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研究生：	林博仁 Lin, Bo-Ren
論文名稱：	高分子半導體/絕緣體混摻之薄膜電晶體研究及其應用 The study of polymeric semiconductor/insulator blend thin-film transistors and their applications
指導教授：	鄭弘隆 Cheng, Horng-Long
共同指導:	王右武 Wang, Yu-Wu
學位類別：	博士 Doctor
系所名稱：	理學院 - 光電科學與工程學系 Department of Photonics
論文出版年：	2020
畢業學年度：	109
語文別：	英文
論文頁數：	156
中文關鍵詞：	有機薄膜晶體、電特性和穩定性、結構和形態、雙閘極有機薄膜電晶體、閾值電壓、邏輯閘、拉曼製圖、聚合物混摻、相分離、異質結主動層、光感電晶體、光敏性
外文關鍵詞：	Organic thin film transistor (OTFT), electrical characteristics and stability, structure and morphology, dual-gate OTFT, threshold voltage, logic gate, Raman mapping, polymer blend, phase-separated, heterojunction, phototransistor, photosensitivity
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本文主要研究有機薄膜晶體(OTFT)的電性能及其相關應用。研究了將絕緣聚合物材料導入有機半導體主動層的相關效果。研究中使用的混摻主動層是由基於半導體材料poly (3-hexylthiophene) (P3HT)與絕緣材料poly (methyl methacrylate) (PMMA)所組成。本文共分為五章。第一章簡要介紹了基於有機/聚合物半導體的OTFT。在第二章中，我們研究了在各種條件下製備的基於P3HT:PMMA混摻OTFT的電特性。在第三章中，我們使用具有偽雙層結構的基於P3HT:PMMA混摻主動層在不同氣氛下對OTFT進行了電穩定性研究。在第四章中，研究了基於P3HT:PMMA混摻雙閘極OTFT的電特性，並展示了其在多功能應用中的巨大潛力。在第五章中，我們討論了基於雙層異質結主動層的光感電晶體，該主動層的製作是通過N,N′-ditridecylperylene-3,4,9,10-tetracarboxylic diimide, PTCDI-C13H27沉積P3HT:PMMA混摻主動層上。最後對論文進行了總結。

在第二章中，我們研究了基於P3HT:PMMA混摻主動層的製備條件對相應OTFT的電特性的影響。通過溶液製程，使用幾種不同的溶劑，製備了具有各種組成的P3HT:PMMA二元混摻主動層，以獲得具有多種相分離形態的微結構。討論了主動層的微結構性質與相應的OTFT的電性之間的相關性。與純P3HT OTFT相比，P3HT:PMMA混摻OTFT的電性能有所提高。OTFT的性能與P3HT:PMMA混摻主動層的相分離的微觀結構特性密切相關。

在第三章中，我們探討了基於P3HT:PMMA混摻OTFT在各種環境中的操作穩定性。純P3HT元件通常表現出顯著的非理想，不穩定和快速衰減的電氣特性，尤其是在潮濕的空氣環境中，這阻礙了它們的實際應用。在本節研究中，即使是在環境空氣中，基於P3HT元件之動態操作穩定性也可通過製備具有嵌入式源電極和漏電極的半導體/絕緣體多摻混物的偽雙層結構來實現。此偽雙層主動層由PMMA緩衝層與P3HT:PMMA混摻主動層所結合。具有偽雙層主動層的P3HT:PMMA混摻元件在環境空氣中的動態連續操作下也可以抵抗閘極偏壓而具有很強的耐受性，因此顯示出出乎意料的非衰減電流特性。

在第四章中，提出了具有不對稱頂部和底部電荷調製層(CML)的設計來改進P3HT:PMMA雙閘極混摻OTFT的電特性，從而證明了OTFT具有增強的功能，即大電流增強行為，高效的閾值電壓可控性和獨立的雙重邏輯門功能。此CML透過多層堆疊自動生成的，其包含了P3HT:PMMA混摻主動層、poly(vinylidene fluoride) (PVDF)緩衝層和cross-linkedpoly(4-vinylphenol) (cPVP)絕緣層。由於非對稱的CML存在，P3HT:PMMA雙閘極混摻元件具有空前的電特性，例如頂部閘極電位容易影響底部通道層。然而，僅當施加底閘極電壓(正或負)時，頂部通道層才能正常運作。根據此不尋常的電特性，可使用一雙閘極電晶體即可實現基本雙重邏輯閘功能。

在第五章中，我們使用P3HT:PMMA/PTCDI-C13異質結主動雙層製作光感TFT，並研究其電和光響應特性。將PTCDI-C13沉積到具有各種相分離形態的P3HT:PMMA混摻主動層上，以在界面上形成具有不同分子構型的各種異質界面。與純P3HT層和P3HT/PTCDI-C13雙層作為主動層的光感TFT相比，基於P3HT:PMMA/PTCDI-C13元件的光敏性顯著提高。在微觀水平上討論了所製備的具有特定異質結的光感TFT增強光響應的可能起源。

This thesis focused on the electrical properties of organic thin-film transistors (OTFTs) and their related applications. The related effects of introducing insulating polymer materials into the organic semiconducting active layer were investigated. The active layers used in this study were based on the polyblends of semiconducting regioregular poly(3-hexylthiophene) (P3HT, a p-channel material) with insulating poly(methyl methacrylate) (PMMA). This thesis is divided into five chapters. Chapter 1 gives a brief introduction of organic/polymeric semiconductor-based OTFTs. In Chapter 2, we studied the electrical characteristics of OTFTs based on P3HT:PMMA blends prepared under various conditions. In Chapter 3, we performed an electrical stability study of OTFTs at various atmospheres using a P3HT:PMMA blend-based pseudo-bilayer. In Chapter 4, the electrical characteristics of P3HT:PMMA blend-based dual-gate OTFTs were studied, and showed their great potential for multifunction applications. In Chapter 5, we discussed phototransistors based on bilayer heterojunction active layers prepared by the deposition of a thin N,N′-ditridecylperylene-3,4,9,10-tetracarboxylic diimide (PTCDI-C13H27, an electron acceptor) layer upon the P3HT:PMMA blend-based bottom layer. The last chapter presented a summary of the thesis.

In Chapter 2, we investigated the effects of preparation conditions of P3HT:PMMA blend-based active layer on the electrical characteristics of the corresponding OTFTs. The P3HT:PMMA binary blend-based active layers with various compositions were prepared by spin-coating process using several different solvents to obtain microstructures with diversified phase-separation morphology. Correlation between the microstructural properties of the active layers and the electrical properties of the corresponding OTFTs were discussed. Compared with neat P3HT-based OTFTs, the electrical performances of P3HT:PMMA polyblend-based OTFTs were improved. The OTFT’s performances were strongly related to the phase-separated microstructural properties of the P3HT:PMMA blend active layers.

In Chapter 3, we explored the operational stability of the P3HT:PMMA blend-based OTFTs in various environments. Neat P3HT-based OTFTs often exhibit significant non-ideal, unstable, and fast-decaying electrical characteristics, especially in a moisture-containing ambient air environment, which hindered their practical applications. The dynamic operational stability of P3HT-based OTFTs even in ambient air can be achieved through the preparation of a P3HT:PMMA blend-based pseudo-bilayer configuration with embedded source and drain electrodes. The pseudo-bilayer active layer consisted of a PMMA bottom layer and a P3HT:PMMA blend top layer. The OTFTs with the pseudo-bilayer active layer have strong endurance against gate-bias stress even under dynamic continuous operation conditions in ambient air, thereby showing unexpected non-decaying current features.

In Chapter 4, the improved electrical characteristics of P3HT:PMMA blend-based dual-gate (DG) OTFTs with asymmetric top and bottom charge modulation layers (CMLs) design were presented, thus demonstrating OTFTs with enhanced functionality, i.e., large current enhancement behavior, highly efficient threshold voltage controllability, and self-contained dual-mode logic gate features. The asymmetric CMLs are automatically generated through the preparation of stacks of the P3HT:PMMA blend layer, poly(vinylidene fluoride) (PVDF) buffer layer, and cross-linked poly(4-vinylphenol) (cPVP) insulator layer. Owing to the presence of asymmetric CMLs, the P3HT:PMMA blend-based DG-OTFTs exhibited unprecedented electrical characteristics, such as the easy depletion of the bottom channel by the top gate potential. However, the top channel can work properly only when given a bottom gate potential (either positive or negative). Given these unusual electrical features, the design of the fundamental dual-mode logic gates can be achieved with only one DG transistor.

In Chapter 5, we investigated the electrical and photoresponse properties of OTFTs using P3HT:PMMA blend/PTCDI-C13 heterojunction active bilayer. A PTCDI-C13 top layer was thermally deposited onto the P3HT:PMMA blend bottom layers with various phase-separated morphologies to form varied heterogeneous interfaces with different molecular configurations on the interface. Compared with OTFTs that use the neat P3HT layer and P3HT/PTCDI-C13 bilayer as the active layer, the photosensitivity of P3HT:PMMA/PTCDI-C13-based OTFTs was significantly enhanced. The possible origins of the enhanced photoresponse of the as-prepared OTFTs with specific heterojunction were discussed at the microscopic level.

中文摘要	I
Abstract	IV
誌謝	VII
Contents	IX
Table contents	XIII
Figure contents	XIV
Chapter 1	1
1 Introduction	1
1.1 Brief overview of organic/polymer semiconductor transistors	1
1.2 Overview of p-type organic/polymer blend film transistors	2
2 Principles of OTFT operation and parameters of Characteristics	6
2.1 Typical OTFTs	6
2.2 Operating principle of OTFTs	6
2.3 Operating principle of dual-gate OTFTs	9
2.4 Operating principle of organic/polymer phototransistors	10
3 Charge transport mechanism in organic/polymer semiconductors	10
3.1 Variable range hopping (VRH)	11
3.2 Multiple trapping and release model (MTR)	12
4 Charge photogeneration	13
5 Research motivation and organization of thesis	14
Reference	18
Chapter 2 Characteristics of P3HT:PMMA polyblend-based thin-film transistors	31
1 Introduction	31
2 Experimental section	32
2.1 Device preparation	32
2.2 Characterization	33
3 Results and discussion	33
3.1 Electrical properties of P3HT:PMMA OTFTs	33
3.2 Morphological analysis of the polyblend-based ALs	34
3.3 Absorption and Raman spectroscopy analysis of the polyblend-based ALs   35
3.4 P3HT:PMMA polyblend-based ALs using different kinds of solvent systems   38
4 Conclusion	40
Reference	42
Chapter 3 Electrical stability study of polymer-based organic transistors in ambient air using active semiconducting:insulating polyblend-based pseudo-bilayer	53
1 Introduction	53
2 Experimental section	56
2.1. Device preparation	56
2.2. Characterization	56
2.3. Quantum chemical calculations	57
3 Results and discussion	57
3.1. Microstructural properties of the polyblend active layers	57
3.2. Electrical characteristics of OTFTs	59
3.3. Dynamic real-time stability in continuous operation mode	61
3.4. Microstructural properties of polyblend-based AL in relation to gas response properties of OTFTs	63
3.5. Molecular perspective on moisture effects of OTFTs	65
4 Conclusion	69
References	71
Chapter 4 Enhanced-functionality of dual-gate organic transistors based on semiconducting:insulating polyblend-induced asymmetric charge modulation layers	86
1 Introduction	86
2 Experimental section	89
2.1 Sample preparation	89
2.2 Characterization	90
3 Results and discussion	91
3.1 Electrical characteristics of dual-gate transistors	91
3.2 Raman mapping and absorption spectroscopy	96
3.3 Working mechanisms of DG-OTFTs with atb-CMLs	99
3.4 Prediction of Possible Logic Gate Operations	102
4 Conclusion	104
References	106
Chapter 5 Enhanced-photosensitivity of phototransistor based on the morphology engineering in heterojunction organic/polymer active layer	125
1 Introduction	125
2 Experimental section	127
2.1. Materials and device preparation	127
2.2. Characterization	129
2.3. Quantum chemical calculations	129
3 Results and discussion	129
3.1 Microstructural properties and corresponding to photosensitivity of phototransistors	130
3.2 Energy level diagram and basic optical properties of organic/polymer semiconductor ALs with special heterogeneous interface structure.	133
3.3 Working mechanism of photosensitivity for phototransistors based on ALs with special heterogeneous interface structure.	135
3.4 Low-voltage phototransistors based on ALs with special heterogeneous interface structure.	136
4 Conclusion	137
References	139
Chapter 6 Summary	151
Appendix	153
List of publications	155


                                    

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