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研究生:雷秀玲
研究生(外文):Xiu-ling Lei
論文名稱:以表面增強拉曼及共振拉曼搭配分子理論計算研究化學分子和DNA的作用方式
論文名稱(外文):Studying the interaction between molecules and DNA using the molecular computation theory and surface-enhanced Raman and resonance Raman
指導教授:楊子萱楊子萱引用關係
學位類別:碩士
校院名稱:國立中正大學
系所名稱:化學所
學門:自然科學學門
學類:化學學類
論文種類:學術論文
論文出版年:2006
畢業學年度:94
語文別:中文
論文頁數:96
中文關鍵詞:拉曼
外文關鍵詞:raman
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表面增強拉曼光譜surface-enhanced Raman scattering (SERS)已經廣泛用來研究分子與基質表面的作用機制或是分子吸附於表面的位向。其優點是可以偵測極少量的樣品,得到很高的訊號。這個優點可以用來研究比較貴的樣品,如DNA等以減少研究上的成本。
本研究主要以SERS研究carbazole衍生物與DNA作用情形。3,6-Bis
(1-methyl-4-vinylpyridinium) carbazole diiodide (BMVC),3,6-bis(1-methyl-
2-vinylpyridinium) carbazole (2-BMVC),3,6-bis(1- methyl-3-vinylpyraziniu-
m) carbazole (3NBMVC)與雙股DNA序列ds(GCGCAATTGCGC)(LD)作用後,從SERS差異光譜有看到不同。藉由分子理論計算進一步了解這種差異是化學分子哪部分變化所產生。此外,結合實驗SERS與計算光譜,探討carbazole衍生物在奈米銀的吸附方位。
另外我們選擇已知的DNA 溝槽鍵結分子DODCI與BMVC做比較,DODCI與DODCI/LD的SERS光譜明顯不同,間接推測carbazole衍生物與DNA並非溝槽鍵結方式。
3NBMVC 即使與DNA作用後也沒有螢光,所以我們以共振拉曼研究它與DNA G-四角結構的作用。3NBMVC與DNA G-四角結構作用後,顏色改變,但從共振拉曼光譜看不到光譜的改變。而單純hum24在鈉離子與鉀離子溶液的螢光光譜是不同,表示鈉離子與鉀離子造成hum24結構有差異。
Surface-enhanced Raman scattering (SERS) has been widely used to study the interactions and the orientations of molecules adsorbed on substrate. With its high sensitivity, the amount of samples to be used is reduced greatly. So we can apply it to study expensive samples. Such as DNA for reducing the cost.
The main subject of this thesis is studying the interaction between carbazole derivatives and DNA by SERS. The samples include 3,6-Bis-(1-m-
ethyl-4- vinylpyridinium) carbazole diiodide (BMVC), 3,6-bis (1-2-vinyl py-
ridinium) carbazole (2-BMVC), 3,6-bis(1- methyl-3-vinylpyrazinium) carba-
zole (3NBMVC) and double helix DNA, ds(GCGCAATTG CGC)(LD) solu-
tions. There are differences in the SERS spectrums of carbazole derivative before and after adding LD. By molecular computat ion theory we calculate
the vibration mode of the molecules. By comparision of experimental SERS spectra and calculate Raman spectra, we model how carbazole derivatives absorb on silver nanoparticles.
We compare DODCI, the groove binding molecule with DNA, with BMVC. The SERS spectrums of DODCI and DODCI/LD, exhibit apparent
differences. We conclude that carbazole derivatives do not interact with DNA by groove binding.
No fluorescence is detected when 3NBMVC interacts with DNA. Therefore we take the resonance Raman spectrums of 3NBMVC and 3NBMVC/G- quardruplexes. When 3NBMVC interact with G-quardruplexes,
the solution color changes. However there is no difference observed in the resonance Raman spectrums. The fluorescence of hum24, (TTAGGG)4, in Na+ or in K+ solutions is different. This indicates that Na+ and K+ can cause different hum24 structures.
中文摘要……………………………………………………………………Ⅰ
英文摘要……………………………………………………………………Ⅱ
目錄…………………………………………………………………………Ⅲ
圖目錄………………………………………………………………………Ⅴ
表目錄………………………………………………………………………XI
第一章 前言
1-1 疾病與去氧核醣核酸(DNA)的關係………………………………1
1-2 去氧核醣核酸(DNA)儲存遺傳訊息………………………………4
1-3 DNA的結構…………………………………………………………6
1-4 染料的簡介…………………………………………………………8
第二章 實驗基本原理
2-1 拉曼散射……………………………………………………………13
2-2 共振拉曼散射………………………………………………………15
2-3 表面增強拉曼散射…………………………………………………17
2-4 表面增強拉曼的機制………………………………………………18
2-4-1 物理增強……………………………………………………………18
2-4-2 化學增強……………………………………………………………19
2-5 拉曼光譜儀…………………………………………………………21
2-5-1 雷射光源……………………………………………………………21
2-5-2 分光儀………………………………………………………………21
2-5-3 CCD(Charge-Coupled Device)感測元件………………………23
2-6 理論計算……………………………………………………………24
2-6-1 計算軟體(Gaussian 03)…………………………………………24
2-6-2 計算方法(密度泛函理論density functional theory)………25
2-6-3 基底函數組(Basis set)…………………………………………26
第三章 實驗步驟
3-1 銀膠體溶液…………………………………………………………28
3-2 實驗藥品……………………………………………………………29
3-3 實驗儀器架設………………………………………………………33
第四章 結果與討論
4-1 BMVC及其衍生物的吸收光譜………………………………………35
4-2 螢光光譜……………………………………………………………36
4-3 表面增強拉曼光譜…………………………………………………37
4-4 實驗SERS與計算Raman的比較…………………………………………41
4-5 共振拉曼光譜 (3NBMVC及其複合物)…………………………………84
4-6 共振拉曼與SERS的比較………………………………………………91
第五章 結論……………………………………………………………………92
參考文獻………………………………………………………………93
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