臺灣博碩士論文加值系統

本論文研究的是上發光型有機發光二極體(TEOLED)的光電特性。本研究以玻璃,PET,矽晶圓…等，當基板製作TEOLED。(1)最初本研究著重在玻璃和矽基板上發光型有機發光二極體開發。選擇Ag（4.2 eV）作為反射陽極材料，選擇三氧化鉬MoO3作為空穴注入層（HIL），HOMO = 5.3 eV，LUMO = 2.3 eV，N,N'-Di(1-萘基) -N,N'-二苯基-(1,1'-聯苯)-4,4'-二胺 (NPB) 作為空穴傳輸層 (HTL)，HOMO = 5.5 eV 和 LUMO = 2.4 eV，Tris(8-羥基喹啉) ) 鋁 (Alq3 ) 發射層 (EML)，HOMO 5.62 eV 和 LUMO 2.85 eV，以及 2,2',2"-(1,3,5-苯並三基)-三(1-苯基-1-H-苯並咪唑) (TPBi)作為電子傳輸層(ETL)，HOMO = 6.7 eV，LUMO = 2.7 eV。半透明陰極由LiF/Al組成。元件結構如下:glass or PET/ITO/Ag (80 nm)/MoO3 (2 nm)/NPB (30 nm)/Alq3 (55 nm) / TPBi (10 nm) /LiF (0.8 nm) /Al（15 nm）。作為研究的一部份，還測量了柔性PET基板的最大彎曲半徑，以優化其彎曲性能。glass/ITO 上的元件的亮度為 738.4 cd/m2，電流密度為 7.93 mA/cm2，電流效率為 9.30 cd/A。 PET/ITO 上的元件亮度為 459.9 cd/m2，電流密度為 5.31 mA/cm2，電流效率為 8.98 cd/A。 已成功證明PET基板可承受4毫米的最大彎曲半徑而不變形。(ii) 本研究的主要目標是開發一種微型TEOLED元件，該元件具有增強的光電特性，如色純度、亮度、效率、穩定性和壽命。 因此，使用了厚度為 675 µm 的矽晶圓基板（基板購自台灣 Summit-Tech Resource Crop）。 微顯示器在增強現實 (AR) 和混合現實 (MR) 設備的創建中發揮著至關重要的作用。 此外，OLED元件在性能和穩定性方面可以受益於矽晶圓基板。例如，它可以幫助降低製造和使用過程中損壞或分層的風險，並可以提高元件的散熱性能。 因此，該元件可以更加耐用和可靠，並具有改進的性能特徵。為了在矽基板上製作微型上發光OLED元件，選擇Al作為反射陽極，Dipyrazino[2,3-f:2',3'-h] quinoxaline-2,3,6,7,10， 採用 11-六甲腈 (HATCN) 作為電洞注入層 (HIL)，HOMO = 9.5 eV，LUMO = 4.5 eV，N, N'-Di(1-萘基)-N,N'-二苯基-(1, 1′-聯苯)-4,4′-二胺 (NPB) 作為電洞傳輸層 (HTL)，HOMO = 5.5 eV，LUMO = 2.4 eV，2,4-二苯基-6-雙(12-苯基吲哚) [2 ,3-a]咔唑-11-基)-1,3,5-三嗪 (DIC–TRZ) 熱激活延遲熒光 (TADF) 主體發射材料，HOMO = 5.5 eV，LUMO = 2.65，Tris[2-(p -甲苯基)吡啶]銥(III)，HOMO = 5.6 eV，LUMO = 3.0 eV，Ir(mppy)3 作為摻雜發射材料，2,2',2"-(1,3,5-苯並三基)-tris (1-苯基-1-H-苯並咪唑)(TPBi)作為電子傳輸層(ETL)，HOMO = 6.7 eV，LUMO = 2.7 eV，半透明陰極由LiF/Al組成，元件結構如下 矽/Al (100 nm)/ HATCN (10 nm) / Dic-TRZ: Ir(mppy)3 (40 nm)/ TPBi (30 nm) / LiF 1.2 nm /Al 19.9 nm。矽基板的選擇對於在微型TEOLED中開發增強光電特性的研究目標的成功至關重要。 研究優化半透明陰極層的厚度和陽極層的表面粗糙度，這些因素會影響TE-OLED的光學性能、TEOLED的微共振腔效應、TE-OLED的摻雜濃度影響、HTL引起的頻譜偏移 + EML 層厚度以及基於摻雜濃度和熱導率的元件壽命。 通過調整Al（19.9 nm）有機層、HIL（HATCN 10 nm）、HTL（NPB 30 nm）、ETL（TPBi 30 nm）的厚度，ETL (TPBi 30 nm)、EML (DIC–TRZ: Ir(mppy)3 40 nm) 和摻雜濃度，我們成功地在矽基板上製造了高效的TEOLED。 這使得摻雜濃度較高的元件具有更好的光電性能。 在我們的實驗中，38% 的摻雜濃度導致最大電流密度為 201.97 mA/cm2，亮度為 4776 cd/m2，電壓為 9 V 時效率為 2.36 cd/A。高摻雜濃度導致光譜區域較窄，表明微共振腔效應較強。 除了測量不同濃度元件的壽命外，製造的元件的壽命還根據亮度性能而變化。 我們的摻雜濃度為 38% 的 Si-TEOLED 實現了 420 小時（半衰期）。

This dissertation is about the study of electro-optical characteristics of top-emission organic light-emitting diodes. The purpose of this study is to develop the top emission OLED device on various substrates, such as glass, PET, and silicon wafers. (i) In the beginning, this study was focused on the development of top emission on glass and PET substrate. As the reflective anode material, Ag (4.2 eV) was chosen, and Molybdenum trioxide MoO3 was chosen as the hole injection layer (HIL) with HOMO = 5.3 eV and LUMO = 2.3 eV, N, N′-Di(1-naphthyl)-N,N′-diphenyl-(1,1′-biphenyl)-4,4′-diamine (NPB) as the hole transport layer (HTL) with HOMO = 5.5 eV and LUMO = 2.4 eV, Tris(8-hydroxyquinoline)aluminum (Alq3 ) Emission layer (EML) with HOMO 5.62 eV and LUMO 2.85 eV, and 2,2',2"-(1,3,5-Benzinetriyl)-tris(1-phenyl-1-H-benzimidazole) (TPBi) as electron transport layer (ETL) with HOMO = 6.7 eV and LUMO = 2.7 eV. The semi-transparent cathode is composed of LiF/Al. The device structure is as follow: Glass or PET/ITO/Ag (80 nm)/MoO3 (2 nm)/ NPB (30 nm) / Alq3 (55 nm) / TPBi (10 nm) /LiF (0.8 nm) /Al (15 nm). As part of the study, maximum bending radius for flexible PET substrates was also measured in order to optimize their bending performance. Device on Glass /ITO resulted in luminance of 738.4 cd/m2, current density of 7.93 mA/cm2, and current efficiency of 9.30 cd/A. And the device on PET/ITO resulted in luminance of 459.9 cd/m2, Current density of 5.31 mA/cm2 and the current efficiency of 8.98 cd/A. It has been successfully demonstrated that PET substrates can withstand the maximum bending radius of 4 mm without deforming. (ii) The main goal of the research is to develop a micro Top emission OLED (Organic Light Emitting Diode) device that has enhanced electro-optical properties such as color purity, luminance, efficiency, stability, and lifetime. As a result, silicon wafer substrates with a thickness of 675 µm have been used (The Substrate Purchase from Summit-Tech Resource Crop. Taiwan). A microdisplays plays a crucial role in the creation of augmented reality (AR) and mixed reality (MR) devices. Furthermore, OLED devices can benefit from silicon wafer substrates in terms of performance and stability. For example, it can help reduce the risk of damage or delamination during fabrication and use, and can improve the heat dissipation properties of the device. As a result, the device can be more durable and reliable, with improved performance characteristics. To fabricate the micro top-emission OLED device on silicon wafer substrate, Al is selected as a reflective anode, Dipyrazino[2,3-f:2',3'-h] quinoxaline-2,3,6,7,10,11-hexacarbonitrile (HATCN) is employed as the hole-injection layer (HIL) with HOMO = 9.5 eV and LUMO = 4.5 eV, N, N′-Di(1-naphthyl)-N,N′-diphenyl-(1,1′-biphenyl)-4,4′-diamine (NPB) as the hole transport layer (HTL) with HOMO = 5.5 eV and LUMO = 2.4 eV, 2,4-diphenyl-6-bis(12-phenylindolo) [2,3-a] carbazole-11-yl)-1,3,5-triazine (DIC–TRZ) Thermally Activated Delayed Fluorescence (TADF) host emitting material with HOMO = 5.5 eV and LUMO = 2.65, Tris[2-(p-tolyl)pyridine]iridium(III) with HOMO = 5.6 eV, LUMO = 3.0 eV, Ir(mppy)3 as dopant emitting material, and 2,2',2"-(1,3,5-Benzinetriyl)-tris(1-phenyl-1-H-benzimidazole) (TPBi) as electron transport layer (ETL) with HOMO = 6.7 eV and LUMO = 2.7 eV. The semi-transparent cathode is composed of LiF/Al. The device structure is as follow Silicon/Al (100nm)/ HATCN (10 nm) / Dic-TRZ: Ir(mppy)3 (40 nm)/ TPBi (30 nm) / LiF 1.2 nm /Al 19.9 nm. The choice of a silicon wafer substrate is crucial to the success of the research goal of developing enhanced electro-optical properties in micro Top emission OLEDs. The study is optimize the thickness of a semitransparent cathode layer and the surface roughness of anode layers, which affect the optical properties of TE-OLEDs, the microcavity effect on TEOLEDs, the dopant concentration impact on TE-OLEDs, the spactra shift due to HTL + EML layer thickness, and the device's lifetime based on dopant concentration and thermal conductivity. By adjusting the thickness of Cathode Al (19.9 nm) organic layer, HIL (HATCN 10 nm), HTL (NPB 30 nm), ETL (TPBi 30 nm), EML (DIC–TRZ: Ir(mppy)3 40 nm) and dopant concentrations, we successfully fabricated an efficient top emission OLED on si substrate. This results in better electro-optical performance for devices with higher dopant concentrations. In our experiments, a 38% dopant concentration resulted in a maximum current density of 201.97 mA/cm2, a luminance of 4776 cd/m2, and an efficiency of 2.36 cd/A at a voltage of 9 V. The high dopant concentration resulted in a narrow spectral area, indicating a strong microcavity effect. In addition to measuring the lifetime of devices with different concentrations, the lifetime of fabricated devices varies according to luminance performance. 420 hours (half-life) were achieved by our Si-TEOLED with a 38 % dopant concentration.

Abstract......i
Chinese abstract......iii
Acknowledgment......v
Table of contents......vi
List of tables......ix
List of Figures......xi
List of symbols and abbreviations......xvi
Chapter 1 Introduction......1
1.1 History of organic light emitting diodes......1
1.1.1 OLED Market Size......4
1.2 Principle of OLED devices......5
1.3 Generations of OLED and Light Emission Mechanism......9
1.3.1 List of materials use for small molecule OLED devices (Example)......11
1.4 Physics of OLED......16
1.4.1 Organic semiconductors......16
1.4.2 Theory of Space charge limited current and Injection limited current......17
1.4.3 Light Emission Efficiency in OLED......19
1.5 Classifications of OLED......20
1.5.1 AMOLED (Active Matrix Organic Light Emitting Diode):......20
1.5.2 Passive-matrix OLED (PMOLED):......20
1.5.3 Bottom emission OLED:......21
1.5.4 Top-emission OLED:......21
1.5.5 Transparent OLED:......22
1.5.6 Inverted OLED:......22
1.6 Application of OLED technology......22
1.7 Advantages and disadvantages of OLED devices......24
1.7.1 Advantages......24
1.7.2 Disadvantages......24
Chapter 2 Litrature Review......25
2.1 Introduction of top emission OLED devices......25
2.1.1 Materials for anode layer (Top-emission OLED)......26
2.1.2 Materials for cathode layer (Top-emission OLED)......27
2.2.3 Microcavity phenomenon in (Top- emission OLED)......27
2.2 Paper study of top- emission OLED on, Glass PET substrate......31
2.3 Paper study of top –emission OLED on, silicon substrate......33
Chapter 3 Experiment materials and Equipments......41
3.1 Material and function......41
3.2 Equipment and operating system for TOLED fabrication......42
3.2.1 Ultrasonic cleaner and UV Ozone......42
3.2.2 Thermally Evaporated Machine......43
3.2.3 Glove box system......46
3.2.4 Measurment system......46
3.2.5 Life time measurement system......47
3.2.6 Bending test system......48
3.2.7 Other measuring equipment......48
3.3 OLED fabrication process......49
3.3.1 Fabrication process of Glass and PET substrate based TEOLED device......49
3.3.2 Fabrication process of Silicon substrate based TEOLED device......54
Chapter 4 Results and Discussions......62
4.1 Result discussion of Glass and PET substrate based TE-OLED......62
4.1.1 Glass/ITO TE-OLEDs......62
4.1.2 PET/ITO TE-OLEDs......66
4.1.3 Flexibility test......69
4.2 Results discussion of silicon based TE-OLED device......70
4.2.1 Semitransparent cathode layer......70
4.2.2 Anode layer on (Silicon substrate)......77
4.2.3 Hole only and Electron only device......85
4.2.4 Hole injection layer (HATCN)......87
4.2.5 Hole transport layer (NPB)......91
4.2.6 Electron transport layer (TPBi)......95
4.2.7 Emission layer DIC-TRZ:Ir(mppy)3......99
4.2.8 Si-TEOLED life time measurement......103
4.2.9 HTL +EML layer thickness (Spectra shift)......105
4.2.10 Comparison of EL intensity of TE-OLED (Si) and BE-OLED (glass)......108
4.2.11 Thermal conductivity of Si- TEOLED......109
Chapter 5 Conclusions......110
References......114
Extended Abstract......124

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