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研究生： 陳孟琳
Meng-Ling Chen
論文名稱： 含三價銪離子發光晶體之能量轉移研究
指導教授： 張伯琛
Bor-Chen Chang
口試委員:
學位類別： 碩士
Master
系所名稱： 理學院 - 化學學系
Department of Chemistry
論文出版年： 2013
畢業學年度： 101
語文別： 中文
論文頁數： 89
中文關鍵詞： 銪離子 、鋱離子 、釹離子 、能量轉移 、光譜 、稀土元素
外文關鍵詞： europium, spectroscopy, energy transfer, rare earth element, terbium, neodymium
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    • 本論文使用中溫水熱法合成以 1,4-cyclohexanedicarboxylate (CHDC)作為配位基含有不同比例稀土元素之 R2(CHDC)3晶體(R= Y, Eu, Tb)及以高溫高壓水熱法合成一系列矽酸鹽晶體 Cs3EuxNd1-xSi6O15 (x= 1, 0.975,0.96, 0.95)，這些晶體皆以粉末 X 光繞射分析圖譜確認晶體為相同結構與純度，以單晶X光繞射分析鑑定其晶體資料，再以感應耦合電漿原子發射光譜分析儀(ICP-AES)鑑定配位中心的元素比例。此類晶體均有可見光區的發光外，亦具有奇特之能量轉移現象。我們測量了這些晶體的放光光譜、激發光譜及其發光中心的放光衰退曲線以釐清其能量轉移機制。藉由分析這些光譜學資料，我們證明在R2(CHDC)3晶體中 Tb3+會單向性地轉移能量給 Eu3+，同時在 R2(CHDC)3 晶體中也明顯地發現濃度淬熄(concentration quenching)效應。而在Cs3EuxNd1-xSi6O15 (x= 1, 0.975, 0.96, 0.95)中發現 Eu3+之放光強度與放光衰退曲線在混入Nd3+會有類似鍺酸鹽晶體 K3(EuxNd1-x)3Ge6O18 中 Eu3+之淬熄行為，但其影響幅度矽酸鹽晶體明顯小於鍺酸鹽晶體，我們並證明矽酸基及鍺酸基作為配位基對 Eu3+放光中心有能量轉移的效應。

    Mid-temperature and high-temperature hydrothermal synthesis techniques have been used to respectively synthesize R2(CHDC)3, (R= Y, Eu, Tb, and CHDC= 1,4-cyclohexanedicarboxylate) with various compositions of rare earth elements and Cs3EuxNd1-xSi6O15 (x= 1, 0.975, 0.96, and 0.95). Power X-ray diffraction (PXRD) data of these compounds have been obtained for confirming their structure and purity, while single-crystal X-ray (XRD) data were taken for determining accurate crystallographic data. The compositions of rare earth elements were verified by the inductively coupled plasma atomic emission spectroscopy (ICP-AES). We have measured the photoluminescence (PL)spectra, excitation spectra, and emission decay curves of these compounds. In R2(CHDC)3, the energy transfer from Tb3+ to Eu3+ was found to be unidirectional and efficient, whereas the concentration quenching phenomena were also clearly observed in these compounds. The PL quenching caused by mixing Nd3+ in Cs3EuxNd1-xSi6O15 compounds was found to be similar to that in K3(EuxNd1-x)3Ge6O18 compounds with a profoundly smaller quenching magnitude. In these silicates and germanates, the energy transfer between the ligand to the luminescent center was also observed.

    中文摘要 ................................................................................................................ I 英文摘要 .............................................................................................................. II 謝誌 ..................................................................................................................... III 目錄 ..................................................................................................................... IV 表目錄 ................................................................................................................ VII 圖目錄 .............................................................................................................. VIII 第一章 緒論 ....................................................................................................... 1 1-1 鑭系元素與稀土元素 ................................................................................ 1 1-2 鑭系元素的放光 ........................................................................................ 2 1-2-1 銪離子的放光 ...................................................................................... 5 1-2-2 鋱離子的放光 ...................................................................................... 8 1-2-3 釹離子的放光 ...................................................................................... 9 1-3 論文研究目標 .......................................................................................... 10 第二章 實驗 ..................................................................................................... 14 2-1 合成方法 .................................................................................................. 14 V 2-1-1 水熱合成法 ........................................................................................ 14 2-1-2 晶體製備 ............................................................................................ 18 2-1-3 使用藥品 ............................................................................................ 20 2-2 鑑定方法 .................................................................................................. 20 2-2-1 單晶 X 光繞射實驗 ........................................................................... 21 2-2-2 粉末 X 光繞射實驗 ........................................................................... 23 2-2-3 感應耦合電漿原子發射光譜 ............................................................ 23 2-3 光譜技術簡介 .......................................................................................... 24 2-4 光譜儀簡介 .............................................................................................. 26 2-4-1 光源 .................................................................................................... 26 2-4-2 單光儀 ................................................................................................ 27 2-4-3 偵測器 ................................................................................................ 27 2-4-4 示波器 ................................................................................................ 29 2-4-5 儀器架設 ............................................................................................ 29 第三章 結果與討論 ......................................................................................... 34 3-1 R2(CHDC)3 ................................................................................................ 34 3-1-1 晶體鑑定 ............................................................................................ 34 VI 3-1-2 晶體結構 ............................................................................................ 37 3-1-3 放光光譜 ............................................................................................ 39 3-1-4 激發光譜 ............................................................................................ 41 3-1-5 Eu0.08Tb1.92(CHDC)3 ............................................................................ 43 3-1-6 放光衰退曲線 .................................................................................... 48 3-2 CsEuxNd1-xSi6O15 ....................................................................................... 53 3-2-1 晶體鑑定 ............................................................................................ 53 3-2-2 晶體結構 ............................................................................................ 54 3-2-3 放光光譜 ............................................................................................ 56 3-2-4 激發光譜 ............................................................................................ 58 3-2-5 Eu3+放光衰退曲線 .............................................................................. 59 第四章 結論 ..................................................................................................... 62 參考文獻 ............................................................................................................. 65 附錄 ..................................................................................................................... 67

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