In this work, we present the visualization of the internal flows in a drying sessile polymer dispersion drop on hydrophilic and hydrophobic surfaces with Spectral Radar Optical Coherence Tomography (SR-OCT). We have found that surface features such as the initial contact angle and pinning of the contact line, play a crucial role on the flow direction and final shape of the dried drop. Moreover, imaging through selection of vertical slices using optical coherence tomography offers a feasible alternative compared to imaging through selection of narrow horizontal slices using confocal microscopy for turbid, barely transparent fluids.

In this study, multilayer organic light-emitting diodes (OLEDs) consisting of three solution-processed layers are fabricated using slot die coating, gravure printing, and inkjet printing, techniques that are commonly used in the industry. Different technique combinations are investigated to successively deposit a hole injection layer (poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT:PSS)), a cross-linkable hole transport layer (N,N′-bis(4-(6-((3-ethyloxetan-3-yl)methoxy)-hexyloxy)phenyl)-N,N′-bis(4-methoxyphenyl)biphenyl-4,4′-diamin (QUPD)), and a green emissive layer (TSG-M) on top of each other. In order to compare the application techniques, the ink formulations have to be adapted to the respective process requirements. First, the influence of the application technique on the layer homogeneity of the different materials is investigated. Large area thickness measurements of the layers based on imaging color reflectometry (ICR) are used to compare the application techniques regarding the layer homogeneity and reproducible film thickness. The total stack thickness of all solution-processed layers of 32 OLEDs could be reproduced homogeneously in a process window of 30 nm for the technique combination of slot die coating and inkjet printing. The best efficiency of 13.3 cd A−1 is reached for a process combination of slot die coating and gravure printing. In order to enable a statistically significant evaluation, in total, 96 OLEDs were analyzed and the corresponding 288 layers were measured successively to determine the influence of layer homogeneity on device performance.

The authors present the feasibility of sheet fed direct gravure printing for ultrathin, organic semiconductor films on ITO coated glass. Printing with chrome plated gravure cylinders is often believed to require flexible substrates to promote fluid transfer to the substrate. However, the results demonstrate a stable process for the smallmolecule Spiro-MeOTAD dissolved in toluene on rigid substrates. The authors obtained layer thicknesses in the range of 5-100 nm. They identified certain boundaries for gravure cell size yielding printed films with thickness of 10-15 nm with good homogeneity suitable for organic light emitting diodes or organic photovoltaics. For gravure cells smaller or larger than the optimal range, the printed layer is afflicted with dot-or ribbinglike structures. The authors show that the latter may result from nip-induced Saffman-Taylor instabilities rather than spinodal dewetting or Marangoni effects. Finally, electrical characterization of a completed stack (PEDOT:PSS electrode) give evidence for integrity of the printed semiconductor layers. V C 2011 Society for Imaging Science and Technology.[DOI: xxxxxx] INTRODUCTIONIn this article, we present our recent direct gravure printing experiments of ultrathin, small-molecule based semiconductor layers with thicknesses in the range of 5-100 nm on indium tin oxide (ITO) coated glass substrates. Smallmolecule semiconductors are well adapted materials for vacuum deposition of layers for organic devices such as organic light emitting diodes (OLEDs) and organic photovoltaics. This manufacturing technique imposes limits to high throughput and cost efficiency. A rapid and reliable solution based coating or printing process can offer many advantages in this respect, as many small-molecule materials are known to be soluble in a variety of solvents. Studies on principal differences between vacuum and solution processed layers and their effect on device performance have been done by Lee et al. using spin-coating techniques. 1 However, spin-coating technique is not suitable for large scale production. It is our aim to close the still persistent gap between spin-coating and laboratory-scale processing methods on one side and to develop a gravure printing process suitable for large volume production of OLED lighting, display, and photovoltaic applications.

A basic solution‐processable organic light‐emitting diode (OLED) stack comprising two organic layers is presented in this study. The hole injection layer (poly(3,4‐ethylenedioxythiophene)‐poly(styrenesulfonate), PEDOT:PSS) is slot die coated and flexographically printed for process comparison in terms of film homogeneity and the device performance. The emissive layer consisting of a small molecule host–guest system with a green triplet emitter is slot die coated. The single layer thicknesses are mapped by an in‐house developed imaging color reflectometry enabling the precise measurement of the layer thicknesses over the whole coating area (>50 cm2). Luminance, current density, and light and current efficiency are defined for two different pixel sizes with the active area of 6 × 4 and 14 × 14 mm2. A total of 100 OLEDs are measured showing a very low standard deviation for the different pixels. The solely slot die coated OLEDs show much higher current and power efficiency than the OLEDs with flexographically printed PEDOT:PSS. Small molecule OLEDs reach efficiencies up to 30 cd A−1 and 8 lm W−1. Additionally OLED demonstrators with an active area of ≈27 cm2 are fabricated.

We considered pattern formation, i.e. viscous fingering, in the ink splitting process between an elastic flexographic printing plate and the substrate. We observed an unexpected scaling behavior of the emerging pattern length scale (i.e., finger width) as a function of printing velocity, fluid viscosity, surface tension, and plate elasticity coefficients. Scaling exponents depended on the ratio of the capillary number of the fluid flow, and the elastocapillary number defined by plate elasticity and surface tension. The exponents significantly differed from rigid printing plates, which depend on the capillary number only. A dynamic model is proposed to predict the scaling exponents. The results indicate that flexo printing corresponded to a self-regulating dynamical equilibrium of viscous, capillary, and elastic forces. We argue that these forces stabilize the process conditions in a flexo printing unit over a wide range of printing velocities, ink viscosities, and mechanical process settings.

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Printing process development for fabrication of organic electronic devices is described, with focus on semiconductor layers for organic light‐emitting diodes and photovoltaic cells. This development is considerably more complex than for a graphical printing process. Key aspects are an adequate dosing and transfer of highly volatile inks, the reliable coalescence of the droplets deposited on the substrate to a closed liquid film, and the successful relaxation and leveling of the liquid–air interface in the solvent evaporation phase in the presence of Marangoni stresses and pattern formation instabilities. The conditions for successful implementation of a gravure or inkjet process, using steadily developing, new generations of polymer as well as small molecule semiconductors are, to a large extent, but not exclusively, originating from the molecular features of organic semiconductors and their printable solutions. In addition, recent developments in surface technology, and in the physics of thin‐film dynamics and spontaneous pattern formation contribute to a proper understanding of liquid layer dynamics in printed electronics. The role of ink formulation, Marangoni stresses related to concentration and temperature gradients, the effect of the disjoining pressure, and solvent evaporation are discussed.