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- ItemAB- Versus AA+BB-Suzuki Polycondensation: A Palladium/Tris(tert-butyl)phosphine Catalyst Can Outperform Conventional Catalysts(Weinheim : Wiley-VCH, 2020) Zhang, Kenan; Tkachov, Roman; Ditte, Kristina; Kiriy, Nataliya; Kiriy, Anton; Voit, BrigitteA Pd/Pt-Bu3 catalyst having bulky, electron-rich ligands significantly outperforms conventional “step-growth catalysts” Pd(PPh3)4 and Pd(Po-Tol3)3 in the Suzuki polycondensation of the AB-type arylene-based monomers, such as some of the substituted fluorenes, carbazoles, and phenylenes. In the AA+BB polycondensation, Pd/Pt-Bu3 also performs better under homogeneous reaction conditions, in combination with the organic base Et4NOH. The superior performance of Pd/Pt-Bu3 is discussed in terms of its higher reactivity in the oxidative addition step and inherent advantages of the intramolecular catalyst transfer, which is a key step joining catalytic cycles of the AB-polycondensation. These findings are applied to the synthesis of a carbazole-based copolymer designed for the use as a hole conductor in solution-processed organic light-emitting diodes. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
- ItemSelf-Replication of Deeply Buried Doped Silicon Structures, which Remotely Control the Etching Process: A New Method for Forming a Silicon Pattern from the Bottom Up(Weinheim : Wiley-VCH, 2021) Schutzeichel, Christopher; Kiriy, Nataliya; Kiriy, Anton; Voit, BrigitteA typical microstructuring process utilizes photolithographic masks to create arbitrary patterns on silicon substrates in a top-down approach. Herein, a new, bottom-up microstructuring method is reported, which enables the patterning of n-doped silicon substrates to be performed without the need for application of etch-masks or stencils during the etching process. Instead, the structuring process developed herein involves a simple alkaline etching performed under illumination and is remotely controlled by the p-doped micro-sized implants, buried beneath a homogeneous n-doped layer at depths of 0.25 to 1 µm. The microstructuring is realized because the buried implants act upon illumination as micro-sized photovoltaic cells, which generate a flux of electrons and increase the negative surface charge in areas above the implants. The locally increased surface charge causes a local protection of the native silicon oxide layer from alkaline etching, which ultimately leads to the microstructuring of the substrate. In this way, substrates having at their top a thick layer of homogeneously n-doped silicon can be structured, reducing the need for costly, time-consuming photolithography steps. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
- ItemCharge Carrier Mobility Improvement in Diketopyrrolopyrrole Block-Copolymers by Shear Coating(Basel : MDPI, 2021) Ditte, Kristina; Kiriy, Nataliya; Perez, Jonathan; Hambsch, Mike; Mannsfeld, Stefan C.B.; Krupskaya, Yulia; Maragani, Ramesh; Voit, Brigitte; Lissel, FranziskaShear coating is a promising deposition method for upscaling device fabrication and enabling high throughput, and is furthermore suitable for translating to roll-to-roll processing. Although common polymer semiconductors (PSCs) are solution processible, they are still prone to mechanical failure upon stretching, limiting applications in e.g., electronic skin and health monitoring. Progress made towards mechanically compliant PSCs, e.g., the incorporation of soft segments into the polymer backbone, could not only allow such applications, but also benefit advanced fabrication methods, like roll-to-roll printing on flexible substrates, to produce the targeted devices. Tri-block copolymers (TBCs), consisting of an inner rigid semiconducting poly-diketo-pyrrolopyrrole-thienothiophene (PDPP-TT) block flanked by two soft elastomeric poly(dimethylsiloxane) (PDMS) chains, maintain good charge transport properties, while being mechanically soft and flexible. Potentially aiming at the fabrication of TBC-based wearable electronics by means of cost-efficient and scalable deposition methods (e.g., blade-coating), a tolerance of the electrical performance of the TBCs to the shear speed was investigated. Herein, we demonstrate that such TBCs can be deposited at high shear speeds (film formation up to a speed of 10 mm s−1). While such high speeds result in increased film thickness, no degradation of the electrical performance was observed, as was frequently reported for polymer−based OFETs. Instead, high shear speeds even led to a small improvement in the electrical performance: mobility increased from 0.06 cm2 V−1 s−1 at 0.5 mm s−1 to 0.16 cm2 V−1 s−1 at 7 mm s−1 for the TBC with 24 wt% PDMS, and for the TBC containing 37 wt% PDMS from 0.05 cm2 V−1 s−1 at 0.5 mm s−1 to 0.13 cm2 V−1 s−1 at 7 mm s−1. Interestingly, the improvement of mobility is not accompanied by any significant changes in morphology.