傳統共軛高分子用於高分子發光二極體(PLED)，因為適合大面積和成本製作而被廣泛地研究。然而，此類型的高分子作為主體通常存在三重態能量(ET)低於客體的問題，使得ET從高放光效率的客體反向傳遞到低放光效率的主體而導致低發光效率，從而限制其在全彩顯示器或照明應用的發展。相較下，σ-π共軛高分子是個很好的結構可以做為同時滿足高ET和適當載子遷移率的主體材料。為此，本論文對σ-π共軛高分子主體的合成和光電特性進行系統性的研究。
在以下章節中，第一章將提供有機發光二極體(OLEDs)的概述，包括基本工作原理、半導體介面理論、主客體系統的放光機制以及熱活化延遲螢光(TADF)等。然後，第二章將對目前高效率的O/PLEDs進行全面性的介紹並給予本論文的研究動機。第三章記錄基本量測及鑑定、元件製作和合成細節等實驗方法。
在第四章中，我們研究了σ-π共軛高分子主體材料的光物理特性，發現矽σ-π共軛高分子主體側鏈上的電洞傳輸基團(TPA)和/或電子傳輸基團(OXD)會形成激發複體。而且，從磷光光譜可同時發現獨立基團(TPA和/或OXD)、激發複體、矽σ-π共軛高分子主鏈的放光，稱之為多重三重態。此多重三重態的形成提供了三重態激子能量轉移到磷光客體的額外途徑。
在第五章中，我們證實了引入鍺(Ge)重原子到σ-π共軛高分子中可以得到高ET (2.86 eV)的高分子主體P(DMAC-Ge)，其不僅可以讓主體得以有效將能量轉移給藍光客體，而且可以降低極化率而讓產生的光色更藍移以及增強自旋軌道耦合以促進客體的反向系統間跨越（RISC）速率而捕捉更多的三重態激子用於發光。當元件使用P(DMAC-Ge)作為主體並混摻天藍光TADF客體，其達到創紀錄的最大外部量子效率(EQE) 24.1%，且在亮度500 cd/m2下的EQE仍有22.8%。因此，目前的研究開拓了一種新的高分子主體的結構設計，並得以作為其它光色TADF客體材料的主體。
第六章延伸了第五章的研究工作，我們設計一系列中心原子(X)由C、Si、Ge 和Sn組成並以雙聯苯-X作為重複單元的σ-π共軛高分子，藉此了解σ-π共軛高分子主鏈的基本特性。我們發現當不同IVA族原子作為中心原子時，其不同σ-π共軛高分子之間明顯存在光學與電性的差異，此影響也反映在其電激發光的表現上。此研究工作在高分子主體的主鏈設計上提供了有用的方針。
在第七章中，我們使用P(DMAC-Ge)分別作為天藍磷光以及藍/綠/紅/白TADF PLEDs的主體。其優化的元件效率對於天藍磷光以及藍/綠/紅/白TADF元件分別達到創紀錄的外部量子效率19.7%、22.3%、20.8% 和4.9%，且放光峰分別為。當進步一摻雜入DMAC-TRZ / Ir-O / Ir-R至發光層中可得到T-P混摻的白光PLED，其色度座標為(0.34, 0.40)並達到創紀錄的EQE 17.2%。此研究工作為首度使用單一種主體材料達到高效率全彩PLEDs的應用。
在第八章中，我們提出四種電子予體型高分子主體，目的在於了解不同電子予體型的主體材料在主/客體系統中對於藍/綠/紅TADF客體的影響。研究中，我們觀察到來自予體-受體 (D-A)相互作用所形成的單重態和三重態的主/客激發複體。然後，我們對主/客激發複體對於光致發光(PL)和電致發光(EL)性質的影響進行一系列的探討，並從中找出最好的高分子主體結構以實現高效能全彩TADF元件的應用。此外，TADF客體得PL效率由於受到主/客激發複體的影響，最終也反映在它們元件的量子效率上。我們相信這類D-A的相互作用同樣也會發生在小分子主/客體混摻的系統中以及非摻雜的TADF發光體系統中。
 

Conventional conjugated polymers for use as polymer light-emitting diodes (PLEDs) have been studied extensively due to their capability for large-area and low-cost fabrication. However, this type of PLED usually suffers from the issue of the host with lower triplet energy (ET) than the guest materials. It leads to a low emitting efficiency through back transfer of ET from the guest to the polymer hosts in their corresponding devices and thereby limits the development for full-color display or lighting application. In comparison, the σ-π conjugated polymer is a promising candidate structure for developing into the host that can satisfy the requirement of high ET as well as adequate carrier mobility. For this purpose, in this thesis, the investigations for σ-π conjugated polymer hosts are carried out, including their synthesis and optoelectronic properties.
In the following chapters, an overview of OLEDs is given in Chapter 1, including the basic working principle, fundamental theory on semiconductor junctions, emission mechanism in host-guest system, and principle of thermally activated delayed fluorescence (TADF) OLEDs etc. Then, a comprehensive summary of the state-of-the-art O/PLEDs and the thesis motivation are given in Chapter 2. The experimental methods are presented in Chapter 3, which includes the general measurements and characterization, device fabrication and details of synthetic methods.
In Chapter 4, the photophysical properties of σ‒π polymer host materials are investigated. The bipolar and unipolar side arm on Si-based σ-π conjugated polymer hosts can form the excited-state complexes between their hole transport moiety (triphenylamine, TPA) and/or electron transport moiety (oxadiazole, OXD) side arms. Moreover, the triplet states of the isolated moiety (TPA or/and OXD), excited-state complex and σ-π polymer backbone can exist simultaneously, called multiple triplet states. The formation of multiple triplet states provides an additional route for transferring triplet exciton energy to phosphor dopant.
Chapter 5 demonstrates that the heavy-atom germanium (Ge) in σ-π conjugated polymer host, poly(acridan grafted biphenyl germanium), P(DMAC-Ge), provides high ET level (2.86 eV) to give efficient energy transfer from host to blue guest, low orientation polarizability leading to bluer emission from the guest, and the enhancement of spin-orbit coupling to promote the reversed intersystem crossing (RISC) rate of guest and thus harvesting more triplet excitons for light emission. The sky-blue TADF electroluminescence using this host/guest pair gives the record-high external quantum efficiency (EQE) 24.1% at maximum and 22.8% at 500 cd/m2. Thus, the present study opens up a new promising design route of polymer host for various TADF guests for highly efficient TADF PLED.
Chapters 6 extends the work of Chapter 5, a series of σ‒π polymers grafted biphenyl side chain, composed of biphenyl-X as the repeat unit, where X= C, Si, Ge and Sn with the radii 70, 110, 125 and 145 pm, respectively, are proposed for further exploring differences of the σ‒π polymer backbones with various group IVA central atoms. The most crucial point in this study is that the ET levels and charge transport properties of σ‒π polymers are highly affected by their central atoms, which result in significant differences in electroluminescence properties. Such findings in this work provide useful guidelines on the construction and selection of backbones for designing polymer hosts.
Chapter 7 employs the polymer host P(DMAC-Ge) in sky-blue phosphorescence and blue/green/red/white TADF PLEDs, respectively. The optimized devices using P(DMAC-Ge) as host along with the cohost DCzPPy in the EML and doping with sky-blue Ph- and B/G/R TADF- guests, respectively, achieve record-high maximum EQEs of 19.7%, 22.3%, 20.8% and 4.9% with emission peaks at 470, 485, 508 and 630 nm, respectively. Upon further dopping the three-color dopants (DMAC-TRZ/Ir-O/Ir-R) into the emitting layer, the T-P hybrid white PLED shows the record-high EQE 17.2% with CIE (0.34, 0.40). This is the first report using the single cohost to achieve the full-color TADF PLEDs with high device performance.
In Chapter 8, four donor type D-polymer hosts comprising Si-/Ge- based biphenyl unit polymer backbones and various donor side arms are proposed, which aims at understanding the effect of hosts on the optoelectronic properties of the blue/green/red (B/G/R) TADF emitters in host/TADF-guest system. The singlet and triplet host/guest exciplexes from the donor-acceptor interactions between the polymer hosts and TADF emitters are observed. Importantly, this work provides a serial comparison to the influence of the host/guest exciplex on PL and EL properties, and finds out the promising structure of polymer host to realize highly efficient full-color TADF device applications. Furthermore, the PL efficiencies of the TADF emitters influenced by host/guest exciplexes also reflect on their external quantum efficiencies (EQEs). Such D-A interactions should also occur in small-molecule host/guest system as well as non-doped TADF emitter system.

CHAPTER 1: INTRODUCTION 1
1-1 Preface 1
1-2 Application and current development of OLEDs 2
1-3 Evolution of organic electroluminescence devices 5
1-4 Metal-semiconductor junctions 6
1-4.1 Metal-metal junction 6
1-4.2 Schottky junctions 7
1-4.3 Ohmic junction 11
1-5 Basic working principle of OLED 12
1-6 Fluorescent, phosphorescent and TADF OLEDs 14
1-7 Emission mechanisms in host-dopant system 16
1-8 Developments and Fundamental principles of TADF OLEDs 19
1-8.1 Development of TADF OLEDs 19
1-8.2 TADF mechanism and working principle 20
1-8.3 Requirements for an ideal TADF emitter design 23
1-8.4 Key parameters for TADF electroluminescence 24
1-9 Electronic spin-orbit coupling 24
1-10 References 26
CHAPTER 2: Literature Review and Thesis Motivation 28
2-1 State-of-the-art R/G/B OLEDs by Dry Process 28
2-2 State-of-the-art R/G/B OLEDs by Solution Process 29
2-3 State-of-the-art White TADF OLEDs by Dry Process 31
2-4 State-of-the-art White TADF OLEDs by Solution Process 33
2-5 State-of-the-art R/G/B and White Phosphorescent OLEDs by Dry and Solution Processes 34
2-6 Literature Analysis 36
2-7 Thesis Motivation 37
2-8 References 38
CHAPTER 3: EXPERIMENTAL METHODS 43
3-1 Synthetic Methods 43
3-2 General Measurements and characterization 61
3-2.1 Physical characterization 61
3-2.2 Optical characterization 62
3-2.3 Electrochemical characterization 63
3-2.4 Theoretical Methodology 64
3-2.5 Device fabrication 64
3-3 Materials for Device Fabrications 65
3-3.1 Anode and Hole Injection Materials 65
3-3.2 Transport Layer Materials 65
3-3.3 Phosphorescent and TADF emitters 66
3-4 References 66
CHAPTER 4: Influence of Multiple Triplet States in Bipolar and Unipolar Diphenylsilane σ-π Conjugated Polymer on Electro –phosphorescence 67
4-1 Introduction 67
4-2 Redults and Discussion 70
4-2.1 Si-based σ-π polymer hosts 70
4-2.2 Thermal, electrochemical and photophysical properties of σ-π polymer host 71
4-2.3 Multiple triplet state in σ-π polymer host 78
4-2.4 Influence of excited-state complex of polymer host on device performance 83
4-3 Conclusion 85
4-4 References 85
CHAPTER 5: Acridan Grafted Poly(biphenyl germanium) with High Triplet Energy, Low Polarizability and External Heavy-Atom Effect for Highly Efficient Sky-Blue TADF Electroluminescence 89
5-1 Introduction 89
5-2 Results and Discussion 91
5-2.1 Synthesis and Physical Characterization of σ-π Conjugated Polymers 91
5-2.2 Orientation Polarizability Effect of Host on Emission Color of TADF Guest 96
5-2.3 External Heavy-Atom Effect on TADF Guest 102
5-2.4 Device Performance for Host with σ-π Conjugated or Non-Conjugated Backbone 106
5-3 Conclusion 115
5-4 References 115
CHAPTER 6: Optoelectronic Properties of High Triplet σ‒π Conjugated Poly[(biphenyl group-IVA-atom (C, Si, Ge, Sn)] Backbones 120
6-1 Introduction 120
6-2 Results and Discussion 122
6-2.1 Design Strategy for High ET σ‒π Polymer 122
6-2.2 Theoretical Calculations and Photophysical Characteristics 126
6-2.3 Electrochemical, Triplet Energy and Charge Transport Properties 129
6-2.4 Sky-Blue Ph- and TADF- PLEDs with P(dBPh-X)s as Host 137
6-3 Conclusion 140
CHAPTER 7: Poly(Acridan Grafted Biphenyl Germanium) as a Universal Host for High-Efficiency Full-Color Thermally Activated Delayed Fluorescence Electroluminescence Devices 147
7-1 Introduction 147
7-2 Results and Discussion 150
7-2.1 Significance of Ge-Polymer Backbone Effect on Electron Transport and Device Performance 150
7-2.2 Optical Characteristics and Electroluminescence Dynamics for the Polymer Host P(DMAC-Ge) 155
7-2.3 High Performance Sky-Blue Phosphorescence and B/G/R TADF PLEDs 159
7-2.4 TADF/Phosphor (T-P) Hybrid TADF White PLEDs 163
7-3 Conclusion 167
7-4 References 168
CHAPTER 8: Exploration of Donor-Acceptor Interactions in Donor-Grafted Polymer Host/TADF-Guest System for Highly Efficient Photoluminescence and Electroluminescence 175
8-1 Introduction 175
8-2 Results and Discussion 177
8-2.1 Possible Emitting Species in Host/TADF-Guest System 177
8-2.1.1 Thermal, optical and electrochemical properties 179
8-2.2 Exciplexes (Dg/Ag)* from Intermolecular D/A Interaction 183
8-2.3 Donor-Acceptor Interaction in Simulated Donor/Acceptor System 185
8-2.4 Exciplexes (Dh/Ag)* from Host-Guest Interaction 189
8-2.5 Influence of the Exciplexes 3(Dh/Ag)* on B/G/R TADF Emissions 199
8-2.5.1 Influence of the Exciplexes 3(Dh/Ag)* on B/G/R TADF Emissions 202
8-2.6 Mechanism of D-polymer Host-TADF Guest Interaction 203
8-2.7 Influence of (Dh/Ag)* on Device Characterization 204
8-2.7.1 Side Chain Effects of D-polymer Hosts on EL Spectral Stability 207
8-3 Conclusion 210
8-4 References 211

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(25) Tang, X.; Liu, X.-Y.; Jiang, Z.-Q.; Liao, L.-S., High-Quality White Organic Light-Emitting Diodes Composed of Binary Emitters with Color Rendering Index Exceeding 80 by Utilizing Color Remedy Strategy. Adv. Funct. Mater. 2019, 29, 1807541.
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