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Tuning Chain Relaxation from an Amorphous Biopolymer Film to Crystals by Removing Air/Water Interface Limitations
Authors:Qian Han  Dr Fei Tao  Yan Xu  Hao Su  Dr Facui Yang  Dr Volker Körstgens  Prof Peter Müller-Buschbaum  Prof Peng Yang
Institution:1. Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119 China

These authors contributed equally to this work.;2. Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119 China;3. Lehrstuhl für Funktionelle Materialien, Physik Department, Technische Universität München, James-Franck-Str. 1, 85748 Garching, Germany;4. Lehrstuhl für Funktionelle Materialien, Physik Department, Technische Universität München, James-Franck-Str. 1, 85748 Garching, Germany

Heinz Maier-Leibnitz Zentrum (MLZ), Technische Universität München, Lichtenbergstr. 1, 85748 Garching, Germany

Abstract:A promising route to the synthesis of protein-mimetic materials that are capable of strong mechanics and complex functions is provided by intermolecular β-sheet stacking. An understanding of the assembly mechanism on β-sheet stacking at molecular-level and the related influencing factors determine the potential to design polymorphs of such biomaterials towards broad applications. Herein, we quantitatively reveal the air/water interface (AWI) parameters regulating the transformation from crowding amorphous aggregates to ordered phase and show that the polymorph diversity of β-sheet stacking is regulated by the chain relaxation-crystallization mechanism. An amorphous macroscale amyloid-like nanofilm is formed at the AWI, in which unfolded protein chains are aligned in a short-range manner to form randomly packed β-sheets. The subsequent biopolymer chain relaxation-crystallization to form nanocrystals is further triggered by removing the limitations of energy and space at the AWI.
Keywords:amyloids  biopolymer chain relaxation  nonclassical crystallization  nucleation  surface tension and spatial freedom
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