含三價銪離子發光晶體之能量轉移研究

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陳孟琳(Meng-Ling Chen) 查詢紙本館藏

畢業系所

化學學系

論文名稱

含三價銪離子發光晶體之能量轉移研究

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摘要(中)

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。

摘要(英)

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.

關鍵字(中)

★ 銪離子
★ 鋱離子
★ 釹離子
★ 能量轉移
★ 光譜
★ 稀土元素

關鍵字(英)

★ europium
★ spectroscopy
★ energy transfer
★ rare earth element
★ terbium
★ neodymium

論文目次

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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指導教授

張伯琛(Bor-Chen Chang)

審核日期

2013-7-24

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