高性能電洞注入/傳遞之新型三苯胺聚合物和聚胺酯的合成與性質研究及其在有機電致發光元件的應用

林坤榮

doi:10.6342/NTU.2008.02268

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高性能電洞注入/傳遞之新型三苯胺聚合物和聚胺酯的合成與性質研究及其在有機電致發光元件的應用

High-Performance Hole-Injection/Transport Poly(p-methylenetriphenylamine), Poly(4-vinyltriphenylamine) and Polyurethane for Light-Emitting Diodes (LEDs) Applications

林坤榮 , Ph.D　　Advisor：謝國煌　　Co-advisor ：梁文傑

英文 DOI： 10.6342/NTU.2008.02268

有機發光二極體；三苯胺聚合物；聚胺酯；電洞傳導層；電聚合； Triphenylamine (TPA) ； Poly(p-methylenetriphenylamine) (PMTPA) ； Poly(4-vinyltriphenylamine) (PVTPA) ； Polymeric light-emitting diodes (PLEDs) ； Electropolymerization ； Electroluminescence (EL) ； Hole-transport layer (HTL) ； Polyurethanes (PUs)

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The synthesis and characterization of hyperbranched poly(p-methylenetriphenylamine) (PMTPA) are described. We discovered that N-[4-(tosyloxybutyloxymethyl)phenyl]-N,N-diphenylamine showed unexpected chemical reactivity and polymerized to form hyperbranched PMTPA under neat conditions. The hyperbranched PMTPA was electrochemically active and was deposited on electrode surface when oxidized. The SEM study revealed that electropolymerization of PMTPA would form uniform coating onto ITO surface. Polymeric light-emitting diodes (PLEDs) employing electroactive polymers of either hyperbranched PMTPA or linear Poly(4-vinyltriphenylamine) (PVTPA) as hole-transport layer in the EL device of ITO/electrochemically polymerized HTL/EML(PVK-PBD-Ir(ppy)3)/Mg/Ag demonstrated the brightness over 20,000 cd/m2 and low turn-on voltage. In particular, the device performance was very steady regardless of the thickness of the PMTPA layer, ranging from 4 to 10 nm. 
In addition, PLEDs using a series of linear poly(4-vinyltriphenylamines) (PVTPAs) as hole-transport layer were fabricated. The relationships between their molecular weight, thermal stabilities, surface morphology and electronic properties were investigated. The SEM study revealed that electropolymerization of lowest molecular weight (~2700 g/mol) of PVTPA with 3 CV cycles would form uniform coating on ITO surface and show the highest brightness (~34,400 cd/m2) among others. However, surface modification tactic has to be adopted for the other higher molecular weight of PVTPAs because numerous cracks were observed on the electrode surface. We discovered applying some homogeneous thin film primed the ITO anode prior to the electrodeposition of PVTPA would reduce dramatically the uneven distribution of the electroactive layer and eventually have a smooth, crack-free film surface.
By the way, our experiments also showed that the PU polymer could also be applied for flexible PLED with similar performance enhancement. Based on the promising results, we concluded that OPV-IPDI was a good hole-transport material for light-emitting diode application.

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