| One key component in more advanced multilayer polymer light-emitting diode (PLED) structures is the hole transport layer (HTL). Conventional PLED conductive polymer HTLs exhibit serious drawbacks such as corrosion of anodes, significant absorption in visible region, and mediating oxidative doping of polyfluorene emissive layers (EMLs). In addition, the question still remains as to whether conventional PLED HTLs have the electron-blocking capacity required to achieve high-performance PLEDs. If not, the question arises as to how a PLED structure can be modified to afford greater electron-blocking at the HTL/EML interface.;In the present thesis work, three generations of PLED HTLs were developed based on a siloxane-derivatized, crosslinkable, hole-transporting material, 4,4'-bis[(p-trichlorosilylpropylphenyl)phenylamino]biphenyl, TPDSi2. The first generation is the self-assembled monolayer (SAM) of TPDSi2, which can increase the work function of indium tin oxide (ITO) anode, enhance ITO anode hole injection, and hence improve PLED performance. The second generation is the spin-coated blend of TPDSi2 and a hole transporting polymer TFB on ITO, which forms an insoluble crosslinked network that can be used as a PLED HTL. The third generation is a double-layer HTL with the TPDSi2 + TFB on top of a conventional PLED HTL, which combines the hole injection capacity of conventional PLED HTLs and the electron-blocking capacity of the TPDSi2 + TFB blend. PLED devices based on these new HTLs exhibit comparable or superior performance compared to those based on conventional HTLs; high current efficiencies of ∼17 cd/A and maximum luminance of ∼140,000 cd/m2 have been achieved. These siloxane-based HTLs not only enhance PLED anode hole-injection by chemically bonding the HTL to the ITO anode, they also exhibit great electron-blocking capacity. The present organosiloxane HTL approach offers many other attractions such as convenience of fabrication, flexibility in choosing HTL components, and reduced HTL-induced luminescence quenching, and can be applied as a general strategy to achieve high-performance PLEDs. |
