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研究生：	李崇根 Lei, Song-Kan
論文名稱：	藉由表面修飾調整金或銀之電洞注入能力於高分子發光二極體 Tuning the hole injection capability of silver/gold via surface modification for polymer light-emitting diodes
指導教授：	溫添進 Wen, Ten-Chin
學位類別：	碩士 Master
系所名稱：	工學院 - 化學工程學系 Department of Chemical Engineering
論文出版年：	2008
畢業學年度：	96
語文別：	英文
論文頁數：	106
外文關鍵詞：	surface modification, self-assembled monolayer, metal anode, polymer light-emitting diodes
相關次數：	點閱：78 下載：1
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本論文之研究包含兩個部份，第一部分利用氟取代基在不同位置之氟苯硫酚修飾金屬電極；第二部分利用噻吩及其衍生物修飾銀電極，探討其對高分子發光二極體 (PLEDs)電洞注入之影響並應用在上發光型高分子發光二極體 (T-PLEDs)。兩部分的內容分別敍述如下﹕
在第一部分中，分別利用鄰-氟苯硫酚(2-FTP)、間-氟苯硫酚(3-FTP)和對-氟苯硫酚(4-FTP) 三種不同位置之氟取代基分子，分別修飾厚度為4nm和150nm的金、銀電極，探討不同位置之氟取代基對高分子發光二極體電洞注入之影響。藉由分析元件之電流-電位特徵圖，可以得知經修飾後元件的電洞注入能力大小分別為: 4-FTP > 3-FTP > 2-FTP，顯示出表面偶極會到受氟原子位置的影響。此外，經由動態接觸角跟化學分析能譜的分析，可得知氟苯硫酚分子在金、銀以及在不同厚度的基板上，其分子的排列會有所不同，尤其是2-FTP分子。2-FTP 的分子排向很容易受到銀不同的表面型態所影響，使2-FTP在不同厚度的銀基板上有不同的分子排向，不同的分子排向導致產生不同大小的表面偶極。
在第二部分中，利用不同濃度(分別為1mM和1M)的噻吩(TP)、3-甲基噻吩(CH3TP)、3-氰基噻吩(CNTP)來修飾銀電極並探討對高分子發光二極體電洞注入之影響。由反射式UV-Vis光譜的分析得知高濃度(1M)的TP和CH3TP 會在銀的表面上自發性聚合，同時形成多層結構的高分子膜。但是，低濃度(1mM)的TP、CH3TP、CNTP以及高濃度(1M)的CNTP只是單純吸附在銀的表面上，且在銀的表面上比較傾向於平躺的結構。元件電洞注入能力的大小分別為:在高濃度(1M)時，CNTP > Ag > CH3TP > TP；但在低濃度(1mM)時，TP、 CH3TP 、CNTP > Ag，由此可知元件經由不同濃度(1mM和1M)的噻吩衍生物修飾過以後，元件具有不同的電性特性，這是因為經由低濃度噻吩衍生物修飾過以後，由於表面偶極效應使得元件的起始電壓能夠提前；而在高濃度的時候，由於聚合的TP、 CH3TP所形成的多層高分子膜引起阻擋電洞進入的效應，使得元件的起始電壓會大大的增加。

In this study, fluorothiophenol, and thiophene derivatives were used to modified metal anode and study the effect on hole injection for polymer light-emitting diodes (PLEDs), respectively, and their application on top-emissive PLEDs (T-PLEDs), respectively. The contents include two parts:
In first section, we have investigated the effect of fluorothiophenol (2-FTP, 3-FTP and 4-FTP) modified nano-scale (4nm) and bulk (150nm) metal (Ag and Au) substrates on hole injection for PLEDs. The hole injection ability increases in the order: 4-FTP > 3-FTP > 2-FTP, demonstrating that the surface dipole depends strongly on the position of the fluorine atom. We also observe that the arrangement of thiols layer on Ag is different from that on Au, as well as the thickness of metals. Especially for 2-FTP, its molecular orientation is affected strongly by the surface morphology of Ag substrate. The different orientations of 2-FTP would affect the magnitude of dipole moment normal to the surface.
In second section, two different concentrations (1mM and 1M) of thiophene (TP), 3-methylthiophene (CH3TP), and 3-cyanothiophene (CNTP) were used to modify Ag anode and study the effect of thiophene derivatives on hole injection. Spontaneous polymerization of TP and CH3TP absorbed on Ag surfaces at 1M concentration was observed and formed multilayer structure on Ag surface. However, all the adsorbed TP, CH3TP, and CNTP molecules as SAMs have a dominated flat-lying configuration on Ag surface at low concentration (1mM) as well as high concentration (1M) CNTP. The hole injection ability increases in the order: CNTP > Ag > CH3TP > TP at 1M concentration, but TP, CH3TP, CNTP > Ag at 1mM concentration. The variant electrical properties of thiophene derivatives-modified devices at 1mM and 1M concentration is due to the surface dipole effect and blocking hole effect by forming multilayer polymer film, respectively.

Contents
中文摘要..................................................i
Abstract................................................iii
誌謝......................................................v
Contents.................................................vi
List of Figures..........................................ix
List of Tables.........................................xiii
Symbols and abbreviation................................xiv

Chapter 1 Introduction....................................1
1-1 Organic Light-Emitting Diodes.........................1
1-1-1 Small molecule and polymer OLEDs....................2
1-1-2 Mechanism of electroluminescence for PLEDs..........4
1-1-3 Bottom-emissive and top-emissive O/PLEDs............7
1-1-4 Anode modifications in top-emissive PLEDs...........9
1-2 Self-Assembled Monolayer.............................10
1-2-1 Application of SAMs on T-PLEDs.....................12
1-2-2 Thiol molecules on silver and gold surfaces........14
1-2-2-1 Effect of growth time on SAMs....................14
1-2-2-2 Effect of solvent on SAMs........................15
1-2-2-3 Effect of surface roughness on SAMs..............16
1-2-2-4 Effect of temperature on SAMs....................16
1-2-2-5 Orientations of SAMs on metal surfaces...........16
1-3 Research Motivation..................................18
1-3-1 The effect of SAMs based on fluorothiophenol on 
PLEDs....................................................18
1-3-2 The effect of SAMs based on thiophene derivatives on PLEDs....................................................19
Chapter 2 Surface modification of metal anode using fluorothiophenols and its effect on hole injection.......32
2-1 Foreword.............................................32
2-2 Experiment...........................................33
2-2-1 Materials..........................................33
2-2-2 Fabrication of PLEDs devices and measurements......33
2-2-2-1 Etching of ITO-coated glass......................33
2-2-2-2 Cleaned ITO-coated glass.........................34
2-2-2-3 Prepared metal substrates and formation of thiols layer....................................................34
2-2-2-4 Fabricated hole dominated PLEDs and T-PLEDs......34
2-2-2-5 Device measurement and other analysis............35
2-3 Results and discussion...............................37
2-3-1 Surface wettability of SAMs-modified metals........37
2-3-2 Surface composition on metals and interaction of thiol with metals........................................40
2-3-3 Relation between surface energy and work function for SAMs modification....................................42
2-3-4 Hole injection ability of PLEDs with SAMs-modified anode....................................................45
2-3-5 Top-emissive PLEDs performance with SAMs-modified anode....................................................46
2-4 Conclusion...........................................48

Chapter 3 Surface modification of thiophene derivatives on Ag anode and its effect on hole injection................64
3-1 Foreword.............................................64
3-2 Experiment...........................................65
3-2-1 Materials..........................................65
3-2-2 Fabrication of PLEDs devices and other measurements65
3-3 Results and discussion...............................67
3-3-1 Optical property of thiophene derivatives on Ag surface..................................................67
3-3-2 Surface characteristic of thiophene derivatives on Ag surface...............................................69
3-3-3 Hole injection ability of PLEDs with thiophene derivatives-modified anode...............................72
3-3-4 Thermal annealing effect on hole injection ability with CH3TP-modified anode................................74
3-3-5 Top-emissive PLEDs performance with thiophene-modified anode...........................................76
3-4 Conclusion...........................................78

Chapter4 Summary.........................................92
References...............................................94
Appendix................................................101
Curriculum Vitae........................................106
                                    

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