在本研究中，我們利用表面增強拉曼散射( surface-enhanced Raman scattering, SERS )應用於生醫感測的特性，搭配奈米科技領域中使用範圍極廣的生物有機高分子DNA 材料，製作出高靈敏度的SERS 基板，並應用於生物鹼coralyne 與DNA 雜交的生物檢測。
我們將DNA 材料經活性改質後，溶於有機溶液中，利用其特殊雙股螺旋結構，配合弱感光劑Iragacure-2959 與簡單的光還原法，合成出表面高粗糙度的花狀金奈米粒子。藉由改變DNA、金鹽類與光感劑的莫耳數比，調控金奈米粒子的形貌與尺寸。接著利用製作出的金奈米粒子，與簡單的casting 方式，製作SERS 基板後進行靈敏度檢測，對於GM19 與DTNB 兩種待測分子，對於最低濃度可量測兩者皆為10-9 M，SERS 訊號增強幅度( enhancement factor )則分別可達4.4×105 與2.6×106。
我們並將此 SERS 基板應用於感測器，檢測抗癌物質coralyne與DNA 雜交前後的SERS 光譜差異。藉由螢光光譜得知DNA 與coralyne 的最佳結合比例，並透過SERS 檢測中強度比值( I736/I1318 )推算出溶液內，單股與雙股DNA 的比例，驗證coralyne 含量的多寡。

In this work, we used the bio-organic polymer material full name (DNA), which has been widely employed in nanotechnology, in surface-enhanced Raman scattering (SERS) for biomedical sensing. A SERS substrate is presented to be used in sensing the interaction of alkaloid coralyne and DNA hybridization.
We use the modified double helix DNA and weak photoreducing agent, Iragacure-2959, to synthesize rough surface flower-like gold nanostructures by photoreduction. By controlling the molar ratio of DNA, gold salt precursor and photoreducing agent, various morphologies and size of gold nanostructures can be obtained. We demonstrate the application of gold nanostructures as SERS substrate. The lowest detectable concentration of analytes, GM19 and DTNB is 10-9 M and the enhancement factor is 4.4×105 and 2.6×106, respectively.
We apply this SERS substrate for sensors to detect the interaction of alkaloid coralyne and DNA. We determined the best combination ratio of coralyne and DNA by fluorescence spectroscopy. In addition, we also use the SERS intensity ratio (I736/I1318), which indicates the single-stranded and double-stranded DNA ratio, to verify coralyne concentration.

摘要 II
Abstract III
致謝 IV
目錄 V
圖目錄 VII
表目錄 X
第一章 文獻回顧與介紹 1
1.1 拉曼散射 1
1.1.1 一般拉曼散射基本原理 1
1.1.2 表面增強拉曼散射效應 (SERS) 5
1.1.2.1 電磁效應 5
1.1.2.2 化學效應 6
1.1.3 SERS應用於感測器 7
1.2 金屬奈米粒子 9
1.2.1 金屬奈米粒子特性 9
1.2.2 金屬奈米粒子簡介 10
1.2.3 以DNA模板合成特殊形貌金屬奈米粒子 16
1.3 研究動機 19
第二章 實驗製備與量測 20
2.1 DNA材料製備 20
2.1.1 DNA配置 20
2.1.2 DNA-CTMA合成 24
2.2 光合成金奈米粒子製備 24
2.3 SERS基板製備 26
2.4 量測儀器介紹 29
2.5 藥品及實驗器材 31
第三章 結果與討論 32
3.1 簡介金奈米粒子 32
3.1.1 金奈米粒子生長機制 32
3.1.2 金奈米粒子光譜檢測與形貌分析 34
3.2 金奈米粒子最佳條件優化 36
3.2.1 DNA片段長度對金奈米粒子製備的影響 36
3.2.2 DNA片段分布對金奈米粒子製備的影響 39
3.2.3 DNA-CTMA濃度調控金奈米粒子形貌 40
3.3 表面增強拉曼散測量測分析 44
3.3.1 不同形貌金奈米粒子對SERS影響 44
3.3.2 不同SERS基板製備探討 46
3.3.3 花狀金奈米粒子濃度分析 51
3.3.4 精胺對於SERS的影響 53
3.3.5 SERS基板靈敏度檢測 56
3.4 利用SERS檢測DNA與coralyne雜交效果 62
第四章 結論與未來展望 71
參考文獻 73

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