以光譜學研究含稀土元素發光晶體內之能量轉移過程

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蕭郁如(Yu-Ru Hsiao) 查詢紙本館藏

畢業系所

化學學系

論文名稱

以光譜學研究含稀土元素發光晶體內之能量轉移過程

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摘要(中)

本論文使用中溫水熱法合成不同比例稀土元素之R2(C8H10O4)3晶體(R= Y, Eu, Tb; C8H10O4= 1,4-cyclohexanedicarboxylate)和高溫固態合成法合成K4(UO2)Eu2Ge4O14。合成的化合物以單晶X光繞射鑑定晶體結構並以粉末X光繞射實驗鑑定晶體的純度，再以感應耦合電漿原子發射光譜做鑭系元素的定量。我們測量了這些晶體的光致放光光譜、激發光譜及其時間解析光譜以釐清其能量轉移機制與速率。藉由分析這些光譜資料，我們證明Eu2(C8H10O4)3 和Tb2(C8H10O4)3中之濃度淬熄現象為上能階之能量轉移，而混合Eu3+及Tb3+之化合物中，Tb3+轉移能量給Eu3+之機制則為光子間的能量轉移，並且在不同波長有不同之轉移速率和機制。在K4(UO2)Eu2Ge4O14化合物中，我們證明了UO22+會將能量轉移予Eu3+放光，且發現在不同激發波長其轉移速率也有所不同。

摘要(英)

Mid-temperature hydrothermal and high-temperature solid-state synthesis techniques have been respectively used for the synthesis of R2(C8H10O4)3, (R=Y, Eu, Tb, and C8H10O4= 1,4-cyclohexanedicarboxylate) and that of K4(UO2)Eu2Ge4O14. Single-crystal and powder X-ray diffraction (XRD) data of these compounds have been obtained for confirming their structure and purity. The compositions of lanthanide elements were verified by the inductively coupled plasma atomic emission spectroscopy (ICP-AES). We have recorded the photoluminescence (PL) spectra, excitation spectra, and time-resolved spectra for clarifying the energy transfer mechanisms and the transfer rates in these compounds. Based upon the analysis of our data, we show that the concentration quenching in Eu2(C8H10O4) as well as in Tb2(C8H10O4) is an energy migration process, while the energy transfer from Tb3+ to Eu3+ in the Eu3+/Tb3+ hybrid compounds is a photon energy transfer process and the Tb3+-Eu3+ energy transfer rate is wavelength-dependent. In addition, we have also confirmed that the Eu3+ emission in K4(UO2)Eu2Ge4O14 is activated by the sensitization of UO22+ and the energy transfer rate also highly depends on the excitation wavelength.

關鍵字(中)

★ 以光譜學研究含稀土元素發光晶體內之能量轉移過程

關鍵字(英)

論文目次

中文摘要 ................................ ................................ ................................ ................ I
英文摘要 ................................ ................................ ................................ .............. II
謝誌 ................................ ................................ ................................ ..................... III
目錄 ................................ ................................ ................................ ..................... IV
表目錄 ................................ ................................ ................................ ................ VIIVII
圖目錄 ................................ ................................ ................................ .............. VIIIVIII
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................................ ................................ ....................... 3
1-2-1銪離子的放光 ................................ ................................ ....................... 5
1-2-2鋱離子的放光 ................................ ................................ ....................... 7
1-3研究目標 ................................ ................................ ................................ ... 8
第二章實驗 ................................ ................................ ................................ ....... 12
2-1實驗目標實驗目標 ................................ ................................ ................................ . 12
2-2合成方法合成方法 ................................ ................................ ................................ . 13
2-2-1水熱合成法 ................................ ................................ .......................... 13
2-2-2高溫固態法 ................................ ................................ .......................... 16
V
2-2-3晶體合成 ................................ ................................ .............................. 17
2-2-4使用藥品 ................................ ................................ .............................. 18
2-3鑑定方法 ................................ ................................ ................................ . 19
2-3-1單晶X光繞射 ................................ ................................ ..................... 19
2-3-2粉末X光繞射 ................................ ................................ ..................... 22
2-3-3感應耦合電漿原子發射光譜 ................................ ............................. 22
2-4光譜裝置簡介 ................................ ................................ ......................... 23
2-4-1光源 ................................ ................................ ................................ ..... 23
2-4-2單光儀 ................................ ................................ ................................ . 25
2-4-3偵測器 ................................ ................................ ................................ . 25
2-4-4示波器 ................................ ................................ ................................ . 27
2-5光譜技術簡介................................ ................................ ......................... 27
2-6光譜分析研究及實驗裝置 ................................ ................................ .... 29
第三章結果與討論 ................................ ................................ ........................... 33
3-1 R2(CHDC) (CHDC)(CHDC) 3 ................................ ................................ .............................. 33
3-1-1晶體鑑定 ................................ ................................ ............................. 33
3-1-2晶體結構 ................................ ................................ ............................. 37
3-1-3放光譜 ................................ ................................ ............................. 39
3-1-4激發光譜 ................................ ................................ ............................. 41
VI
3-1-5 Eu 3+ 之放光衰退曲線之放光衰退曲線 ................................ ................................ .......... 43
3-1-6濃度淬熄機制濃度淬熄機制 ................................ ................................ ..................... 47
3-1-7 Tb 3+ 之放光衰退之放光衰退曲線 ................................ ................................ .......... 52
3-1-8 Tb 3+ 與 Eu 3+ 間能量轉移機制間能量轉移機制 ................................ .............................. 55
3-1-9 Tb 3+ 與 Eu 3+ 間能量轉移之效率和速間能量轉移之效率和速間能量轉移之效率和速間能量轉移之效率和速................................ .............. 58
3-2 K2 K 4(UO (UO2)Eu )Eu2Ge 4O14 ................................ ................................ ................. 63
3-2-1化合物鑑定化合物鑑定 ................................ ................................ ......................... 63
3-2-2晶體結構 ................................ ................................ ............................. 64
3-2-3放光譜 ................................ ................................ ............................. 66
3-2-4激發光譜 ................................ ................................ ............................. 67
3-2-5 UO 22+ 和 Eu 3+ 間的能量轉移間的能量轉移 ................................ ............................... 68
第四章結論 ................................ ................................ ................................ ....... 73
參考文獻 ................................ ................................ ................................ ............. 76

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指導教授

張伯琛(Bor-Chen Chang)

審核日期

2014-7-29

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