Sebastian Stolz

The Compromises of Printing Organic Electronics: A Case Study of Gravure‐Printed Light‐Emitting Electrochemical Cells

Light-emitting electrochemical cells (LECs) are fabricated by gravure printing. The compromise between device performance and printing quality is correlated to the ink formulation and the printing process. It is shown that the rheological properties of the ink formulations of LECs can be tailored without changing the chemical composition of the material blend.

Soluble Diazaiptycenes: Materials for Solution-Processed Organic Electronics

The synthesis and characterization of soluble azaiptycenes is reported. Optical and physical properties were studied and compared with those of the structurally consanguine azaacenes. Electrochemical experiments and quantum-chemical calculations revealed the electronic structure of the iptycene derivatives. Their crystallization behavior was examined. A highly fluorescent amorphous diazatetracene derivative was integrated into a simple organic light-emitting diode, showing enhanced performance compared with that of previously reported, structurally similar tetracenes.

Investigation of Solution-Processed Ultrathin Electron Injection Layers for Organic Light-Emitting Diodes

We study two types of water/alcohol-soluble aliphatic amines, polyethylenimine (PEI) and polyethylenimine-ethoxylated (PEIE), for their suitability as electron injection layers in solution-processed blue fluorescent organic light-emitting diodes (OLEDs). X-ray photoelectron spectroscopy is used to determine the nominal thickness of the polymer layers while ultraviolet photoelectron spectroscopy is carried out to determine the induced work-function change of the silver cathode. The determined work-function shifts are as high as 1.5 eV for PEI and 1.3 eV for PEIE. Furthermore, atomic force microscopy images reveal that homogeneous PEI and PEIE layers are present at nominal thicknesses of about 11 nm. Finally, we solution prepare blue emitting polymer-based OLEDs using PEI/PEIE in combination with Ag as cathode layers. Luminous efficiency reaches 3 and 2.2 cd A(-1), whereas maximum luminance values are as high as 8000 and 3000 cd m(-2) for PEI and PEIE injection layers, respectively. The prepared devices show a comparable performance to Ca/Ag OLEDs and an improved shelf lifetime.

Degradation Mechanisms in Organic Light-Emitting Diodes with Polyethylenimine as a Solution-Processed Electron Injection Layer

In this work, we investigate the performance and operational stability of solution-processed organic light-emitting diodes (OLEDs), which comprise polyethylenimine (PEI) as an electron injection layer (EIL). We show that the primary degradation mechanism in these OLEDs depends on the cathode metal that is used in contact with the EIL. In the case of Al, the deterioration in OLED performance during electrical driving is mainly caused by excitons which reach and subsequently degrade the emitter/PEI interface. In contrast, in the case of Ag, device performance degradation occurs due to an additional mechanism: hole accumulation at the emitter/PEI interface and a consequent drop in the emitter quantum yield. As a result, the operational lifetime of OLEDs that use PEI as EIL can vary significantly with the cathode material, and at a current density of 20 mA cm-2, LT50 lifetimes of ∼200 h and <10 h are obtained for Al and Ag, respectively. Finally, we show that the first degradation mechanism can be significantly slowed by using a mixture of PEI and ZnO nanoparticles as EIL. As a result, the operational lifetime of OLEDs with an Al cathode is increased to more than 1000 h, without adversely affecting device performance. This lifetime is significantly longer than that of a LiF/Al reference OLED.

Comparison of biodegradable substrates for printed organic electronic devices

Building on the results of the green chemistry movement, the development of biodegradable strain sensors and OLEDs, produced from sustainable materials and solvents, is presented. The choice of solvents and substrate is discussed in the context of terms relevant to printing, namely solvent solubility parameters, surface wetting envelopes and surface roughness. A new method for producing biodegradable and flat substrates from a common and commercially available cellulose diacetate foil is presented. Challenges associated with working with biodegradable foils are presented and different techniques are discussed to ultimately overcome these challenges and produce functional devices. Lastly, many green solvents and several commercially available biodegradable foils are compared for consideration in future work.

High-Performance Electron Injection Layers with a Wide Processing Window from an Amidoamine-Functionalized Polyfluorene

In this work, we present organic light-emitting diodes (OLEDs) utilizing a novel amidoamine-functionalized polyfluorene (PFCON-C) as an electron injection layer (EIL). PFCON-C consists of a polyfluorene backbone to which multiple tertiary amine side chains are connected via an amide group. The influence of molecular characteristics on electronic performance and morphological properties was tested and compared to that of the widely used, literature known amino-functionalized polyfluorene (PFN) and polyethylenimine (PEI). PFCON-C reduces the turn-on voltage (VON) of poly(p-phenylene vinylene) (PPV)-based OLEDs from ∼5 to ∼3 V and increases the maximum power efficiency from <2 to >5 lm W(-1) compared to that of PFN. As a result of its semiconducting backbone, PFCON-C is significantly less sensitive to the processing parameters than PEI, and comparable power efficiencies are achieved for devices where thicknesses of PFCON-C are between 15 and 35 nm. Atomic force microscopy (AFM) measurements indicate that the presence of nonpolar side chains in the EIL material is important for its film-forming behavior, while Kelvin probe measurements suggest that the amount of amine groups in the side chains influences the work-function shift induced by the EIL material. These results are used to suggest strategies for the design of polymeric electron injection layers.

One-step additive crosslinking of conjugated polyelectrolyte interlayers: improved lifetime and performance of solution-processed OLEDs

We crosslink an amino-functionalized polyfluorene by the solvent additive 1,8-diiodooctane (DIO). DIO remains in the film after drying of the main solvent and chemically binds to the amino-side groups after a low temperature annealing step, rendering the polyfluorene film insoluble in non-polar solvents. We correlate the amount of DIO, the reduction of operational voltage and increase in lifetime of solution-processed OLEDs. We demonstrate a fully solution-processed device using the crosslinked polyfluorene electron injection layer and an inkjet-printed Ag top electrode.

Correlation of Device Performance and Fermi Level Shift in the Emitting Layer of Organic Light-Emitting Diodes with Amine-Based Electron Injection Layers

We investigate three amine-based polymers, polyethylenimine and two amino-functionalized polyfluorenes, as electron injection layers (EILs) in organic light-emitting diodes (OLEDs) and find correlations between the molecular structure of the polymers, the electronic alignment at the emitter/EIL interface, and the resulting device performance. X-ray photoelectron spectroscopy measurements of the emitter/EIL interface indicate that all three EIL polymers induce an upward shift of the Fermi level in the emitting layer close to the interface similar to n-type doping. The absolute value of this Fermi level shift, which can be explained by an electron transfer from the EIL polymers into the emitting layer, correlates with the number of nitrogen-containing groups in the side chains of the polymers. Whereas polyethylenimine (PEI) and one of the investigated polyfluorenes (PFCON-C) have six such groups per monomer unit, the second investigated polyfluorene (PFN) only possesses two. Consequently, we measure Fermi level shifts of 0.5-0.7 eV for PEI and PFCON-C and only 0.2 eV for PFN. As a result of these Fermi level shifts, the energetic barrier for electron injection is significantly lowered and OLEDs which comprise PEI or PFCON-C as an EIL exhibit a more than twofold higher luminous efficacy than OLEDs with PFN.