽/玻璃基板材料的電漿子極化子能源裝置的製程。
    選用的玻璃基板材料種類為石英玻璃,因為石英表面平整度較為平整,並觀察到在升降溫過程中,薄膜受到應力影響而產生皺摺、龜裂進而導致剝落的形變。從蒸鍍底層金薄膜發現,蒸鍍時需要160°C的溫度才可以讓金沉積在石英玻璃上可以有足夠的平整度及良率。
    從鍍二氧化鈦薄膜時分別從溫度及氧氣壓力做調整,最終確定鍍膜溫度在225度、壓力150 mtorr時薄膜才不會觀察到任何形變產生。
    從二氧化鈦沉積在金/鈦/矽/石英玻璃基板上的拉曼光譜及XRD分析,拉曼分析後結晶向比較像brookite,而不是如參考文獻[1]中的anatase,而經過熱退火後峰值有往anatase方向偏移,從XRD分析中,我們可以發現退火後明顯在29.4的位置有峰出現,應是對應到anatase結晶向,所以推測我們的二氧化鈦應是部分brookite部分anatase結晶向。
    還發展將金或合金薄膜利用雷射退火技術,在合適的雷射功率及掃描次數下,形成有合適大小及均勻分布的金奈米顆粒及合金奈米顆粒。
    此外還測試了將底層金換成鋁薄膜的技術,透過改變底層薄膜,增加耦合強度,也利用鋁在短波長的高反射率,更加容易的觀察到二氧化鈦薄膜上鍍金奈米顆粒前後及增加顆粒鑲嵌深度時薄膜吸收的情況。
    本研究中發展在玻璃基板上的電漿子極化子能源裝置,還未能夠觀察到足夠的吸收,或是強耦合造成的吸收峰分裂,僅有看到局域表面電漿共振形成的吸收峰的出現。推測在鍍膜過程中因為二氧化鈦結晶程度不佳,造成二氧化鈦折射率不足,導致最後鍍完金奈米顆粒後吸收不夠,而無法看到吸收峰的分裂可能因為二氧化鈦表面平整度可以更平整,讓金奈米顆粒可以在平整的薄膜形成。
    ;This study primarily utilizes pulsed laser deposition (PLD) with metal and metal oxide targets—gold (Au), silver (Ag), titanium dioxide (TiO₂), and nickel oxide (NiO)—to independently develop the fabrication process of a plasmon–polariton energy device composed of gold nanoparticles/TiO₂/Ti/Au/Ti/Si on a glass substrate.
    Quartz glass was chosen as the substrate material due to its superior surface flatness. During thermal cycling, stress-induced deformation such as wrinkling, cracking, and eventual delamination of the film was observed. It was found that a substrate temperature of 160°C was necessary during the deposition of the base Au layer to achieve adequate smoothness and yield on quartz.
    For the TiO₂ film, both substrate temperature and oxygen pressure were optimized. It was determined that a deposition temperature of 225°C and an oxygen pressure of 150 mtorr were optimal for avoiding any visible film deformation.
    Raman and XRD analyses were conducted on TiO₂ films deposited on Au/Ti/Si/quartz substrates. The Raman spectra suggested a crystalline phase closer to brookite rather than anatase, as reported in reference literature. However, after thermal annealing, the peaks shifted toward those characteristic of anatase. XRD results confirmed a significant peak at 29.4°, indicating the presence of anatase. Thus, it is inferred that the TiO₂ film likely contains a mixture of brookite and anatase phases.
    The study also developed a laser annealing technique to transform gold or alloy thin films into uniformly distributed gold or alloy nanoparticles of suitable size by tuning the laser power and scan count.
    In addition, experiments were conducted using aluminum (Al) thin films instead of gold as the bottom layer. By modifying the underlying film, coupling strength was enhanced. The high reflectivity of Al at short wavelengths also allowed clearer observation of the absorption characteristics of the TiO₂ film before and after the deposition of Au nanoparticles, and as a function of nanoparticle embedding depth.
    Although a plasmon–polariton energy device on a glass substrate was successfully fabricated, clear signatures of strong coupling—such as absorption peak splitting—were not observed. Only localized surface plasmon resonance (LSPR) peaks were detected. This is possibly due to insufficient crystallinity of TiO₂ during deposition, leading to a lower refractive index. As a result, even after depositing Au nanoparticles, absorption remained inadequate. It is speculated that further improvements in TiO₂ surface flatness could help the nanoparticles form more uniformly, potentially enabling the observation of absorption peak splitting due to strong coupling.
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