量子點因具有放射波長可調性、激發波段寬廣及高量子效率等優勢，因此在近年來逐漸取代傳統螢光粉製備成白光發光二極體(White light-emitting diode, WLED)。然而要得到白光需混合不同光色的量子點，製備過程複雜且費時，且易因重吸收效應導致元件發光效率下降。而近年來三元合金化量子點的製程逐漸受到重視，此製程可藉由控制組成進而調控粒徑尺寸及放射波長。因此，本研究利用膠體化學法，在低溫下使用非配位錯合劑-油酸(OA)及溶劑-十八碳烯(ODE)製備同時具有能帶邊緣及表面能態放射波長之ZnxCd1-xS (又稱Znx)量子點，並將Znx量子點與封裝膠混合製成WLED。
本研究分為三個部分，第一部分為控制鋅與鎘的莫耳比製備Znx(x為鋅的莫耳比，分別為0.2, 0.5, 0.8)量子點，探討其光學性質變化。結果顯示當反應時間固定(13分鐘)時，隨著鋅含量增加，粒徑尺寸變小且放射波長藍移，且因鋅的共價性可使量子點穩定性提升。
第二部分為控制反應時間對Zn0.5量子點的影響，並在量子點外圍包覆二氧化矽，探討量子點包覆二氧化矽前後的光學性質變化。結果顯示當反應時間為5分鐘時，量子效率最高可達86 %。隨著反應時間增加，放射波長出現紅移，原因為合金化的非線性光學效應導致。當反應時間為20分鐘時，大量鋅置換造成放射波長藍移，且量子點成長趨於飽和，隨著反應時間增加，Znx量子點從富含鎘的核心逐漸變成表面富含鋅鎘的梯度合金，在鋅擴散至內部後可使量子點的穩定性提升。而量子點在包覆二氧化矽後團聚造成放射波長出現紅移現象，且由於二氧化矽的結晶性良好，導致透光性變差，使量子點轉換效率降低，而在包覆二氧化矽後可有效提升熱穩定性。
第三部分為探討包覆二氧化矽前後的Zn0.5量子點混合環氧樹脂後，以紫光晶片激發得到白光LED元件(Zn0.5-XLEDy及Zn0.5@SiO2-XLEDy，X=反應時間、y=量子點含量)，並探討白光元件特性。結果顯示Zn0.5-5LED10及Zn0.5@SiO2-5LED3有最高發光效率分別為30.6及19.4 lm/W，而Zn0.5@SiO2-13LED2在261小時長時間點亮後，發光效率僅僅下降6 %，穩定性最佳。
以上結果得知，可藉由調控鋅鎘莫耳比例及反應時間製備ZnxCd1-xS白光量子點，並且在白光量子點外圍包覆二氧化矽後可提升穩定性。利用紫光晶片作為激發源，可得到高發光效率及穩定性的WLED。

Quantun dots (QDs) have gradually replaced traditional phosphors to prepare white light-emitting diodes (WLEDs) due to they have the advantages of color tunability, broad excitation and high quantum yield (QY). However, obtaining white light need to mixing different color of QDs resulting in reducing luminous efficacy of the device due to the reabsorption effect. Moreover, the preparation process is complexed and troublesome. In recent years, the process of ternary alloyed QDs has gradually getting attention not only the emission wavelengths can be controlled by the particle size but by controlling the composition. Therefore, in this study, we demonstrated a colloidal chemistry method to prepare ZnxCd1-xS (named as Znx) QDs with band edge and surface state emission wavelengths by using non-coordinating complexing agent-oleic acid (OA) and solvent-octadecene (ODE) at low temperature. Then, Znx QDs were coated with silica and mixed with encapsulant to prepare WLED.
This study is mainly divided into three parts. The first one is the preparation and characterization of Znx QDs by controlling the molar ratios of zinc and cadmium. The results show that the particle size becomes smaller and the emission is blue-shifted as increasing the zinc content, and the stability of QDs can be improved due to the higher covalent of ZnS than CdS.
The second part is to control the reaction time of Zn0.5 QDs, and coating with the silica on the QDs surface (named as Zn0.5@SiO2). The results show that the highest QY (86 %) can be obtained at reacts for 5 min. When increases the reaction time, the emission wavelength will red-shifted due to the nonlinear optical effects of alloying. Perlong the reaction time to 20 min, emission wavelength was blue shift due to a large amount of zinc replacement Cd, and the QDs growth tends to saturate. As the reaction time increases, Znx QDs gradually change from a cadmium-rich core to a rich in zinc-cadmium on the surface . After zinc diffuses into the interior, the stability of the QDs can be improved. The QDs agglomerate after coating with the silica resulting in the emission wavelength red-shifted. The thermal stability of Zn0.5@SiO2 QDs can be effectively improved by coating with silica. However, the conversion efficiency of QDs is reduced due to the good crystallinity of silica resulting in the light transmittance is decay.
The third part is the fabrication and measurement of devices. Zn0.5 and Zn0.5@SiO2 QDs were mixed with epoxy resin and excited by the UV chip (named as Zn0.5-XLEDy and Zn0.5@SiO2-XLEDy, X = reaction time, y = QDs content). The results show that Zn0.5-5LED10 and Zn0.5@SiO2-5LED3 have the highest luminous efficacy of 30.6 and 19.4 lm/W, respectively. After operated for a long period of 261 h, the luminous efficacy of Zn0.5@SiO2-13LED2 was, only reduced 6 % shows the highest stability of WLED.
The above results show that ZnxCd1-xS QDs can be prepared by controlling the zinc -cadmium molar ratios and reaction time, and the QDs coated with silica can improve the stability. WLED with high luminous efficacy of 30.6 lm/W and stability can be obtained by pumping with UV chip.

摘要........................................................................i
Abstract....................................................................iii
誌謝........................................................................v
目錄.......................................................................vi
表目錄......................................................................viii
圖目錄.......................................................................ix
第一章 前言..................................................................1
1.1 白光LED發展史............................................................1
1.2 市售白光LED..............................................................2
第二章 文獻回顧..............................................................4
2.1 零維奈米材料-量子點......................................................4
2.2 白光LED之製備方式........................................................5
2.3 白光量子點..............................................................12
2.4 量子點表面包覆..........................................................26
2.5 研究動機與目的..........................................................31
第三章 實驗方法與步驟........................................................33
3.1 實驗藥品................................................................33
3.2 ZnxCd1-xS量子點之製備方法................................................35
3.3 ZnxCd1-xS量子點包覆二氧化矽之製備方法.....................................35
3.4 白光LED元件封裝及穩定性..................................................35
3.5 Znx及Znx@SiO2量子點與LED元件之特性分析...................................39
第四章 結果與討論............................................................42
4.1 ZnxCd1-xS量子點之合成及分析..............................................42
4.1.1 Zn含量及反應時間對ZnxCd1-xS量子點之影響.................................42
4.1.2 Znx量子點之表面形貌及實際組成分析.......................................50
4.1.3 Znx量子點之晶體結構分析................................................53
4.1.4 Znx量子點之XPS與表面組成分析...........................................55
4.1.5 Znx量子點之穩定性......................................................59
4.2 Zn0.5及Zn0.5@SiO2量子點之合成及分析......................................66
4.2.1反應時間對Zn0.5量子點光學性質之影響......................................66
4.2.2 Zn0.5量子點之表面形貌、晶體結構及實際組成分析............................69
4.2.3 Zn0.5量子點之XPS表面組成分析...........................................73
4.2.4 Zn0.5量子點之穩定性....................................................77
4.2.5 Zn0.5@SiO2量子點光學性質、表面形貌及晶體結構分析.........................84
4.2.6 Zn0.5及Zn0.5@SiO2量子點之熱穩定性測試...................................89
4.3 Zn0.5及Zn0.5@SiO2量子點白光發光二極體元件.................................91
4.3.1 Zn0.5及Zn0.5@SiO2量子點白光發光二極體元件之穩定性測試....................98
第五章 結論.................................................................106
參考文獻....................................................................107
Extended Abstract..........................................................117

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