靜電紡絲纖維於光電元件之應用

陳蓉瑤

doi:10.6342/NTU201600331

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静电纺丝纤维於光电元件之应用

Electrospun Nanofibers for Optoelectronic Device Applications

陈蓉瑶 , 博士　　导师：陈文章　　

英文 DOI： 10.6342/NTU201600331

静电纺丝；二次电场；表面电浆共振；萤光太阳能聚合器；有机场效电晶体；有机太阳能电池； electrospinning ； secondary electric field ； surface plasmonic resonance ； luminescent solar concentrator ； organic field-effect transistor ； organic photovoltaic device

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摘要 │ 参考文献 (198) │ 国际计量

摘要〈TOP〉

光电元件中电荷载子的非等向性传递，促使一维奈米结构研究蓬勃地发展。此外，奈米尺度的几何局限性更改变了原材料在块材状态时的性质。相较其他制备一维奈米结构的方法，静电纺丝提供了简便、快速又连续化的制成，对於大量制造上更有其成本上的优势。除了单一材料奈米纤维，静电纺丝纤维更是一个良好载体，可导入其他功能性材料来提升光电元件的特性。然而目前将静电纺丝纤维应用在光电元件的例子仍是少数。在此篇论文中我们制备出各种功能性静电纺丝纤维，应用於有机场效电晶体和提升有机太阳能电池效能表现。其研究细节分述如下:
第二章中我们在一般静电纺丝装置导入二次电场的方式来提升静电纺丝的拉伸效果来达到顺向高分子链的效果，由差式扫描量热法(differential scanningcalorimetry)和X 光绕射光谱(X-ray diffraction)结果显示聚(3-己烷基噻吩)(P3HT)经由二次电场拉伸後有效拉伸P3HT 高分子链并抑制P3HT 进行thiophene 堆叠，且高分子链沿纤维长轴方向排列，使载子由原本的π-π 堆叠造成的载子传递改成链上传递，有效提升载子迁移率达1000 倍，此做法可移除原本需加热後处理提升载子迁移率的问题，使静电纺丝技术更具有工业化优势。
第三章中由原本单纯的高分子系统延伸至有机/无机复合材料，结合银还原和静电纺丝的方法提出一维银导电奈米纤维的制备，藉由调控电纺参数，可有效提升银奈米颗粒的结晶度和顺向性，且银线的导电度可高达5.6*105 S m-1。进一步地利用银奈米纤维的表面电浆共振现象加上静电纺丝可顺向性，制备出埋有顺向、相交和不织布型态银奈米纤维的P3HT:PC61BM 太阳能电池，成功提升太阳能电池效率至4.19 %达到18.7 %的提升效果。
在第四章中，以交联过的聚甲基丙烯酸(PMAA)为主体制备出含有银和共轭性茀系衍生物(PFBT)奈米颗粒的静电纺丝萤光太阳能聚合器(luminescent solar concentrator)，其中PFBT 可当光学转换材料，银奈米颗粒则提供表面电浆效应和导电通路。PFBT 可吸收主动层材料吸收效率低的光源并转换成主动层材料吸收率高的波段，且由於银的存在可发挥其表面电浆共振效应，除了提升主动层材料激发子的产生速率，更能提升PFBT 的发光效率。此双功能性复合电纺纤维埋入P3HT:PC61BM 和PTB7:PC71BM 有机太阳能电池中可达到效率上18 %的提升。
以上的研究显示静电纺丝纤维可经由调控电纺参数制备出各式功能性奈米纤维，且其不管是巨观上的纤维顺向性抑或是微观上高分子链的顺向性皆提供光电元件应用上独特的特性。

并列摘要〈TOP〉

One-dimensional (1D) nanostructures coupled with its possible technological applications have fueled the exponential growth of optoelectronics because of the anisotropic transportation of charge-carrier. The geometry confinement provided by 1D nanostructures also alter the optoelectrical characteristic compared to their bulkcounterpart. Among of the various fabrication of 1D nanostructure, electrospinning is a versatile assembly method for fabricating uniform and ultrafine nanofibers with different patterning via various geometric collectors. Also, electronspun nanofibers can serve as matrix for functional materials such as metallic nanoparticle, conjugated polymer and quantum dot for diverse application in optoelectronic device. However, the applications of such nanofibers in optoelectronic devices have not been fully explored yet. Furthermore, the unique process of electrospinning enable the distinctive characteristic of electrospun nanofiber is also not investigated. In this thesis, we produce diverse functional ES nanofibers and explore their morphology, opto-electrical properties and applications on organic field-effect transistor (OFET) and organic photovoltaic(OPV). The details of each topic are summarized as below:

In chapter 2, an extra electric field below the spinneret in electrospinning setup was introduced for producing poly(3-hexylthiophene) (P3HT) nanofibers. The liquid jet is greatly prolonged by the additional extensional force and thinner fibers can thusbe obtained. The chain conformation and orientation in fibers are probed by differential scanning calorimetry (DSC) and X-ray diffraction techniques. Under the influence of the secondary electric field, P3HT chains are extensively stretched and aligned along the fiber axis. The electrospun P3HT nanofibers are fabricated into field-effect transistors and the charge carrier mobilities of the nanofibers with and without secondary electric field are found to be 1.54×10-4 and 1.62×10-1 cm2 V-1 s-1, respectively. The dramatic enhancement of mobility by more than 1000 times is due to the effective charge transport through the delocalization of electrons along the highly extended and oriented P3HT backbones rather than the ordinary π-π stacking. In addition to P3HT, we find this simple method also works for other poly(3-alkylthiophene).

In chapter 3, the significant enhancement of the P3HT:PC61BM ([6,6]-phenyl C61-butyric acid methyl ester) photovoltaic devices using different patterns of the electrospun Ag/PVP composite nanofibers, including non-woven, aligned-, and crossed-patterns were reported. The composite electrospun nanofibers were prepared through the in-situ reduction of silver (Ag) nanoparticles in Ag/poly(vinyl pyrrolidone) (PVP) through two-fluid coaxial electrospinning technique. The composition, crystalline orientation, and particle size of Ag were successfully manipulated by controlling the core/shell solution concentration (AgF-1, AgF-2 and AgF-3), as evidenced by FE-SEM, TEM and SAED analyses. The smallest diameter of thecomposite nanofibers led to the highest orientation of the Ag nanoparticles and resulted in the largest conductivity comparable to that of ITO, due to the geometrical confinement. Such composite nanofibers exhibited the surface plasmon resonance (SPR) effect, evidenced by the absorption peak around 425 nm, which provide near field enhancement of electromagnetic field around active layer. In addition, the composite nanofibers with the crossed- or nonwoven patterns further enhanced high carrier mobility, compared to those of aligned-pattern. It led to the 18.7% enhancement on the power conversion efficiency of photovoltaic cell (ITO/composite nanofibers/PEDOT:PSS/P3HT:PC61BM/Ca/Al) compared to the parent device. The above results indicated the high conductivity and SPR effect of the Ag/PVP electrospun nanofibers could significantly improve the photocurrent as well as PCE, leading to promising organic solar cell applications.

In chapter 4, plasmonic-enhanced luminescent solar concentrator (LSC) electrospun nanofiber by coaxial electrospinning technique with poly[2,7-(9,9-dihexylfluorene)-alt-4,7-(2,1,3-benzothiadiazole)](PFBT) nanoparticle as the LSC and Ag nanoparticle as the SPR center was explored. The ES nanofiber, crosslinked poly(methacrylic acid) (PMAA),provides a solvent-proof matrix for LSC without changing the conventional OPVs configuration. Besides, the in-situ reduction of Ag nanoparticle simultaneously enhanced the exciton generation of PFBT and active material with the SPR effect. The dualfunctional ES nanofibers allow significant light harvesting through down conversion and enhanced exciton generation, leading to remarkably 18 % enhancement on the PCE for both P3HT:PC61BM and PTB7 (polythieno[3,4-b]-thiophene-cobenzodithiophene): PC71BM([6,6]-phenyl C71-butyric acid methyl ester) [6,6]-phenyl) photovoltaic cells. This configuration provides a novel method to integrate the plasmonicenhanced LSC electrospun nanofiber into OPV device with the combination of two light trapping methods (SPR and LSC) and the maintenance of active area coverage.

The above studies address the characteristics of electrospun nanofibers can be feasibly manipulated the composition and process condition during electrospinning. The orientation property in micro-scope and macro-scope of electrospun nanofibers also indicate the unique application in optoelectronic devices.

参考文献 ( 198 ) 〈TOP〉

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