二維過渡金屬二鹵化物：合成、特性分析及在燭光 OLED 中的應用

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研究生：	夏荻本 Sharma, Dipanshu
論文名稱：	二維過渡金屬二鹵化物：合成、特性分析及在燭光 OLED 中的應用 Two-Dimensional Transition Metal Dichalcogenide: Synthesis, Characterization, and Application in Candlelight OLED
指導教授：	周卓煇 Jou, Jwo-Huei
口試委員:	蔡永誠 Tsai, York 董福慶 Tung, Fu-Ching 岑尚仁 Chen, Sun-Zen 如是 Siddiqui, Iram
學位類別：	博士 Doctor
系所名稱：	工學院 - 材料科學工程學系 Materials Science and Engineering
論文出版年：	2025
畢業學年度：	113
語文別：	英文
論文頁數：	104
中文關鍵詞：	過渡金屬二硫屬化物、二硫化鉬、二硫化鎢、低色溫燭光有機發光二極體
外文關鍵詞：	TMD, MoS2, WS2, Candlelight OLED
相關次數：	點閱：3 下載：0
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低色溫燭光有機發光二極體（OLED）為傳統照明技術提供了一種更具健康益處的替代方案，能顯著減少藍光暴露，避免其對生理節律的干擾、褪黑激素的抑制以及長期視網膜損害的潛在風險。本論文探討過渡金屬二硫屬化物（TMDs），特別是二硫化鉬（MoS2）和二硫化鎢（WS2），作為 OLED 空穴注入層（HIL）摻雜材料，以提升其光電特性。TMDs 憑藉其優異的載流子遷移率、可調控的光學性質和二維層狀結構，在本研究中以 0%、5%、10% 和 15% 的濃度摻入 PEDOT:PSS 基質的 HIL 中，以評估其對 OLED 效能的影響。
實驗結果顯示，摻雜 10% MoS2 的 OLED 在功率效率（PE）、電流效率（CE）及外量子效率（EQE）方面表現顯著提升，分別達到 32.7 lm/W、21 cd/A 和 13.6%，較未摻雜 TMDs 的對照組提高約 39%、21% 和 40%。相較之下，摻雜 10% WS2 的 OLED 之 PE、CE 和 EQE 分別為 30.1 lm/W、20 cd/A 和 13.1%，顯示其效能提升幅度相對較低。MoS2 摻雜 OLED 的優異表現主要歸因於增強的空穴注入能力、優化的能級排列以及更均衡的電荷傳輸，使載流子復合損耗降低，進而提升整體效率。
除了效能上的提升，本研究亦突顯 TMD 摻雜 OLED 在推動可持續發展與人因照明技術方面的潛力。開發的燭光 OLED 可提供溫暖且低強度的光照，有助於符合生理節律友好的照明標準，減少過量藍光對健康的負面影響。此外，TMD 在 OLED 結構中的應用，亦推動了符合環境、社會與治理（ESG）原則的節能照明技術發展。
未來研究可進一步優化 TMD 的合成工藝，以利大規模應用，並探討其他二維材料對 OLED 效率及器件壽命的影響。透過材料工程與器件優化策略的整合，本研究為次世代照明技術的發展提供貢獻，致力於實現兼顧人類健康與環境永續性的創新光源。

Low-color-temperature candlelight organic light-emitting diodes (OLEDs) offer a promising alternative to conventional lighting by significantly reducing blue light exposure, which has been linked to circadian rhythm disturbances, melatonin suppression, and long-term retinal damage. This thesis explores the incorporation of transition metal dichalcogenides (TMDs), specifically molybdenum disulfide (MoS2) and tungsten disulfide (WS2), into hole injection layers (HILs) to enhance OLED performance. TMDs, known for their excellent charge carrier mobility, tunable optical properties, and layered two-dimensional structure, were integrated into PEDOT:PSS-based HILs at doping concentrations of 0%, 5%, 10%, and 15%.
Experimental results demonstrate that OLEDs incorporating 10% MoS2 exhibit significant enhancements, achieving a power efficacy (PE) of 32.7 lm/W, a current efficacy (CE) of 21 cd/A, and an external quantum efficiency (EQE) of 13.6%. These values represent increases of approximately 39%, 21%, and 40%, respectively, compared to undoped devices. OLEDs with 10% WS2 achieved a PE of 30.1 lm/W, a CE of 20 cd/A, and an EQE of 13.1%, demonstrating relatively lower efficiency gains. The superior performance of MoS2-doped OLEDs is attributed to improved hole injection, optimized energy level alignment, and enhanced charge balance, resulting in reduced recombination losses and higher overall efficiency.
Beyond performance improvements, this research highlights the potential of TMD-doped OLEDs in promoting sustainable and human-friendly lighting technologies. The developed candlelight OLEDs provide a warm, low-intensity illumination that aligns with circadian-friendly lighting principles, mitigating adverse health effects associated with excessive blue light exposure. Additionally, the incorporation of TMDs into OLED architectures supports the advancement of environmentally responsible, energy-efficient lighting solutions in line with Environmental, Social, and Governance (ESG) principles.
Future investigations should focus on optimizing TMD synthesis for large-scale integration and exploring the effects of alternative 2D materials on OLED efficiency and device longevity. By leveraging material engineering and device optimization, this study contributes to the development of next-generation lighting technologies that prioritize human well-being and environmental sustainability.

Table of Contents
Chinese Abstract    ....ii-iii

English Abstract    .....iv-v

Acknowledgement    …vi-viii

Table of Contents……………………………………………………………………………....x-xv

Figure Captions    ...…xvi-xix

Table Captions.    ….…….xx

Abbreviations    ...…xxi-xxiii
Chapter 1.    Introduction and Motivation…………………………………………………..1
Chapter 2.    Fundamentals of Organic Light-Emitting Diode (OLED)
1    History and Development of OLED……………………………………………...6
2    Worldwide OLED revenue……………………………………………………...12
2.1 Display…………………………………………………………………….12
2.2 Lighting………………………………………………………………..…..13
3    Structural Composition and Operational Principles of OLEDs………………....15
3.1    OLED Manufacturing Techniques………………………………………18
3.1.1 Dry Fabrication Method…………………………………………19
3.1.2 Wet Fabrication Process…………………………………………19
3.2    OLEDs Functional Layers……………………………………………….21
3.2.1 Electrodes………………………………………………………..21
3.2.1.1 Anode………………………………………………….22
3.2.1.2 Cathode……………………………………...…………22
3.2.2 Charge Carrier Layers    …………………………….……………..22
3.2.2.1 Hole-Injection Layer (HIL)……………………………22
3.2.2.2 Hole-Transport Layer (HTL)………………….……….23
3.2.2.3 Electron-Transport Layer (ETL)………………….……23
3.2.2.4 Electron-Injection Layer (EIL)………………………...23
3.2.3 Emissive Layer (EML)…………………………………………..23
3.3    Key parameters…………………………………………………………..24
3.3.1 Turn-on Voltage (Von)…………………………………………..24
3.3.2    Operating Voltage………………………………………………..24
3.3.3 Power Efficacy (PE)………………………………..……………24
3.3.4 Current Efficacy (CE)……………………………………………25
3.3.5 External Quantum Efficiency (EQE)…………………………….25
3.3.6 Luminance………………………………………………….…….26
3.3.7 Correlated Color Temperature (CCT)…………………...….……26
3.3.8 CIE……………………………………………………………….28
3.3.9 Color rendering index (CRI)……………………….…………….29
3.3.10 Spectrum Resemblance Index (SRI)……………………………29
3.3.11 Maximum permissible exposure (MPE)………………………..31
3.3.12 Melatonin Suppression Sensitivity (MSS)………………..…….31
Chapter 3.    Literature review
1    Two-Dimensional (2D) Materials……………………………..…………………33
1.1    Overview of 2D Materials…………………………….…………….……33
1.2    Importance of 2D Materials in Optoelectronics…………………….……36
2    Transition Metal Dichalcogenides (TMDs)……………………………….……..38
2.1    General Properties of TMDs…………………………………….……….38
2.2    MoS2 and WS2 as 2D Materials…………………….……..……………..40
3    Low-Colour-Temperature and Candlelight OLEDs………………..…………….41
3.1.    Introduction to Low-Colour-Temperature Lighting………..…………….41
3.2.    Advances in Candlelight OLEDs……………………………..………….42
Chapter 4.    Characterization and Experiments
1    OLED Materials Utilized……………………………………………..………….47
1.1 Conducting Electrodes: Anode and Cathode……………………..…….…..47
1.2 Charge Injection Layers: HIL/HTL Materials……………………..….……48
1.3 Emissive Layer Materials……………………………………………..……48
1.3.1    Host Material…………………………………………..…………49
1.3.2    Emitter Materials…………………………………..……………..49
1.4 Electron Injection and Transport Layer Materials…………..……………..49
2      Material Characterization Techniques…………..……………………….……….52
2.1 Ultraviolet-Visible (UV-Vis) Spectroscopy…………….………….………52
2.1.1 Absorbance Measurements………………………………….……52
2.1.2    Transmittance Measurements…………………………….………52
2.2 Ultraviolet Photoelectron Spectroscopy (UPS)…………………….………52
2.3 Scanning Electron Microscopy (SEM)……………………………………..53
2.4 X-ray Diffraction (XRD)……………………………………….…………..53
2.5 Atomic Force Microscopy (AFM)…………………………………………54
3       Device Fabrication…………………………..…………………………………...54
3.1 Substrate Cleaning and Ultraviolet Ozone Treatment……………………..54
3.2 Hole Injection Layer (HIL) Coating…………….………………………….55
3.3 Emissive Layer (EML) Coating    ……………………………………………55
3.4 Deposition of ETL, EIL, and Cathode………….…………………………..55
4       Device Testing……………………………..…………………………….……….56
4.1 Current Density-Voltage-Luminance (J-V-L)…………………….………..56
4.2 Electroluminescence (EL) and Photometric Measurements……………….56
Chapter 5.    Result and Discussion
1       Material Synthesis…..…………………………………………………..………..57
1.1 Preparation and synthesis of MoS2 and WS2……………….......…………..57
1.2 Exfoliation of Few-Layer TMDs………………………………...…………58
2      Material Characteristics of TMD Nanosheets……...….…….…………..………..61
2.1 X-Ray Diffraction (XRD) ……………………………………....………….61
2.2 Raman Spectroscopy……………………………………………..……...…62
2.3 Scanning Electron Microscopy (SEM)……………………………..………63
2.4 Ultraviolet-Visible (UV-Vis) Spectroscopy………………………..………65
2.5 Ultraviolet Photoelectron Spectroscopy (UPS)……………..………..…….66
2.6 Atomic Force Microscopy (AFM)………………………………………….68
3    Performance Evaluation and Characterization of Solution-Processed Phosphorescent OLEDs………………………………………………………………….72
3.1 Charge Transport in Candlelight OLEDs…………………….……………73
3.2 Electroluminescent properties in Candlelight OLEDs……….…………….75
3.3 Effects on Health and the Ecosystem……………………………………....79
Chapter 6.    Conclusion………………………………………………………………………82
Reference        …………………………………………………………………………………..84
Curriculum Vitae of the Author………………………………………………………………101

                                

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