| Summary: | The discovery of highly efficient organic light-emitting diodes (OLEDs) in the 1980s has stimulated extensive research on organic semiconductors and devices. Underlying this breakthrough is the realization of the organic heterojunction (OH). Besides OLEDs, the implementation of the OH also significantly improves the power conversion efficiency in organic photovoltaic cells (OPVs). The continued technological advancements in organic electronic devices depend on the accumulation of knowledge of the intrinsic properties of organic materials and related interfaces. Among them, charge-carrier transport and carrier injection are two key factors that govern the performance of a device.
This thesis mainly focuses on the charge carrier injection and transport at organic heterojunctions. The carrier transport properties of different organic materials used in this study are characterized by time-of-flight (TOF) and admittance spectroscopy (AS). An injection model is formulated by considering the carrier distribution at both sides of the interface. Using a steady-state simulation approach, the effect of accumulated charges on energy level alignment at OH is revealed. Instead of a constant injection barrier, it is found that the barrier varies with applied voltage. Moreover, an escape probability function in the injection model is modified by taking into account the total hopping rate and available hopping sites at the interface. The model predicts that the injection current at low temperature can be dramatically modified by an extremely small density of deep trap states. More importantly, the temperature dependence of the injection current is found to decrease with increasing barrier height. This suggests that extracting the barrier height from the J vs 1/T plot, as commonly employed in the literature, is problematic. These theoretical predictions are confirmed by a series of experiments on heterojunction devices with various barrier heights. In addition, the presence of deep trap states is also consistent with carrier mobility measurements at low temperature.
From the point of view of application, an interface chemical doping method is proposed to engineer the carrier injection at an organic heterojunction. It is found that the the injection current can be effectively increased or suppressed by introducing a thin (2 nm) doped organic layer at the interface. This technique is further extended to study the impact of an injection barrier at the OH. in OLEDs, on device performance. It is shown that a 0.3 eV injection barrier at the OH, that is normally negligible at metal/organic interface, can reduce the device efficiency by 25 %. This is explained by the carrier distribution in the density-of-states at the OH.
Furthermore, the carrier transport properties in a bulk heterojunction system are investigated. The bulk heterojunction consists of an interpenetrating network of a polymeric electron donor and a molecular electron acceptor. This material system has been studied in the last few years as an attractive power conversion efficiency (5% under AM 1.5) of OPV cells has been demonstrated. It is found that the electron mobility is greatly dependent on the thermal treatment of the film. Interfacial dipole effect at the heterojunction between the donor and the acceptor is proposed to be the determining factor that alters the carrier mobility in different nano-scale structures.
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