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研究生： 楊川毅
Yang, Chuan-Yi
論文名稱： 雙極性傳輸有機薄膜電晶體特性研究
Studies of ambipolar conduction in organic thin-film transistors
指導教授： 吳孟奇
Wu, Meng-Chyi
朱治偉
Chu, Chih-Wei
口試委員:
學位類別： 博士
Doctor
系所名稱： 電機資訊學院 - 電子工程研究所
Institute of Electronics Engineering
論文出版年： 2009
畢業學年度： 97
語文別： 英文
論文頁數： 125
中文關鍵詞： 雙極性 、有機薄膜電晶體 、介面修飾
外文關鍵詞： ambipolar, organic thin-film transistor, interfacial modification
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    • 在傳統互補式金氧半薄膜電晶體的應用上，雙極性傳輸是一基本且重要的特性。不過在以往關於有機半導體的研究中，有機材料通常被視為僅具備單一載子傳輸特性；而事實上，只要透過適當的介面修飾處理，原本被視為僅具單一載子傳輸特性的電晶體元件，亦可呈現雙極性載子傳輸特性。本論文的主旨即在探討如何透過修飾兩個重要介面：其一為在介電層與通道層間，其二為在通道層與源/汲極電極間，進而達到理想匹配的雙極性載子傳輸特性。首先在第一個介面的處理上，一般常用來作為閘極介電層的二氧化矽上本質存在有矽醇基團，而這些矽醇基已被證實與阻礙N型載子即電子的堆積有很大的關係，因此我們利用高分子材料(如聚甲基丙烯酸甲酯等)來修飾其表面，減少介面上會捕捉電子的缺陷密度，進而幫助N型傳導的產生。而在另一個介面上，在半導體層與源/汲極電極間插入一超薄奈米級介面修飾層(如氟化鋰、碳酸銫等)，若將此層厚度控制在極薄之一奈米以下，則此修飾層的存在除可幫助電子的注入外，對於原本P型載子即電洞的傳輸亦不致有太大的抑制。本論文中除探討雙極性載子傳輸特性之外，對於影響單一載子傳輸的因素如有機材料本質、分子排列、介電層選擇、與元件結構等亦在第二章中探討。此外，在第五章中也討論雙層雙極性傳輸結構，並比較其與單層雙極性傳輸結構的優劣。在本研究中，無須繁雜的多道製程與步驟，藉由單一主動層與兩個重要介面修飾即可實現平衡匹配的雙極性傳輸特性，大幅簡化製作的難度與提升雙極性傳輸元件的實用性與未來性。

    Ambipolar conduction is an essential and fundamental property in the application of the conventional inorganic complementary metal-oxide-semiconductor thin film transistors. Though in the past, the researchers usually regarded organic semiconductors as the materials that can only be capable of transport unipolar carrier. In fact, ambipolar conduction can be achieved through a proper interfacial modification in organic field-effect transistors. The main topic of this thesis is how to achieve a balanced and matched ambipolar conduction through two important interfacial modification: one is between the gate dielectric and organic semiconductor, the other is between the organic semiconductor and metal electrodes. As for the first interfacial treatment, there exists the silanol groups on the surface of the gate dielectric silicon dioxide layer, and the deep correlation between the presence of the silanol groups and the limit of the electron accumulation has been proved. Therefore, we introduce a polymer (e.g. polymethylmethacrylate) as the interfacial modified layer to lower the density of the electron traps, and facilitate the formation of N-channel conduction. As for the second interface, inserting an ultrathin nano-scaled interlayer (e.g. LiF, Cs2CO3) between organic semiconductor and metal electrode can further enhance the ambipolar conduction. If we control the thickness of this interfacial interlayer no more than 1 nm, and the presence of the ultrathin nano-scaled interlayer could not only facilitate the electron injection but it wouldn’t limit the p-channel conduction. Therefore controlling the thickness of the interlayer within a certain limit can achieve a balanced and matched ambipolar conduction. In addition to ambipolar characteristic, chapter 2 would discuss the factors that influence the unipolar conduction such as the intrinsic property of organic semiconductors, the ordering and alignment of organic molecules, the choices of high-κ dielectric, and the architecture of device structure. Besides, chapter 5 would investigate the bi-layer amipolar field-effect transistors, and compare the pros and cons with those of the single-component counterpart. In this studies, without complicated and multiple fabrication processes, balanced and matched ambipolar characteristic can be easily achieved merely through single active layer and two interfacial modifications. Utilizing this technique to fabricate the ambipolar transistors can immensely simplify the difficulties of fabrication and make the practical applications of ambipolar field-effect transistors more feasible and promising.

    Contents Abstract (in Chinese and English) I Contents IV List of Figures VI List of Tables X Chapter 1 Introduction 1 1.1 History and development of organic field-effect transistors 1 1.2 Theoretical analysis 6 1.3 Overview of this thesis 11 Chapter 2 Unipolar Organic Field-Effect Transistors: Materials, Dielectrics, and Architecture 12 2.1 Unipolar organic field-effect transistors 12 2.1.1 Self-assembled monolayer 12 2.1.2 Pentacene 16 2.1.3 Poly(3-hexylthiophene) 18 2.2 Correlation between structural ordering and transport property 20 2.2.1 Introduction 20 2.2.2 Experimental Details 21 2.2.3 Results and Discussion 22 2.2.4 Summary 30 2.3 High κ hybrid dielectric 31 2.3.1 Introduction 31 2.3.2 Experimental Details 33 2.3.3 Results and Discussion 34 2.3.4 Summary 40 2.4 Study of organic vertical triodes 41 2.4.1 Vertical organic triodes with a high current gain operated in saturation region 41 2.4.1-1 Introduction 42 2.4.1-2 Experimental Details 43 2.4.1-3 Results and Discussion 44 2.4.1-4 Summary 49 2.4.2 Pentacene-based planar- and vertical-type organic thin-film transistors 50 2.4.2-1 Introduction 51 2.4.2-2 Experimental Details 52 2.4.2-3 Results and Discussion 54 2.4.2-4 Summary 60 Chapter 3 Ambipolar Organic Field-Effect Transistors: Dielectric Modification Layer (Interface I) 62 3.1 Ambipolar characteristics of organic field-effect transistors 62 3.2 Correlation between hydroxyl group and electron traps 63 3.3 PMMA dielectric modified layer 64 3.3.1 Introduction 65 3.3.2 Experimental Details 67 3.3.3 Results and Discussion 68 3.3.4 Summary 78 Chapter 4 Ambipolar Organic Field-Effect Tansistors: Ultrathin Nano-scale Interlayer (Interface II) 80 4.1 Ultra-thin nanoscale interlayers 80 4.2 Lithium fluoride (LiF) interlayer 80 4.2.1 Introduction 81 4.2.2 Experimental Details 82 4.2.3 Results and Discussion 83 4.2.4 Summary 89 4.3 Cesium carbonate (Cs2CO3) interlayer 90 4.3.1 Introduction 90 4.3.2 Experimental Details 92 4.3.3 Results and Discussion 93 4.3.4 Summary 101 Chapter 5 Ambipolar Organic Field-Effect Transistors: Bi-layer Structure 102 5.1 C60-based organic field-effect transistors 102 5.1.1 Thickness of C60 103 5.1.2 Choice of solvents 105 5.1.3 Annealing temperature 106 5.1.4 Measure environment 108 5.2 C60 and pentacene bi-layer ambipolar organic field-effect transistors 109 Chapter 6 Conclusions and Future Work 115 References 116 Publication List 124

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