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研究生： 汪立平
Wang, Li-Ping
論文名稱： 具高熱穩定性可調式NaYMgWO6:Tm3+, Dy3+, Sm3+白色螢光粉之光致發光特性探討
Color-Regulation and Luminescence Properties of NaYMgWO6:Tm3+, Dy3+, Sm3+ Phosphor with High Thermal Stability
指導教授： 黃正亮
Huang, Cheng-Liang
學位類別： 碩士
Master
系所名稱： 電機資訊學院 - 電機工程學系
Department of Electrical Engineering
論文出版年： 2024
畢業學年度： 112
語文別： 中文
論文頁數： 178
中文關鍵詞： NaYMgWO6 、WLED 、warm WLED 、Material Studio 、熱穩定性佳
外文關鍵詞： WLED, warm WLED, NaYMgWO6, Thermal stability, Material Studio
相關次數： 點閱：56  下載：0 
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    • 本研究使用高溫固態反應法製備NaYMgWO6雙鈣鈦礦螢光材料，並選用Tm3+、Dy3+與Sm3+作為活化劑，取代材料中的Y3+以形成發光中心。本研究詳細探討摻雜後NaYMgWO6之晶體結構、光學特性以及活化劑間的能量傳遞現象，並通過改變摻雜活化劑的類型與濃度，成功製備出單相白光螢光粉。
    第一部分先透過第一原理計算NaYMgWO6、NaYMgWO6: 1 mol% Tm3+、NaYMgWO6: 5 mol%Dy3+與NaYMgWO6: 7mol% Sm3+的能隙，觀察材料在少量摻雜後的能隙變化，並利用Tauc plot法，由反射光譜計算出材料的能隙，與模擬數據對照顯示出兩者結果接近，主體材料在摻雜少量活化劑後，能隙皆有微小的下降。
    第二部分研究NaYMgWO6: 1 mol% Tm3+在不同燒結溫度下，其光學特性與晶體結構的變化，將燒結溫度固定在800°C − 1100°C，由XRD分析顯示材料在800°C 與900 °C皆可以完整對應到ICSD標準卡號，但在1000°C以上會有相變化發生，SEM圖像也顯示溫度達到1000 °C以上時，晶粒形狀會發生改變，另外透過PL分析，可以觀察到樣品在900°C時擁有最佳的發光強度，因此選用900°C作為後續實驗的燒結溫度。
    第三部分研究NaYMgWO6分別摻雜Tm3+、Dy3+、Sm3+後，對於晶體結構及光譜特性的影響，利用SEM、XRD與GSAS分析，得出主體材料進行少量摻雜後晶體結構並不會有太大的影響，再透過PL、PLE與CIE分析，測量出Tm3+、Dy3+、Sm3+的最佳摻雜濃度分別為1 mol%、5 mol%和7 mol%，且其CIE座標分別位在藍光、黃光、橘紅光範圍。
    最後是透過共摻雜Tm3+、Dy3+以及Tm3+、Dy3+、Sm3+至主體材料NaYMgWO6中，以製備出單相白光螢光粉。同樣以SEM、XRD與GSAS分析，可見主體材料進行少量摻雜後晶體結構並不會有太大的影響，再透過PL、PLE與CIE分析，觀察出共摻雜Tm3+、Dy3+時，透過改變Dy3+的摻雜濃度，成功製備出可調式的冷白光，其CIE座標可以從(0.235,0.166)調至(0.364,0.357)；而在共摻雜Tm3+、Dy3+、Sm3+時，樣品的CIE座標皆落在暖白光範圍，其中摻雜1 mol% Tm3+、1 mol% Dy3+、7 mol% Sm3+的樣品，色溫計算為3099 K，將其進行熱穩定性測量，發現此樣品在LED工作溫度425 K時，發光強度可以維持初始強度的84.7%，代表此樣品具有優異的熱穩定性。

    A series of double perovskite-structured phosphors, NaYMgWO6:Tm3+, Dy3+, Sm3+, were prepared using the high-temperature solid-state reaction method. Material simulations were conducted through Material Studio to predict the material's band gap. Furthermore, the luminescent properties of the materials were analyzed using various techniques including SEM, XRD, PL & PLE spectra, CIE and fluorescence lifetime analysis. By adjusting the doping concentration of Tm3+, Dy3+, and Sm3+ appropriately, each can be assigned to a specific CIE coordinate, enabling the regulation of the phosphors' color temperature. Under 366 nm excitation, the luminescence of NYMWO: Tm3+, Dy3+ phosphors demonstrated a shift in CIE coordinates from (0.235, 0.166), CCT=6949K, to (0.364, 0.357), CCT=4358K, with increasing Dy3+ doping concentration, resulting in adjustable cold white light. Furthermore, co-doping with Sm3+ led to NYMWO: Tm3+, Dy3+, Sm3+ having a color temperature within the warm white range of 3000−4000K. Additionally, the material exhibited excellent thermal stability, retaining 84.7% of its initial PL intensity at 425K.

    中英摘要 I 致謝 XXXII 目錄 XXXIV 表目錄 XXXVIII 圖目錄 XXXIX 第一章 緒論 1 1.1 前言 1 1.2 研究動機與目的 3 1.3 主體材料介紹 4 第二章 理論與文獻回顧 6 2.1 螢光材料介紹 6 2.2 螢光材料設計 6 2.2.1 主體材料選擇 9 2.2.2 活化劑選擇 10 2.3 螢光材料發光分類 11 2.3.1 激發源之種類 11 2.3.2 螢光材料發光特性分類 13 2.4 螢光材料發光機制 16 2.4.1 發光原理介紹 16 2.4.2 輻射發光 17 2.4.3 組態座標圖 19 2.4.4 史托克位移(Stokes Shift) 21 2.4.5 能量轉移 22 2.5 影響發光特性因素 25 2.5.1 主體共價效應(Covalency Effect) 25 2.5.2 結晶場效應(Crystal field Effect) 25 2.5.3 濃度淬滅效應(Concentration quenching Effect) 26 2.5.4 熱淬滅效應(Thermal quenching Effect) 28 2.5.5 毒劑效應(Poisoning Effect) 29 2.6 螢光材料的製備 30 第三章 實驗步驟與方法 32 3.1 實驗材料 32 3.2 實驗步驟 33 3.3 分析儀器與方法 36 3.3.1 第一原理計算 36 3.3.2 X光繞射分析儀 (X-Ray Diffraction Analysis, XRD) 37 3.3.3 掃描式電子顯微鏡(Scanning Electron Microscope, SEM) 38 3.3.4 微拉曼及微光激發光譜儀(Micro-Raman＆Micro-PL Spectrometer) 39 3.3.5 螢光光譜儀( Fluorescence Spectrophotometer) 40 3.3.6 C.I.E. 色度座標分析 41 3.3.7 紫外光-可見光-近紅外光分光光譜儀(UV/Visible/NIR Spectrophotometer, UV-Vis) 43 3.3.8 量子產率(Quantum Yield)量測 44 3.3.9 生命週期螢光光譜分析 44 第四章 實驗結果與討論 45 4.1 NaYMgWO6第一原理計算 45 4.1.1 能階之計算 45 4.1.2 能態密度圖(Density of state, DOS)之計算 49 4.1.3 UV-visible之能階計算 51 4.2 NaYMgWO6摻雜Tm3+在不同溫度下之特性探討 54 4.2.1 XRD分析 54 4.2.2 SEM分析 55 4.2.3 PL分析 57 4.3 NaYMgWO6摻雜不同濃度Tm3+之特性探討 58 4.3.1 XRD分析 58 4.3.2 SEM分析 61 4.3.3 PLE分析 62 4.3.4 PL分析 63 4.3.5 熱淬滅 (Thermal Quenching)分析 66 4.3.6 量子產率分析 69 4.3.7 螢光衰減分析 70 4.3.8 CIE色度座標分析 71 4.4 NaYMgWO6摻雜不同濃度Dy3+之特性探討 72 4.4.1 XRD分析 72 4.4.2 SEM分析 75 4.4.3 PLE分析 76 4.4.4 PL分析 77 4.4.5 熱淬滅 (Thermal Quenching)分析 79 4.4.6 量子產率分析 82 4.4.7 螢光衰減分析 83 4.4.8 CIE色度座標分析 84 4.5 NaYMgWO6摻雜不同濃度Sm3+之特性探討 85 4.5.1 XRD分析 85 4.5.2 SEM分析 88 4.5.3 PLE分析 89 4.5.4 PL分析 90 4.5.5 熱淬滅 (Thermal Quenching)分析 92 4.5.6 量子產率分析 95 4.5.7 螢光衰減分析 96 4.5.8 CIE色度座標分析 97 4.6 NaYMgWO6共摻雜Tm3+與Dy3+之特性探討 98 4.6.1 XRD分析 98 4.6.2 SEM分析 99 4.6.3 PLE分析 100 4.6.4 PL分析 101 4.6.5 Tm3+與Dy3+離子之能量傳遞 102 4.6.6 熱淬滅 (Thermal Quenching)分析 104 4.6.7 量子產率分析 107 4.6.8 螢光衰減分析 108 4.6.9 CIE色度座標分析 109 4.7 NaYMgWO6三摻雜Tm3+、Dy3+與Sm3+之特性探討 110 4.7.1 XRD分析 110 4.7.2 SEM分析 112 4.7.3 PLE分析 113 4.7.4 PL分析 115 4.7.5 熱淬滅 (Thermal Quenching)分析 116 4.7.6 量子產率分析 119 4.7.7 螢光衰減分析 120 4.7.8 CIE色度座標分析 121 4.8 CIE色度座標圖總比較與色溫探討 122 第五章 結論 126 參考文獻 129

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