臺灣博碩士論文加值系統

薄膜電晶體近年來受到廣泛的研究，因其有低成本、低溫製成及可撓曲的優點，並且可以利用溶液製程來製作。但其相對於非晶矽的薄膜電晶體來說，載子遷移率(carrier mobility)比較小以及臨界電壓(threshold voltage)偏大都是等待改善之目標。本論文實驗透過絕緣／半導溶液材料製作、結構設計及低溫噴墨製程，以改善有機薄膜電晶體的電性與達到低成本製程的期許。
本論文中第一部分利用可感光之溶液式高介電有機絕緣層搭配雙閘極結構增進電晶體特性。研究中將有機絕緣層高分子材料聚乙烯醇(PVA)與感光劑(ADC)最佳混合比例，製作出漏電流密度較低之有機絕緣層；而雙閘極(DG)電晶體元件有第二個載子通道以彌補電性上的損失。DG元件等效載子遷移率1.06 cm2/ Vs，開關電流比為1.6×103之有機薄膜雙閘極電晶體元件。最後以此元件來製作反相器電路，雙閘極元件為其驅動元件(Driver)。經由電性分析，我們發現電晶體的臨界電壓會隨著上閘極電壓的不同而有所改變，而這影響著我們反相器輸出入轉換曲線，使我們可以找出適合數位電路應用的情形。
接著我們分散高介電奈米粒子於高分子聚亞醯胺溶液(polyimide)之中，利用分散劑的選擇與份量得到穩定的複合奈米絕緣溶液。透過2 vol%的奈米添加仍保有懸浮穩定性，介電常數(k)可以提高(ｋ~5)，但其漏電流將會偏高。因此改用可交聯提高本質介電特性的聚乙烯苯酚cross-linked poly(4-vinylphenol) (PVP)做為母體摻雜TiO2之奈米粉體，以期提高絕緣層介電常數，進而改善有機薄膜電晶體之特性。為了把TiO2奈米粉體分散得夠小且均勻，我們利用高速珠磨(Pearl mill)分散技術來達到此需求，並對其研磨分散條件做探討。為了充分了解使用噴印技術製備有機薄膜電晶體的奈米複合絕緣層，對噴印製程條件之驅動電壓大小、操作頻率以及壓電波形對噴墨情況最佳化，成功地噴印出奈米複合絕緣層，達到直接圖案化的目的，可免除傳統之黃光製程。更與傳統旋塗而成的絕緣薄膜做一比較，以向心力方式說明成膜機制影響粒子分佈與表面粗糙度。
進一步研究在噴印之奈米複合絕緣層上，蒸鍍Pentacene來製作有機薄膜電晶體。藉由摻雜TiO2的奈米複合絕緣層，成功將載子遷移率提升到0.58 cm2/ Vs，並把臨界電壓降低到-5.4 V。以XRD、SEM及Raman光譜來探討Pentacene沉積在這些不同之絕緣層上的傳輸行為。
主動層材料方面，考慮有機主動層本身載子移動率不易提升，為改善有機電晶體的電性，我們製作無機氧化鋅ZnO奈米粒子懸浮液作為噴印所需墨水，其優勢是粒子合成與分散過程是連續不分開，減少聚集與物理研磨必要。粒子呈微結晶態，將可以減少沉積退火溫度至200 oC。利用噴印技術噴印氧化鋅奈米溶液製作電晶體主動層，結合喷印純PVP透明絕緣層，觀察薄膜透光度與元件電性，也得到移動率和驅動電壓分別為0.69 cm2/Vs與25.5 V，我們並建立了一模型推測薄膜表面缺陷成因來自胺類分散劑揮發過快，墨滴蒸發過程中粒子聚集速度大於均勻沉積速度。透過穿透率量測，元件可見光譜範圍透光度仍有65 ％以上。
更進一步我們嘗試全噴印薄膜電晶體，並採用透明奈米碳管作為三個電極；配製不同莫耳比例的氧化銦鋅錫(IZTO)溶液，找到180 oC低溫退火後電性表現良好的參數。最後我們製作一薄膜電晶體，過程全程使用噴墨印刷技術，初步得到多層薄膜之透光度仍可達80%以上，顯示金屬氧化物半導體薄膜在溶液製程仍有發展的優勢。該噴印電晶體的線性場效移動率約0.194 cm2/Vs，驅動電壓為-5 V,呈現噴墨印刷全程製作電子元件的優勢。
透過結構設計與材料製作改善電晶體特性，接著以噴墨印刷製程與低溫金屬氧化物墨水製作低成本薄膜電晶體，未來將可應用更廣的領域。

Recently, Thin Film Transistors (TFTs) have been studied widely because of potential applications in low cost, low-temperature process and flexible displays. They can be fabricated by easy processes based on solution methods. But the mobility of organic TFTs is lower and the threshold voltage is higher than amorphous Si TFTs.
In our study, first of all, in order to obtain a high performance Organic TFT, we attempt to discover the best blending proportion of the photosensitive agent ADC to PVA for fabricating organic polymer dielectrics of low leakage current. Then we use this organic insulating layer as the transistor gate insulator layer of double gate thin film transistor devices. The active layer formed the second channel by the second gate would improve the device performance. Finally, we use this device to create inverter circuit. It is found that the threshold voltage have to change as the top gate voltage. That affects our input-output conversion curve of inverters.
Second, we prepare the high-k nanocomposite dielectrics for OTFTs by doping TiO2 nanoparticles into polyimide and poly(4-vinylphenol), respectively. To obtain a homogenous organic–inorganic composite film, well-dispersed TiO2 nanoparticles in polyimide solution are important; therefore, several dispersants were assessed on the basis of the measurement of the rheological behavior of slurries. An approximately 400-nm-thick nanocomposite film with homogeneous distribution of TiO2 nanoparticles in polyimide and low roughness is obtained after curing at 200 oC, resulting in a low leakage current density of the nanocomposite film, when less than 2 vol% TiO2 nanoparticles are well dispersed in polyimide slurry. The dielectric constant of the organic–inorganic nanocomposite increases with increasing TiO2 content in polyimide, being situated in the range between 4 and 5
In order to enhance the dielectric constant of nanocomposites and great dispersion for inkjet printing, the polymer PVP and pearl-milling are employed instead of the PI matrix and ball-mill. Then we studied the parameters of ink-jet printing, including voltage, frequency and waveform. We successfully print dielectrics patterns for accomplishing the purpose of directly-patternable. The pentacene-TFT based on the printed nanocomposite dielectrics, which demonstrate high performance with increasing in mobility and reducing threshold voltage. It is observed that a better surface benefits the pentacene growth by Raman spectroscopy.
Further, in order to enhance the channel mobility and satisfy with the requirement of low-cost fabrication, we first prepare a low-cost, mask-free, reduced material wastage, deposited technology using transparent, directly printable, air-stable semiconductor slurries and dielectric solutions. We demonstrate an inkjet-printing deposition for fabricating printable transistors with ZnO nanoparticles as the active channel and poly(4-vinylphenol) (PVP) matrix as the gate dielectric, respectively. After annealing at 200 oC, the inkjet-printed ZnO-TFTs exhibit the carrier mobility of 0.69 cm2/Vs, SS of 29 V/decade, and the threshold voltage of 25.5 V. Consequently, a stable and non-precipitated metal oxide ink with appropriate doping was prepared for the fabrication of an all-inkjet-printed transistor by inkjet printing. Transparent materials including dielectric PVP and conductive CNT were employed into the fabrication of our inkjet printing process. The experimental all-printed TFT was annealed at 180 oC and demonstrated a threshold voltage and mobility, and SS are -5 V, 0.194 cm2/Vs, and 20 V/decade initially.
In our investigations, we attempt to obtain a high performance and low-cost TFT via preparing materials, designing device structure, and using inkjet printing technology. The soluble direct-printing process is a powerful tool for material research and implies that the printable materials and the printing technology enable the use of all-printed low-cost flexible displays and other transparent electronic applications.

中文摘要.............III
Abstract ................V
Acknowledgements.................VIII
Table of Contents....IX
Figure Captions ...XIII
Chapter 1 Introduction............. 22
1.1 Background.................. 22
1.2 Motivation.................... 27
1.2.1 A high performance of thin-film-transistor ................. 27
1.2.2 A low-cost directly patternable technology using solution materials .. 31
Chapter 2 Overviews: Theory and techniques of TFTs based on nanocomposite gate dielectrics and metal oxides........ 34
2.1 TFT device structure design and operation.... 34
2.1.1 Device structures of TFTs .......... 34
2.1.2 Fundamental operation of TFTs ........... 37
2.1.3 Electrical characterization of TFTs ...... 39
2.2 Characteristics and carrier transport of semiconductors ....... 45
2.2.1 Current transport processes................ 46
2.2.2 Organic semiconductor materials (OSC) and pentacene ... 47
2.2.3 Metal oxide semiconductor materials (MOSC) ........... 68
2.3 Gate dielectrics ............ 80
2.3.1 Review of gate dielectrics........... 82
2.3.2 Nanocomposite gate dielectrics ............. 84
2.3.3 Theory of gate dielectrics and relationship in OTFTs ..... 87
2.3.4 A mini-review of basic mixing models for our nanocomposite............. 88
2.3.5 Behaviors of fillers in mediums............. 91
2.4 Mechanism of Inkjet printing technology (IJP) ... 97
2.4.1 Jetting and drop formation of IJP tech... 97
2.4.2 Effect of IJP parameters and defects..... 104
2.4.3 Ink properties ....118
Chapter 3 Experiments ........... 122
3.1 Raw materials ............ 122
3.2 Experiments ............... 124
3.2.1 Simple processing flows ........... 124
3.2.2 Process equipments .................. 135
3.3 Main Measurement ..... 136
Chapter 4 Preparation of Photosensitive Polymer as Patternable Gate Dielectric for High Performance OTFT Fabrications by Double-Gate structure .... 138
4.1 Introduction ............... 138
4.2 Results and Discussion... 140
4.2.1 Characteristics of DCPVA gate dielectric film with MIM structure 140
4.2.2 Characteristics of double-gate OTFT devices using DCPVA ............ 145
4.3 Conclusion.................. 155
Chapter 5 High-k Nanocomposite materials as Printed Gate Dielectrics for Low threshold voltage of OTFTs by Inkjet Printing .......... 156
5.1 Introduction ............... 156
5.2 Results and Discussion... 159
5.2.1 Stabilization of TiO2 nanoparticle dispersion by polyacrylic acid..... 159
5.2.1.1 Effect of dispersant type (PAA and PAE) for TiO2-PI slurries ....... 159
5.2.2 Characteristics of TiO2-PVP nanocomposite dielectric... 172
5.2.3 Characteristics of TiO2-PVP nanocomposite dielectric for OTFTs by inkjet printeing ........ 185
5.3 Conclusion.................. 192
Chapter 6 Preparation of high mobility metal-oxide inks for inkjet-printed active layer of TFTs for low-cost and low temperature deposition.............. 195
6.1 Motivation.................. 195
6.2 Results and Discussion... 197
6.2.1 ZnO nanoparticles ink for inkjet printing................. 197
6.2.2 All-inkjet-printed IZTO TFT by inkjet printing......... 207
6.3 Conclusion.................. 214
Chapter 7 Conclusion and future work........... 216
7.1 Conclusion.................. 216
7.2 Future work ............... 223
7.2.1 Improving the properties of inks ........ 223
7.2.2 Efficiently annealing ................ 224
References ........ 225
Publication list .... 248

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