1996 年，日亞化學的中村修二(Nakamura)研究員 等人成功製備出白光發光二極體 (White - light emitting diode, W-LED)，其利用混光之方式以藍光發光二極體元件搭配黃光摻鈰之釔鋁石榴石(cerium doped yttrium aluminum garnet, YAG:Ce3+)。雖然此種方式所製備之W-LED之發光效率佳，但仍有藍光效率轉換不佳、白光的演色性不高及所使用的YAG:Ce3+螢光粉之熱穩定性較差之問題。近年來，在高功率LED的發展之下，所產生之問題即為熱管理。若無法有效處理熱問題，發光效率將有莫大影響。為改善上述之缺點，需提出一種改善熱穩定之方法。有關於熱的問題，由於氧化物中的磷酸鹽( ABPO4，A=Li+, Na+, K+, Rb+, Cs+，B=Mg2+, Ca2+, Sr2+, Ba2+ )為主體晶格之螢光粉係為一具有共價性質之三維剛性結構，極適合載子之傳輸，亦即，磷酸鹽系列之螢光粉之熱穩定相當優異。這也就是說，以磷酸鹽為主體晶格之螢光粉材料為一解決高功率W-LED熱問題之一可行且有效之方式。因此，在本文中，我們選擇NaSrPO4作為主體晶格，並選擇三個不同的稀土元素激活劑，分別為Tb，Sm和Tb/ Ce，分別採用傳統燒結和微波燒結技術，並討論它們的微觀結構和光致發光特性。實驗結果顯示，透過使用微波輔助燒結可以降低製程時間，和所需的能量以生產高品質的螢光體。此外，助熔劑(flux)的使用改善了燒結機制，因而提高了螢光體的光致發光特性。

In 1996, White-light emitting diode (W-LED) was fabricated by using the blue LED chip and yellow emitting phosphor such as cerium doped yttrium aluminum garnet (YAG: Ce3+) by Nichia. Although the W-LED has high brightness and efficiency, it still has some disadvantages, such as poor color rendering due to the lack of red component, low reproducibility, and the prepared phosphor has low thermal stability. Recently, a problem such as heat generated due to the high power LED must be solved. That is to say, if heat problem cannot be improved effectively, luminous efficiency will be affected. In order to overcome the above shortcomings, it is necessary to take a way to improve thermal stability. A compound, the phosphate oxide ( ABPO4，A= alkaline metals (Li , Na , K , Rb , Cs ), B=alkaline earth metals (Mg2+, Ca2+, Sr2+, Ba2+ )), has been selected as the host lattice due to three dimensional rigid structure. The phosphate oxide is very suitable for carrier transport, and the thermal stability of the phosphate series is quite outstanding. Using phosphate as host lattice in the phosphor material can solve the thermal problem of the high power w-LED. Thus, in this thesis, we choose NaSrPO4 as a host, and choose three different rare earth elements as activator, which are Tb, Sm, and Tb/Ce, respectively, using conventional sintering and microwave assisted sintering technique and their microstructure and photoluminescent properties of NaSrPO4: Re (Re=Tb, Sm, and Tb/Ce) were discussed. The experimental results showed the phosphors prepared by using microwave assisted sintering can reduce the process time, and required energy for the high quality production of phosphors. In addition, using fluxes indeed improve the sintering process and to enhance the photoluminescent properties of the phosphors.

中文摘要 i
Abstract iii
Contents iv
Table Captions vii
Figure Captions viii
Chapter 1 Introduction 1
1-1 Brief introduction of the phosphors 1
1-2 The structure of ABPO4 7
1-2-1 The structure of NaSrPO4 8
1-3 Motivation of this study 9
Chapter 2 Basic theory 11
2-1 Luminescence mechanism 11
2-1-1 Category and application of the phosphor 11
2-1-2 Fluorescence and phosphorescence theory 11
2-2 Emission theory and phosphor process 13
2-2-1 Absorption and excitation of the phosphor 13
2-2-2 Fluorescence and nonradiative transfer 15
2-2-3 Luminescence property of the rare earth elements 16
2-3 Properties of phosphors 18
2-3-1 Poisoning 18
2-3-2 Concentration quenching effect 19
2-3-3 Thermal quenching effect 19
2-4 Solid-state sintering method 20
2-5 Microwave-assisted sintering method 23
Chapter 3 Experimental procedures 28
3-1 Experiment materials 28
3-2 Experiment procedures 28
3-2-1 Fabrication of NaSrPO4:Tb3+ phosphors using conventional sintering 29
3-2-2 Fabrication of NaSrPO4:Tb3+ phosphors using microwave assisted sintering 30
3-2-3 Fabrication of NaSrPO4:Sm3+ phosphors using conventional sintering 31
3-2-4 Fabrication of NaSrPO4:Sm3+ phosphors using microwave assisted sintering31
3-2-5 Fabrication of NaSrPO4:Tb3+:Ce3+ phosphors using microwave assisted sintering 32
3-2-6 Fabrication of NaSrPO4:Tb3+ phosphors with flux using conventional sintering 32
3-3 Measurement system 33
3-3-1 X-ray Diffraction (XRD) 33
3-3-2 Scanning Electron Microscope (SEM) 34
3-3-3 Photoluminescence Spectrometer (PL) 35
Chapter 4 Results and discussion 37
4-1 Preparation of NaSrPO4:Re(Tb3+, Sm3+, Tb3+ /Ce3+ )phosphors and their propertie37
4-1-1 Microstructure, luminescence and thermal stability properties of NaSrPO4:Tb3+ phosphors with various doping concentrations prepared using conventional solid-state sintering 37
4-1-2 Effect of different sintering method on the microstructure and photoluminescent properties of NaSrPO4:Tb3+ phosphors 46
4-1-3 New NaSrPO4：Sm3+ phosphor as orange-red emitting material 59
Concentration(x) 67
4-1-4 Improving crystalline morphology and photoluminescent properties of NaSrPO4:Sm3+ phosphors prepared by microwave assisted sintering 70
4-1-5 Crystal structure effect on the luminescent properties of Tb3+, Ce3+ co-doped NaSrPO4 Phosphor prepared using microwave sintering 75
4-1-6 Effects of NH4Cl flux on microstructure and luminescent characteristics of NaSrPO4:Tb3+ phosphors 84
Chapter 5 Conclusion 92
Reference 94

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