Sustainable Materials and Process Techniques for Engineering Solution-Based Organic Light-Emitting Devices

Advances in organic light emitting devices are crucial for the development of the display and solid state lighting (SSL) technologies. This dissertation is organized and pursued in three main projects to meet some problems in the field. Printing technologies can be the key to next-generation affordable, flexible, large area displays and lighting elements by eliminating vacuum processing. In the first part of the thesis, the conventional gravure printing technique was adapted for the processing of emissive layers in the small molecule based organic light-emitting diodes (OLEDs) and light-emitting electrochemical cells (LECs). The homogeneous printed layers were granted by either modifying the functional ink properties or altering the printing process parameters. Different functional inks comprising the small molecule as an emissive material were formulated by adjusting viscosity, surface tension, and solvent drying kinetics of the inks. As for the process parameters, the gravure cell parameters such as line screen and tone values were altered to control the overall transfer volume of the ink and the thickness of the printed layers. In both cases, the electrically inert polymers were used as host materials to modify the rheological behavior of the ink while suppressing the aggregation of the small molecule in a solid film. The thin film characteristics of printed layers were analyzed in both qualitative and quantitative ways. The printed films were successfully implemented in the active layer of efficient small molecule based electroluminescent devices on flexible plastic foil. The optical and electrical device performance were considered as well as the effect of the printing process in comparison to spin-coated pristine small molecule based reference devices. The quality and performance of the printed emissive layers in both device type showed that the gravure printing method can be an alternative solution for wet-processing roll-to-roll (R2R) manufacturing in the future. White light-emitting diodes draw particular attention in the field, due to their potential application as the backlight in displays or as energy efficient luminaires for SSL. Even though polymer OLEDs are well-suited for wet-based continues R2R fabrication, evaporation of low work function cathodes and therewith encapsulation remain as major obstacles. In the second part of the work, a novel hybrid device architecture was suggested for the color-tuning and white light emission in polymer light-emitting diodes. The single component polymer LEC layer performed as the electron injection layer as well as the second emissive layer on top of a conventional polymer OLED stack. The hybrid structure maintained a sufficient charge carrier injection from an air-stable cathode, due to the unique operation principles of LECs. As a proof of charge transport at the intersection of two emissive layers, dual color emission was simultaneously observed in a bilayer device configuration. A color-tuning in emission was obtained by changing the thickness of the LEC layer. The emission of hybrid devices was shifted from yellow to white light emission region of the CIE color chromaticity diagram, resulting in OLEDs with the high color temperature values. The results demonstrated that this approach showed a promising potential to achieve color-tuning and white light emission from solution processed OLEDs bearing air-stable cathodes. Sustainable bioelectronics is an emerging technology which to replace conventional electronics with disposable counterparts in the future. Thus, bioinspired and bioderived materials usage in organic electroluminescent devices gained much attention in the last years. In the last part of the thesis, we investigated biodegradable natural and naturally derived polymers such as gelatin, deoxyribonucleic acid (DNA) as the ion-solvating polymers in the emissive layer of polymer LECs. Notably, we focused on DNA and DNA-lipid complex based polyelectrolytes due to the unique hybrid ionic/electronic conductivity behavior of DNA. Different solid polymer electrolytes (SPE) were tested with varying additives of salts at different ratios towards improving the ionic conductivity. Additionally, the electrochemical stability window of SPEs was defined to eliminate nonreversible electrochemical side reactions during device operation. The optoelectrical device characteristics, as well as lifetime measurements, were obtained to determine the stability of LECs. Furthermore, the surface morphology of the active layers was investigated to characterize the phase separation between SPE and emissive polymer and aggregations in thin films, which have a significant influence on the device performance. Biosolid polymer electrolytes were successfully implemented in LECs as promising materials of bio-based LECs