臺灣博碩士論文加值系統

有鑒於有機發光二極體 (Organic light-emitting diode, OLED) 領域近數十年來的蓬勃發展，改進相關元件效能與開發相關物理量測技術在領域中目前還充滿研發動力，同時也是未來使用OLED為基礎的產品量產、提升產品品質與功能不可或缺的重要條件。本博士論文主要以提升OLED元件載子注入、傳輸等特性進而提升元件效率、穩定性、甚至使其應用領域更廣為主要研究動機，提出數個與元件中載子注入層相關的研究題目。同時，相關研究成果也為有機電子領域提供研究材料物理特性新的分析手段。
首先，本論文提出數個載子注入結構，透過有機小分子與無機鹽類共摻雜 (electrical doping)的方式，提出『階梯狀摻雜結構 (stepwise)』與『漸進式摻雜結構(graded)』，接得到出色的元件注入效率提升，進而提升OLED元件效率。以上兩個摻雜結構分別使用了NPB:MoO3與MADN:Rb2CO3兩個材料組合。後者更接續被應用在 『倒置式有機發光二極體 (inverted bottom emission organic light-emitting diode, IBOLED) 』結構。
此外，利用『導納頻譜與阻抗頻譜(admittance/impedance spectroscopy) 』技術，有別於一般OLED元件分析手法，只能透過其電壓電流曲線，或元件導通之後的發光行為對元件進行分析，此手法能為我們提供元件中載子行為的寶貴資訊。在元件操作下，可成功觀察包括注入、傳播、堆積、再結合等載子行為。透過不同的元件模型設計，與兩個材料間介面相關的活化能亦能被量化分析。
最後，我們成功結合『電鍍』手法製備的硫氰酸亞銅薄膜於OLED元件。透過調整電鍍時沉積的參數，取得OLED元件需求的薄膜。利用『熱退火』與『UV-O3』的表面處理，有機非晶向薄膜與此無機硫氰酸亞銅之相容性大大提高，元件效能亦得到高度提升。在研究過程中，我們也提供了有機小分子與無機硫氰酸亞銅之介面電物理、光物理、表面能量……等多面向研究成果。

In this thesis, we focus mainly on the processes and factors to improve OLED performance by enhancing the charge carrier injection, transport, and balance. Even though the field has been developed for decades, there is still space for performance improvement for OLEDs. Additionally, new type of carrier injection/transport layer is still drawing much attention for highly efficient, stable OLEDs and also for a wider potential application. It is also crucial to develop different physical analysis models and methodologies. In particular, with OLED device engineering and the development of new device analysis techniques, we provide new way to investigate the carrier behavior in the device under operation to considerably improve the performance of OLEDs and offer the observation and understanding of underlying mechanisms.
First, the several carrier injection layer using electrical doping techneques were proposed. A step-wise hole injection layer using NPB:MoO3 was demostrated. Graded doped n-type electron injection layer using MADN:Rb2CO3 was also prosposed. The J-V-L characteristics of OLEDs indicated that these stepwise/graded injection layers are superior by showing improved device performances on OLEDs. The mechanisms behind the enhancements were studied. In summary, the cascading energy level which efficiently distributed the energy barrier from ITO to carrier transport layer, therefore enhanced both hole injection and transport efficiency and led to better carrier balance and luminance efficiencies in OLEDs. MADN:Rb2CO3 were used for electron injection layer for inverted bottom emission organic light-emitting diode application.
Second, organic analysis techniques based on admittance/impedance spectroscopy were developed. In general, the behavior of charge carriers could only be observed by either the light emitted or the observed current goes through the device. By admittance/impedance spectroscopy, the models provide valuable information about the carrier information in OLEDs under operation, including injection, transport, accumulation, and recombination. Besides, activation energy corresponding to the charge injection energy barrier is also available with this methodology.
Finally, we demonstrate the integration of aqueous electrolyte-based electro-deposited CuSCN with conventional vacuum-deposited OLEDs. By controlling various deposition parameters, we realized the fabrication of CuSCN thin films with an excellent surface roughness that meets the criteria of typical OLED devices. The optical, electrical and material characterizations of these thin films were also investigated. In addition, interfacial energetic evidence obtained by ultraviolet photoelectron spectroscopy (UPS) revealed the mechanisms behind the injection enhancements. For the first time, we successfully incorporated electro-deposited CuSCN into conventional OLEDs, which exhibited notable device performances comparable to the highest reported efficiencies utilizing the identical emitting system. The effect of surface UV-O3 treatment and annealing were well studied.

Abstract i
中文摘要 iii
List of Author’s Journal Paper Publications v
Table of contents vii
List of Figures x
List of Tables xvii
Chapter 1. Introduction 1
1.1. Brief review on organic electronics 1
1.2. The development history and basic of organic light-emitting diodes (OLEDs) 5
1.2.1. History of OLED applications 5
1.2.2. The way of OLEDs to commercialization 9
1.2.3. The challenges remain 12
1.3. Aim and the scope of this thesis 13
1.4. Thesis outline 14
Chapter 2. Theories and background knowledge 15
2.1. Basic of organic semiconductors 15
2.1.1. Molecular orbitals 15
2.1.2. HOMO/LUMO band structure 16
2.2. Design of OLEDs 18
2.2.1. Working principles of OLEDs 18
2.2.2. Device structure classification 20
2.3. Charge carrier injection 21
2.3.1. Ohmic contact 21
2.3.2. Tunneling injection 22
2.4. Doping of organic semiconductors 23
2.4.1. Doping fundamentals 24
2.4.2. Controlling the Fermi level by doping 25
2.4.3. P-type doping and their mechanisms 26
2.5. Admittance/impedance spectroscopy 26
2.6. Ultraviolet photoelectron spectroscopy 27
Chapter 3. Experimental and measurements 31
3.1. Device fabrication 31
3.1.1. Materials and device design 31
3.1.2. Substrate cleaning 36
3.1.3. Thin film deposition 37
3.1.4. Electro-deposition of CuSCN thin film 38
3.2. Treatments to the samples 39
3.2.1. Thermal annealing treatment 39
3.2.2. UV-O3 treatment 40
3.3. Characterization of OLEDs 40
3.3.1. J-V-L and current efficiency 40
3.3.2. Electroluminescence spectra 41
3.3.3. Admittance and impedance spectroscopy 42
3.4. Material, and thin film characterizations 43
3.4.1. Atomic force microscopy 43
3.4.2. Contact angle, surface energy, and polarity 44
3.4.3. Energy dispersive X-ray spectrometer 45
3.4.4. Optical transmittance spectra 45
3.4.5. Secondary ion mass spectrometry 45
3.4.6. Scanning electron microscopy 45
3.4.7. Ultraviolet photoelectron spectroscopy and X-ray photoelectron spectroscopy 46
3.4.8. Variable angle spectroscopic ellipsometry 47
3.4.9. X-ray diffraction 48
Chapter 4. Results and discussion 49
4.1. Topic I. Effects of novel transition metal oxide doped bilayer structure on hole injection and transport characteristics for organic light-emitting diodes 49
4.1.1. Abstract 49
4.1.2. Introduction 50
4.1.3. Results and discussion 51
4.1.4. Conclusion 69
4.2. Topic II. 2-Methyl-9,10-bis(naphthalen-2-yl)anthracene doped rubidium carbonate as an effective electron injecting interlayer on indium-tin oxide cathode in inverted bottom-emission organic light-emitting diodes 70
4.2.1. Abstract 70
4.2.2. Introduction 71
4.2.3. Results and discussion 74
4.2.4. Conclusion 88
4.3. Topic III. Organic Light-Emitting Diodes with an Electro-Deposited Copper(I) Thiocyanate (CuSCN) Hole-Injection Layer Based on Aqueous Electrolyte 89
4.3.1. Abstract 89
4.3.2. Introduction 89
4.3.3. Results and discussion 92
4.3.4. Conclusion 115
4.4. Topic IV. Improvement of OLED performances by applying annealing and surface treatment on electro-deposited CuSCN hole injection layer 116
4.4.1. Abstract 116
4.4.2. Introduction 117
4.4.3. Results and discussion 119
4.4.4. Conclusion 136
Chapter 5. Conclusion 138
Chapter 6. Future work 139
References 140

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