本實驗利用多種螢光粉均勻摻雜於鈉玻璃(Multi-Phosphor-doped Glass, MPGD)作為色轉換層，成功開發高演色性(Color Rendering Index, CRI)及高可靠度(Reliability)之玻璃螢光體。實驗中針對MPDG的光學性質和微結構進行研究，利用YAG的黃色螢光粉(Y3AlO12 : Ce3+)、LuAG的綠色螢光粉(Lu3Al5O12 : Ce3+)以及Nitride的紅色螢光粉(CaAlClSiN3 : Eu2+)分別在680℃、700℃、750℃下燒結成玻璃螢光體，研究發現黃色與綠色玻璃螢光體在不同溫度下燒結可保持相同的量子效率(Quantum Yield, QY)68%，然而紅色玻璃螢光體的量子效率卻隨著溫度的上升從原本的47%大幅降低至5%，在高溫燒結時，低溫玻璃會擴散到螢光粉晶體中，使用場發射型穿透式電子顯微鏡(TEM)可以清楚的看到隨著燒結的溫度越高會導致更厚的擴散層，並且有更多的低溫玻璃擴散進氮化物晶體中，利用能量散佈分析儀(Energy Dispersive System, EDS)的元素分析，在較高溫度的燒結下，碳原子在擴散層中的比例會越高，這表示氮化物螢光粉與低溫玻璃混合後在越高的溫度下燒結會有更多的碳化物產生而嚴重降低紅色玻璃螢光體的量子效率。
利用多種螢光粉(黃色、綠色、紅色)的摻雜比例為0:4:1，在680℃燒結成玻璃螢光體，搭配發光波長445nm的藍光LED作為激發光源，其QY達51%，使用此為色轉換層的白光發光二極體(WLED)，其色座標(Color Coordinator)和相關色溫(Correlated Color Temperature, CCT)為(0.317, 0.315；6336K)，CRI可達90，符合美國能源之星規定室內照明其演色性必須大於80的規範。並且在150℃和250℃經過1008小時的可靠度測試證明高演色性玻璃螢光體的流明損失小於傳統矽膠螢光體的5倍以及10倍，可取代傳統色轉換層應用於高功率WLED，因此本研究高演色性玻璃螢光體白光發光二極體未來應用在固態照明系統上具有很大的潛力。

In this study, we used multi-phosphor-doped sodium glass (MPDG) as color conversion layer, and successfully developed glass phosphor with high color rendering index (CRI) and high reliability. We study the optical properties and microstructure of MPDG in this experiment. We used yellow phosphor of YAG based (Y3AlO12 : Ce3+), green phosphor of LuAG based (Lu3Al5O12 : Ce3+), and red phosphor of nitride based (CaAlClSiN3 : Eu2+) sintering to be glass phosphor at 680℃, 700℃ and 750℃, respectively. The study indicates that the yellow and green glass phosphor can keep the same quantum yield (QY) at different sintering temperature. However, the QY of red glass phosphor is significantly reduced with rising temperature.
The reason of the lowering QY of red glass phosphor can be explained by microstructure analysis when sintered at high temperature, the low temperature glass will diffuse into the phosphor crystal. Field-Emission Transmission Electron Microscope (FE-TEM) clearly shows that the higher sintering temperature induces thicker diffusion layer and more diffusion into phosphor crystal. Element analysis by Energy Dispersive System (EDS) reveals that, for red glass phosphor, higher percentage of carbon atoms in the diffusion layer under high sintering temperature, indicating more carbide was produced at higher temperature in the mixture of nitride phosphor and glass. The carbide severely lowered the quantum yield of the red glass phosphors.
Employing multi-phosphor (yellow, green, red) with doping concentration 0:4:1, and sintered at 680℃. Using a blue LED 445nm of wavelength as pumping source. The QY reaches 51%. The Color Coordinator and Correlated Color Temperature (CCT) of white light emitting diode (WLED) with them as color conversion layer is (0.317, 0.315；6336K). The CRI is up to 90, which meets the regulations of U.S. Energy Star that the CRI for interior lighting must exceed 80. The luminescence loss of glass phosphor is 5 to 10 space times lower than the traditional silicone phosphor under the 1008 hours reliability test under 150℃ and 250℃, respectively, which has great potential in lighting system.

中文論文審定書 i
英文論文審定書 ii
致謝 iii
摘要 iv
Abstract v
內容目錄 vii
圖目錄 ix
表目錄 xiii
第一章 緒論 1
1.1 前言 1
1.2 研究背景與動機 2
第二章 原理與介紹 7
2.1 LED元件發光原理 7
2.2 白光LED原理 10
2.3 螢光粉發光原理 12
2.3.1 螢光粉之組成 13
2.4 斯托克位移 (Stokes shift) 14
2.5 熱淬滅效應 (Thermal quenching effect) 15
2.6 色彩學 16
2.6.1 視覺敏感度 16
2.6.2 CIE色度座標圖 18
2.6.3 色溫 (Color temperature, K) 25
2.6.4 演色係數 (Color rendering index, CRI) 26
第三章 實驗方法與製程 30
3.1 低溫玻璃製程 30
3.2 高演色性玻璃螢光體製程 33
3.3矽膠螢光體製程 38
3.4 量測儀器與原理 40
3.4.1場發射型掃描式電子顯微鏡 (FE-SEM) 40
3.4.2 能量散佈分析儀 (EDS) 42
3.4.3 場發射型穿透式電子顯微鏡 (FE-TEM) 44
3.4.4 熱差分析儀 (DTA) 46
3.4.5 螢光光譜儀 (PLE) 47
3.4.6 積分球 (Integrating Sphere) 49
3.5 可靠度測試 (Reliability Test) 52
第四章 結果與討論 55
4.1玻璃螢光體激發與放光光譜 55
4.2 玻璃螢光體微結構分析 57
4.3 高演色性玻璃螢光體 61
4.4 可靠度測試 66
4.4.1 高溫加速老化 66
4.4.2 恆溫恆濕試驗 75
4.5 高演色性玻璃螢光體改進 79
第五章 結論與未來展望 82
5.1 結論 82
5.2 未來展望 83
參考文獻 84

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