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Selective Dissolution as a Tool for Detecting Spatial Variations in the Degree of Metastability within Lamellar Polymer Crystals

Binghua Wang, Hailong Zou, Xuchen Wang, Changyu Shen, Jingbo Chen, Günter Reiter, Bin Zhang. Nature Communications 16 (2025) 3275

The dissolution of polymer crystals often proceeds at rates varying in time and space. Here, using low molecular weight poly(ethylene oxide) as a model polymer, we exploit step-wise selective dissolution for unveiling how spatial variations in metastability are generated during the growth of lamellar polymer single crystals. The dissolution velocity along defined crystal faces is constant, but ca. 5 times faster for rough than for smooth faces. From the temperature dependence of dissolution, we derive detachment energies of 420 ± 40 kJ/mol and 650 ± 50 kJ/mol for rough and smooth faces, respectively, suggesting that on a rough face polymer chains have ca. 1/3 less neighboring molecules to interact with. The observed high values of the activation energy indicate that, for dissolving a polymer crystal, the progressive detachment of whole chains is indispensable. Our study reveals a strong relation between growth kinetics and the resulting metastability of polymer crystals. (more...)


London dispersion forces and steric effects within nanocomposites tune interaction energies and chain conformation

Baode Zhang, Snežana D. Zarić, Sonja S. Zrilić, Iosif Gofman, Barbara Heck, Günter Reiter. Communications Chemistry 8 (2025) 21

baode.jpgThe interplay between attractive London dispersion forces and steric effects due to repulsive forces resulting from the Pauli principle often determines the geometry and stability of nanostructures. Aromatic polyimides (PI) and carbon nanotubes (CNT) were chosen as building blocks as two components in the hetero delocalized electron nanostructures. Two PIs, having the same diamine part and different linkage substituents between two phenyl rings of dianhydride part, one linked with ether bond (C-O-C) (OPI), the other with C-(CF3)2 (FPI), were investigated. Surprisingly, two CNT/PI nanocomposites show distinct failure mode from CNT yielding to CNT pull-out failure. Calculation of the interaction energy and chain conformations of each PI upon CNT was performed by accurate density functional theory (DFT) calculations and molecular dynamic simulation (MDS). (more...)


Effect of chemical structure on the crystallization kinetics of triple polymorphic high-sulfur-content polythioethers

Valentina Pirela, Leire Unanue, Justine Elgoyhen, Javier Ramos, Juan Francisco Vega, Agurtzane Mugica, Manuela Zubitur, Cuong Minh Quoc Le, Abraham Chemtob, Radmila Tomovska, Günter Reiter, Jaime Martín, Alejandro J. Müller. European Polymer Journal (2025) 113721

This work studies how the chemical structure of relatively similar high-sulfur alternating polythioether homopolymers (DMDS-alt-DVE, DMDS-alt-TEGDVE, and DMDS-alt-BDDVE) affects their structural properties, morphology, polymorphism, and crystallization kinetics. Differential scanning calorimetry (DSC) and polarized light optical microscopy (PLOM) experiments revealed a complex crystallization for the samples in which up to three different polymorphic phases were identified: a very low melting crystal form (VL-Tm form), a low melting crystal form (L-Tm form) and a high melting crystal form (H-Tm form), characterized by their corresponding melting temperature ranges and confirmed via Wide-Angle X-ray Scattering (WAXS). A coexistence of negative and positive spherulites was found, and their origin was revealed by atomic force microscopy (AFM), which showed how the lamellar arrangement varied in the samples from predominantly radial to a cross-hatched morphology. (more...) 


 

Liste der Veröffentlichungen

Tuning topography and patterns of thin polymer films on structured substrates
Konstantinos Roumpos. Inauguraldissertation der Fakultät für Mathematik und Physik 2021. DOI: 10.6094/UNIFR/194127
Morphological transitions in langmuir films of a diblock copolymer from polyethylene glycol and poly-L-lactide
Emna Khechine. Inaugural-Dissertation zur Erlangung des Doktorgrades der Fakultät für Chemie und Pharmazie, 2021
High-throughput injection molding of transparent fused silica glass
Markus Mader, Oliver Schlatter, Barbara Heck, Andreas Warmbold, Alex Dorn, Hans Zappe, Patrick Risch, Dorothea Helmer, Frederik Kotz, Bastian E. Rapp. Science 372 (2021) 182-186
Formation of large polymer crystals from metastable solutions
Tianyu Wu. Inauguraldissertation der Fakultät für Chemie und Pharmazie 2020, DOI: 10.6094/UNIFR/167415
Exploring pathways to equilibrate Langmuir polymer films
Abhijna Das, Sebastian Noack, Helmut Schlaad, Günter Reiter, Renate Reiter. Langmuir 36 (2020) 8184–8192
Energy transport and light propagation mechanisms in organic single crystals
Bernd Wittmann, Stephan Wiesneth, Sajedeh Motamen, Laurent Simon, Françoise Serein-Spirau, Günter Reiter, and Richard Hildner. Journal of Chemical Physics 153 (2020) 144202
Large quantum efficiency enhancements of pristine conjugated polymer MEH-PPV by interlayer polymer diffusion
Po-Tsun Chen, Ya-Wei Yang, Günter Reiter, Arnold C.-M. Yang. Polymer 204 (2020) 122753
Formation of Needle-like Poly(3-hexylthiophene) Crystals from Metastable Solutions
Tianyu Wu, Thomas Pfohl, Sivasurender Chandran, Michael Sommer and Günter Reiter. Macromolecules 53 (2020) 8303–8312
Rheological Properties of Blends of Isotactic Polystyrene–Isotactic Poly(para-methylstyrene) Films Derived from a Comparative Dewetting Study
Austine Amukayia Mulama, Konstantinos Roumpos, Pradipkanti Lairenjam, Andrew Oduor, Günter Reiter. Macromolecules 53 (2020) 9122–9130
Dewetting-Induced Alignment and Ordering of Cylindrical Mesophases in Thin Block Copolymer Films
Heng Zhang, Binghua Wang, Gang Wang, Changyu Shen, Jingbo Chen, Günter Reiter, Bin Zhang. Macromolecules 53, (2020) 9631–9640
Estimation of the Size of Critical Secondary Nuclei of Melt-Grown Poly(l-lactide) Lamellar Crystals
Shujing Zhang, Baohua Guo, Günter Reiter, Jun Xu. Macromolecules 53 (2020) 3482–3492
Translating molecular relaxations in non-equilibrated polymer melts into lifting macroscopic loads
Farzad Ramezani, Jörg Baschnagel, and Günter Reiter. Phys. Rev. Materials 4 (2020) 082601
A new growth process for crystalline ultra-thin layers of conjugated oligomers used in field-effect transistor applications
Sven Renkert, Sadiara Fall, Sajedeh Motamen, Thibaut Jarrosson, Françoise Serein-Spirau, Thomas Heiser, Laurent Simon, Günter Reiter, Jean-Luc Bubendorff. Applied Surface Science 539 (2021) 148024
The memorizing capacity of polymers
Günter Reiter. J. Chem. Phys. 152, 150901 (2020)
Formation of asymmetric leaf-shaped crystals in ultrathin films of oriented polyethylene molecules resulting from high-temperature relaxation and recrystallization
Huihui Li, Duanzijing Liu, Xinyun Bu, Zhenzhen Zhou, Zhongjie Ren, Xiaoli Sun, Renate Reiter, Shouke Yan, Günter Reiter. Macromolecules 53 (2020) 346-354
Controlling phase transitions in Langmuir polymer films
Abhijna Das. Inauguraldissertation der Fakultät für Mathematik und Physik 2020. DOI: 10.6094/UNIFR/167266
Controlling Nucleation in Quasi-Two-Dimensional Langmuir Poly(L-lactide) Films through Variation of the Rate of Compression
Abhijna Das, Ahmed S. El-Tawargy, Emna Khechine, Sebastian Noack, Helmut Schlaad, Günter Reiter, and Renate Reiter. Langmuir 35 (2019) 6129-6136
Activity of the Gramicidin A Ion Channel in a Lipid Membrane with Switchable Physical Properties
Renate Reiter, Ekaterina Zaitseva, Gerhard Baaken, Ibrahim Halimeh, Jan C. Behrends, Andreas Zumbuehl. Langmuir 35 (2019) 14959-14966
Dewetting Rheology for Determining Viscoelastic Properties of Non-equilibrated Thin Polymer Films
Austine A. Mulama, Sivasurender Chandran, Konstantinos Roumpos, Andrew O. Oduor, and Günter Reiter. Macromolecules 52 (2019) 7894-7903
Relation between Charge Transport and the Number of Interconnected Lamellar Poly(3-hexylthiophene) Crystals
Binghua Wang, Jingbo Chen, Changyu Shen, Günter Reiter, Bin Zhang. Macromolecules 52 (2019) 6088-6096
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