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Post-spin Stretch Improves Mechanical Properties, Reduces Necking, and Reverts Effects of Aging in Biomimetic Artificial Spider Silk Fibers

Gabriele Greco, Benjamin Schmuck, Fredrik G. Bäcklund, Günter Reiter and Anna Rising. ACS Applied Polymer Materials, published online

reiter-2024-05.jpgRecent biotechnological advancements in protein production and development of biomimetic spinning procedures make artificial spider silk a promising alternative to petroleum-based fibers. To enhance the competitiveness of artificial silk in terms of mechanical properties, refining the spinning techniques is imperative. One potential strategy involves the integration of post-spin stretching, known to improve fiber strength and stiffness while potentially offering additional advantages. Here, we demonstrate that post-spin stretching not only enhances the mechanical properties of artificial silk fibers but also restores a higher and more uniform alignment of the protein chains, leading to a higher fiber toughness. (more...)


Mechanistically Different Mechanochromophores Enable Calibration and Validation of Molecular Forces in Glassy Polymers and Elastomeric Networks

Raphael Hertel, Maximilian Raisch, Michael Walter, Günter Reiter, Michael Sommer. Angew. Chem. Int. Ed. 2024, e202409369

sommer.jpgSterically distorted donor-acceptor p‑systems, termed DA springs, can be progressively planarized under mechanical load causing a bathochromic shift of the photoluminescence (PL) spectrum. By combining theory and experiment, we here use a simple linear force calibration for two different conformational mechanochromophores to determine molecular forces in polymers from the mechanochromic shift in PL wavelength during multiple uniaxial tensile tests. Two systems are used, i) a highly entangled linear glassy polyphenylene and ii) a covalent elastomeric polydimethylsiloxane network. The mean forces estimated by this method are validated using known threshold forces for the mechanochemical ring-opening reactions of two different spiropyran force probes. The agreement between both approaches underlines that these DA springs provide the unique opportunity for the online monitoring of local molecular forces present in diverse polymer matrices.(more...)


"Printing" on Polymer Single Crystals through Microregional Heating

Tianyu Wu, Haimu Ye, Xinyi Pan, Yaning He, Jun Xu, Günter Reiter. ACS Appl. Polym. Mater. 2024, 6, 14, 7969–7977

tianyu.jpgPolymer single crystals are composed of well-ordered polymer chains and possess a characteristic symmetric shape. If one can precisely control the microregional morphology, polymer single crystals have the potential to be used as functional templates for applications like information storage or cell culture. However, with current experimental approaches, it is rather difficult to generate predictable structures of defined size within polymer single crystals. Here, we propose a research strategy based on a combination of fluorescence labeling and microregional heating by irradiation with focused red light. This approach enabled us to locally heat single crystals while simultaneously following the thereby induced changes via fluorescence imaging with a micrometer lateral resolution. We found that polymers diffused out of the heated region within a stacked single crystal and thereby produced a hole at the irradiated location. (more...)


Mechanism for the Formation of Millimeter-Long Solid Filaments by Spin Coating Dilute Solutions of a Crystallizable Polymer

Da Huang, Thorsten Hugel, and Günter Reiter. Macromolecules 2024, 57, 3696–3705

huang.jpgWe have investigated the formation of millimeter-long filaments induced by spin-coating ca. 130 °C dilute para-xylene solutions of rapidly crystallizable polyethylene chains with a contour length in the micrometer range onto ca. 80 °C mica substrates. These filaments were radially oriented and accumulated on the periphery of the substrate. Our observations can be explained by the stretching of polymers through the flow field induced by spinning the solution on a solid substrate. The corresponding loss in conformational entropy emphasized attractive interactions between polymers, which resulted in the formation of bundles and their assembly into long filaments. Caused by a Plateau–Rayleigh-type instability of a liquid coating on a solid filament and due to crystallization, these filaments were decorated with various small-scale structures. (more...)


 

Liste der Veröffentlichungen

Thermodynamic Features of Perfectly Crystalline Poly(3-Hexylthiophene) Based on Flory’s Relation
Mina Alizadehaghdam, Silvia Siegenführ, Farhang Abbasi, and Günter Reiter. Journal of Polymer Science Part B: Polymer Physics 57, 431–437 (2019)
Thermodynamic Features of Perfectly Crystalline Poly(3-hexylthiophene) Revealed Through Studies of Imperfect Crystals
Mina Alizadehaghdam, Barbara Heck, Silvia Siegenführ, Farhang Abbasi, and Günter Reiter. Macromolecules 52 (2019) 2487–2494
A Structural Fibrillation Parameter from Small Angle X-ray Scattering to Quantify Pulp Refining
Jia Mao, Barbara Heck, Hatem Abushammala, Günter Reiter, and Marie-Pierre Laborie. Cellulose 26 (2019) 4265–4277
Following isothermal and non-isothermal crystallization of poly(3- hexylthiophene) thin films by UV-vis spectroscopy
Mina Alizadehaghdam, Barbara Heck, Silvia Siegenführ, Yaser AlShetwi, Fanuel M. Keheze, Sebastian Stäter, Farhang Abbasia, Günter Reiter. Polymer 210 (2020) 122959
Snails as living 3D printers: free forms for the architecture of tomorrow
Christoph Allgaier, Benjamin Felbrich, Frederik Wulle, Emna Khechine, James H. Nebelsick, Achim Menges, Günter Reiter, Renate Reiter, Armin Lechler, Alexander Verl, Karl-Heinz Wurst. In Knippers, J; Schmid, U.; Speck, T. (eds.) Biomimetics for Architecture, Birkhäuser, Basel 2019, pp 126-133. (ISBN: 978-3-0356-1791-7)
Controlling the Growth of Stacks of Correlated Lamellar Crystals of a Block Copolymer
Sumit Majumder, Renate Reiter, Jun Xu and Günter Reiter. Macromolecules 52 (2019) 9665-9671
Determination of the Critical Size of Secondary Nuclei on the Lateral Growth Front of Lamellar Polymer Crystals
Shujing Zhang, Jiarui Han, Yang Gao, Bao-Hua Guo, Günter Reiter, Jun Xu. Macromolecules 52 (2019) 7439-7447
A Nucleation Mechanism Leading to Stacking of Lamellar Crystals in Polymer Thin Films
Sumit Majumder, Purushottam Poudel, Hui Zhang, Jun Xu, Günter Reiter. Polymer International 69 (2020) 1058
Processing Pathways Decide Polymer Properties at the Molecular Level
S. Chandran, J. Baschnagel, D. Cangialosi, K. Fukao, E. Glynos, L. M. C. Janssen, M. Müller, M. Muthukumar, U. Steiner, J. Xu, S. Napolitano, and G. Reiter. Macromolecules 52 (2019) 7146-7156
Controlling the Pore Size in Conjugated Polymer Films via Crystallization-Driven Phase Separation
Shaowen Guo, Changyu Shen, Jingbo Chen, Günter Reiter, Bin Zhang. Soft Matter 15 (2019) 2981-2989
Adapted Creep Test for the Study of Non-Equilibrated Thin Polymer Films
Farzad Ramezani. Inaugural-Dissertation zur Erlangung des Doktorgrades der Fakultät für Mathematik und Physik der Albert-Ludwigs-Universität Freiburg 2019
Tad Pili Play a Dynamic Role in Caulobacter crescentus Surface Colonization
Matteo Sangermani, Isabelle Hug, Nora Sauter, Thomas Pfohl, Urs Jenala. mBio 10:e01237-19 (2019)
Spatially resolved small-angle X-ray scattering for characterizing mechanoresponsive liposomes using microfluidics
Marzia Buscema, Hans Deyhle, Thomas Pfohl, Andreas Zumbuehl, Bert Müller. Materials Today Bio 1 (2019) 100003
Semicrystalline Non-Isocyanate Polyhydroxyurethanes as Thermoplastics and Thermoplastic Elastomers and Their Use in 3D Printing by Fused Filament Fabrication
Vitalij Schimpf, Johannes B. Max, Benjamin Stolz, Barbara Heck, and Rolf Mülhaupt. Macromolecules 52 (2019) 320-331
Self-Assembly of Oligo(phenylene-thiophene)s on Monolayer Graphene: Molecular Dynamics Simulations
Natalia Borzdun, Victor Nazarychev, Sergey Larin, Guenter Reiter, Sergey Lyulin. J. Phys. Chem. C, 123 (2019) 859–867
Functional macromolecular systems: kinetic pathways to obtain tailored structures
V. Abetz, K. Kremer, M. Müller, and G. Reiter. Macromolecular Chemistry and Physics 220 (2019) 1800334
Growth Kinetics of Stacks of Lamellar Polymer Crystals
Sumit Majumder, Hanna Busch, Purushottam Poudel, Stefan Mecking, and Günter Reiter. Macromolecules 51 (2018) 8738–8745
Self-Interference of Exciton Emission in Organic Single Crystals Visualized by Energy-Momentum Spectroscopy
Christian Schörner, Sajedeh Motamen, Laurent Simon, Günter Reiter, Richard Hildner. ACS Omega 3 (2018) 6728–6736
Formation of Periodically Modulated Polymer Crystals
Purushottam Poudel, Sumit Majumder, Sivasurender Chandran, Hui Zhang, Günter Reiter. Macromolecules 51 (2018) 6119–6126
Generating Nanoscopic Patterns in Conductivity Within a Poly(3-hexylthiophene) Crystal Via Bias-controlled Scanning Probe Nanolithography
Binghua Wang, Bin Zhang, Changyu Shen, Jingbo Chen, Günter Reiter. Macromolecules 51 (2018) 7692-7698
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