有機發光二極體（OLED）在智能手機、智能手表、平板電腦和電視等傳統顯示技術上取得了優異表現，同時逐漸在固態照明行業中占據了相當大的份額；OLED由於在高對比度、超薄、易於適應、全彩色、平板顯示和固態照明等應用方面的優點，吸引了廣泛關注。如今，OLED幾乎壟斷了便攜式顯示市場，並以相當高的效率和操作穩定性積極爭奪大面積顯示屏的地位。
OLED由不同層組成，包括電洞注入層（HIL），其促進大部分載流子（電洞）進入發光層並有效阻止少數載流子（電子）進入電洞傳輸/注入層。氧化鋅（ZnO）由於具有高光學透明性、優異的熱穩定性、寬能隙、天然豐富以及具有經濟性等獨特性質，已成為HIL的有利候選材料。

在這項研究中，我們研究了將氧化鋅（ZnO）奈米材料，即0D奈米點、1D奈米線、2D奈米片和3D奈米花，作為HIL，以改善OLED的性能；這些ZnO奈米材料是使用水熱法合成的，並使用掃描電子顯微鏡（SEM）、穿透式電子顯微鏡（TEM）、X光繞射儀（XRD）、紫外光電子能譜（UPS）、原子力顯微鏡（AFM）和紫外可見光譜等方法對其結構、形態和光學性質進行分析。

形態分析顯示，奈米點的平均尺寸為35 nm，奈米線為20 nm，奈米片為20-25 nm，奈米花則為150 nm；對ZnO奈米材料的光學分析，展示了每種奈米材料吸收和穿透性質的變化；0D的吸收波長為260 nm，1D為391 nm，2D為274 nm，而3D為265 nm；0D、1D、2D和3D奈米粒子的穿透率分別為93%、86%、88%和82%；吸收和穿透性質的差異，歸因於ZnO奈米材料的尺寸和形貌；所有合成的ZnO奈米材料的結晶度都很高，這表明研究中使用的水熱法可有效合成高質量的ZnO奈米材料；該研究還調查了處理時間和加熱溫度對合成的ZnO奈米材料性質的影響；結果顯示，延長處理時間和加熱溫度，導致了顆粒尺寸變大，結晶度降低。

在濕式製程的OLED元件中，將氧化鋅（ZnO）奈米材料摻雜於PEDOT:PSS（HIL）中，顯著提高了元件效率；改善程度取決於ZnO奈米顆粒尺寸和摻入PEDOT:PSS的比例；具體而言，我們發現掺雜0D氧化鋅奈米點顯著提高了效率，相較於未掺雜的PEDOT:PSS對照組，效率提升了24%；同樣地，掺雜1D奈米線、2D奈米片和3D奈米花，相較於未掺雜的元件，效率分別提升了64%、28%和20%。

因此，這項研究突顯了氧化鋅（ZnO）奈米顆粒作為HIL/HTL對於高效率OLED元件的潛力；使用不同尺寸的ZnO奈米材料，增強了層的注入和阻斷特性，且其易於合成和應用於旋轉塗佈，最終提升了元件性能；特別是1D的氧化鋅奈米線對元件性能有巨大影響；這些奈米顆粒可以應用於各種發光顏色（藍色、綠色、黃色、橙色或紅色）、世代類型（第1代、第2代或第3代）和製程（濕式或乾式）；這項研究是使OLED技術更加高效和可持續的重要一步，從而為更美好的未來做出貢獻。

Organic light-emitting diodes (OLEDs) have outperformed the conventional display technologies in smartphones, smartwatches, tablets, and televisions, while gradually thriving to cover a sizable fraction of the solid-state lighting industry. OLEDs have attracted great attention due to their applications in high-contrast, innate thin, easily adaptable, full-color, flat-panel displays and solid-state lighting. Nowadays, OLEDs are almost unanimously leading the portable display market and strongly contest large-area displays with reasonably sound efficiency and operational stability.
OLEDs are composed of different layers, including the hole injection layer (HIL) that facilitates transporting the majority carrier (holes) into the emissive layer and effectively blocks minority carriers (electrons) to transport into the hole-transport/-injection layer. Zinc oxide (ZnO) has emerged as a promising candidate for HILs owing to its unique properties like high optical transparency, excellent thermal stability, wide bandgap, abundance in nature, and economical.
In this study, we investigated the incorporation of ZnO nanomaterials i.e., 0D nanoparticles, 1D nanowires, 2D nanosheets, and 3D nanoflowers as HILs for improved OLED performance. The ZnO nanomaterials were synthesized using the hydrothermal method, and their structural, morphological, and optical properties were characterized using scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), ultraviolet photoelectron spectroscopy (UPS), atomic force microscopy (AFM), and UV-visible spectroscopy.
The morphology analysis showed that the nanoparticles had an average size of 35 nm, nanowires of 20 nm, nanosheets of 20-25 nm, and nanoflowers of 150 nm. The optical characterization of the ZnO nanomaterials revealed variations in the absorption and transmission properties of each nanomaterial. The absorption wavelength for 0D was determined to be 260 nm, 1D was 391 nm, 2D was 274 nm, and 3D had an absorption wavelength of 265 nm. The transmission for 0D, 1D, 2D, and 3D nanostructures was 93, 86, 88, and 82%, respectively. The differences in absorption and transmission properties were attributed to the size and morphology of the ZnO nanomaterials. The crystallinity of all the synthesized ZnO nanomaterials was high, indicating that the hydrothermal method used in the study was effective in synthesizing high-quality ZnO nanomaterials. The study also investigated the effects of processing time and heating temperature on the properties of the synthesized ZnO nanomaterials. The results showed that prolonged processing times and heating temperatures resulted in larger particle sizes and reduced crystallinity.
The inclusion of ZnO nanomaterials doped in PEDOT:PSS (HIL) significantly improved the efficiency of wet-processed OLED devices. The extent of improvement depends on the dimensionality and doping ratio (50,100,200μL) of the ZnO nanomaterials and PEDOT:PSS. Specifically, we found that the incorporation of doped 0D ZnO nanoparticles leads to a notable improvement in efficiency, resulting in a 24% enhancement compared to the undoped PEDOT:PSS counterpart. Similarly, the inclusion of doped 1D nanowires, 2D nanosheets, and 3D nanoflowers lead to an improvement of 64, 28 and 20%, respectively, compared to the undoped device.
Therefore, this study highlights the potential of ZnO nanostructures as HIL/HTLs for high-efficiency OLED devices. The use of various dimensional ZnO nanomaterials enhances the injection and blocking properties of the layer which are easy to synthesize and spin-coat during fabrication, ultimately leading to the enhancement in device performance. Especially, 1D ZnO nanowires that display a tremendous impact on the device performance might be because of the smallest diameter amongst the other materials. The nanoparticles can be utilized in a variety of emission colors (blue, green, yellow, orange, or red), generation types (generation 1, generation 2 or generation 3), and fabrication processes (wet or dry process). This research is a significant step towards making OLED technology even more efficient and sustainable, thus contributing to a better future.

Chinese Abstract……………………………………………………………………ii-iv
English Abstract……………………………………………………………..……..v-vii
Acknowledgement…………………………………………………………….…..viii-x
Contents………………………………………………...………………………..xi-xvii
Figure Captions………………………………………………………………..xviii-xxv
Table Captions……………………………………………………...………..xxvi-xxvii
Abbreviations…………………………………………………….…………..xxviii-xxx
Chapter 1. Introduction and Motivation………………………………………….1-6
Chapter 2. Fundamentals of Organic Light Emitting Diode (OLED)………….7-28
2.1. History and Development of OLED…………………………………………7-13
2.2. World Revenue of OLED…………………………………………...………13-16
2.2.1. Display…………………………………………………………………13
2.2.2. Lighting………………………………………………………………..14
2.3. OLED Device Structure and Working Mechanism…………………….…16-28
2.3.1. Fabrication Techniques……………………………………….……19-20
2.3.1.1. Dry Process………………………………………………….20
2.3.1.2. Wet Process………….………………………………………20
2.3.2. Functional Layers in OLED……………………………………..….21-25
2.3.2.1. Substrate…………………….……………………………….22
2.3.2.2. Electrodes……………………………………………………23
2.3.2.2.1. Anode………………………………………………23
2.3.2.2.2. Cathode…………………………………………….23
2.3.2.3. Carrier Transport Layer……………….………………….24-25
2.3.2.3.1. Hole-injection Layer (HIL)………………………..24
2.3.2.3.2. Hole-transport Layer (HTL)……………………….24
2.3.2.3.3. Electron-transport layer (ETL)……………………..24
2.3.2.3.4. Electron-injection Layer (EIL)……………………..25
2.3.2.4. Emissive Layer………………………………………………25
2.3.3. Key Parameters of OLED…………………………………………..26-28
2.3.3.1. Turn-on Voltage (Von)………………………………………..26
2.3.3.2. Operating Voltage………………………………………...….26
2.3.3.3. Power Efficacy (PE)………………………………………….26
2.3.3.4. Current Efficacy (CE)………………………………………..26
2.3.3.5. External Quantum Efficiency (EQE)…………………...……27
2.3.3.6. CIE Color Coordinates……………………………………….27
2.3.3.7. Luminance………….………………………………………..28
Chapter 3. Literature Review………………………...…………………………29-59
3.1. Nanostructures of Various Dimensions…………………………………….29-36
3.1.1. Zero Dimensional (0D) Nanostructures………………………………..32
3.1.2. One Dimensional (1D) Nanostructures………………………………...33
3.1.3. Two Dimensional (2D) Nanostructures………………………………..34
3.1.4. Three Dimensional (3D) Nanostructures………………………………35
3.2. Nanomaterials for OLEDs……………………………...…………………..36-46
3.2.1. Copper Oxide (CuO)…………………………………………………..36
3.2.2. Molybdenum Trioxide (MoO3)………………………………………..38
3.2.3. Tungsten Trioxide (WO3)………………………………………………40
3.2.4. Vanadium Oxide (V2O5)………………………………………………..42
3.2.5. Zinc Oxide (ZnO)………………………………………………………43
3.3. ZnO Nanostructures of Various Dimensions……………………………....46-55
3.3.1. 0-D ZnO Nanoparticles……………………………………………...…46
3.3.2. 1-D ZnO Nanowires……………………………………………………49
3.3.3. 2-D ZnO Nanosheets…………………………………………………...51
3.3.4. 3-D ZnO Nanoflowers…………………………………………………53
3.4. ZnO Nanostructures for OLEDs………………………………...…………55-59
3.4.1. Use in OLEDs………………………………………………………….55
3.4.2. Advantages and Limitations……………………………………………57
Chapter 4. Characterization and Experiments…………….…………………..60-65
4.1. OLED Materials…………………………………...………………………..60-61
4.1.1. Anode and Cathode Materials…………………………………………60
4.1.2. HIL and HTL Materials………………….…………………………….60
4.1.3. Emissive Materials……………………………………………………..61
4.1.3.1. Host Material………………………………………………...61
4.1.3.2. Emitter Material……………………………………………...61
4.1.4. EIL and ETL Materials……….………………………………………...61
4.2. Material Characterization………………………………………...………..62-64
4.2.1. Ultra-violet Visible (UV-vis) ………..…………………………….…...62
4.2.1.1. Absorbance………..…………………………………….…...62
4.2.1.2. Transmittance………..………………………………….…...62
4.2.2. Ultraviolet Photoelectron Spectroscopy (UPS) ………..……………...63
4.2.3. Scanning Electron Microscopy (SEM) ………..……………………....63
4.2.4. Transmission Electron Microscopy (TEM) ………..………...………...63
4.2.5. X-Ray Diffraction (XRD) ………..…………………………………....63
4.2.6. Atomic Force Microscopy (AFM) .…………………………………....64
4.3. Device Fabrication………………………………………………………..…64-65
4.3.1. Cleaning and UV Treatment.…………………………...……………....64
4.3.2. HIL coating.……………………………………..…………………......64
4.3.3. EML Coating.……………………………………………………….....64
4.3.4. Deposition of ETL, EIL and Cathode.………………………………….65
4.4. Device Testing.…………………………………….…………………………….65
Chapter 5. Result and Discussion………………………………………...……66-126
5.1. 0D- ZnO Nanoparticles Enabling High-efficiency OLEDs……………….66-79
5.1.1. Material Synthesis.………………………………………….………….68
5.1.2. Material Characteristics.……………………………………………….69
5.1.2.1. Scanning Electron Microscopy (SEM) .…………….……….69
5.1.2.2. Transmission Electron Microscopy (TEM) ………………….70
5.1.2.3. X-Ray Diffraction (XRD) ………………………………..….71
5.1.2.4. UV-Visible Spectrum……………………………………..….72
5.1.2.5. Ultraviolet Photoelectron Spectroscopy (UPS) ……………...73
5.1.2.6. Atomic Force Microscopy (AFM) ……………………….….74
5.1.3. Electroluminescent Properties………………………………………....76
5.2. 1D- ZnO Nanoparticles Enabling High-efficiency OLEDs…………...…..80-97
5.2.1. Material Synthesis……………………………………………...……....83
5.2.2. Material Characteristics……………………………………..………....85
5.2.2.1. Scanning Electron Microscopy (SEM) ……….……………..85
5.2.2.2. Transmission Electron Microscopy (TEM) …...……………..86
5.2.2.3. Energy-dispersive X-Ray (EDX) Spectroscopy……………..88
5.2.2.4. X-Ray Diffraction (XRD) …………………….……………..89
5.2.2.5. UV-Visible Spectrum…………………………….…………..90
5.2.2.6. Ultraviolet Photoelectron Spectroscopy (UPS) ….…………..91
5.2.2.7. Atomic Force Microscopy (AFM) …………………………..92
5.2.3. Electroluminescent Properties………………………………..………..93
5.3. 2D- ZnO Nanoparticles Enabling High-efficiency OLEDs……………...98-113
5.3.1. Material Synthesis………………………………………………….…101
5.3.2. Material Characteristics………………………...………………….…103
5.3.2.1. Scanning Electron Microscopy (SEM) .………………….…103
5.3.2.2. X-Ray Diffraction (XRD) .……………………...……….…105
5.3.2.3. UV-Visible Spectrum.…………………….……..……….…106
5.3.2.4. Ultraviolet Photoelectron Spectroscopy (UPS) .……………107
5.3.2.5. Atomic Force Microscopy (AFM) .………………..…….…108
5.3.3. Electroluminescent Properties.…………………………………….…109
5.4. 3D- ZnO Nanoparticles Enabling High-efficiency OLEDs………….….114-126
5.4.1. Material Synthesis………………………………………………….…117
5.4.2. Material Characteristics………………………………………….…...118
5.4.2.1. Scanning Electron Microscopy (SEM) ………….…….…...118
5.4.2.2. X-Ray Diffraction (XRD) ………………………….….…...119
5.4.2.3. UV-Visible Spectrum…………………………………..…...120
5.4.2.4. Ultraviolet Photoelectron Spectroscopy (UPS) …….….…...121
5.4.2.5. Atomic Force Microscopy (AFM) …………….……….…...122
5.4.3. Electroluminescent Properties……………….…………………….....123
Chapter 6. Conclusion……………………………………………………...…127-131
References….…………………………………………………….................…132-150
Appendix….……………………………………………………...................…151-163
Curriculum Vitae of Author………………………………….....................…164-168

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