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Caught in the Act: Mechanistic Insight into Supramolecular Polymerization-Driven Self-Replication from Real-Time Visualization
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-07-31 , DOI: 10.1021/jacs.0c02635 Sourav Maity 1 , Jim Ottelé 2 , Guillermo Monreal Santiago 2 , Pim W J M Frederix 3 , Peter Kroon 3 , Omer Markovitch 2, 4 , Marc C A Stuart 2 , Siewert J Marrink 3 , Sijbren Otto 2 , Wouter H Roos 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-07-31 , DOI: 10.1021/jacs.0c02635 Sourav Maity 1 , Jim Ottelé 2 , Guillermo Monreal Santiago 2 , Pim W J M Frederix 3 , Peter Kroon 3 , Omer Markovitch 2, 4 , Marc C A Stuart 2 , Siewert J Marrink 3 , Sijbren Otto 2 , Wouter H Roos 1
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Self-assembly features prominently in fields ranging from materials science to biophysical chemistry. Assembly pathways, often passing through transient intermediates, can control the outcome of assembly processes. Yet, the mechanisms of self-assembly remain largely obscure due to a lack of experimental tools for probing these pathways at the molecular level. Here, the self-assembly of self-replicators into fibers is visualized in real-time by high-speed atomic force microscopy (HS-AFM). Fiber growth requires the conversion of precursor molecules into six-membered macrocycles, which constitute the fibers. HS-AFM experiments, supported by molecular dynamics simulations, revealed that aggregates of precursor molecules accumulate at the sides of the fibers, which then diffuse to the fiber ends where growth takes place. This mechanism of precursor reservoir formation, followed by one-dimensional diffusion, which guides the precursor molecules to the sites of growth, reduces the entropic penalty associated with colocalizing precursors and growth sites and constitutes a new mechanism for supramolecular polymerization.
中文翻译：
陷入困境：从实时可视化中深入了解超分子聚合驱动的自我复制
自组装在从材料科学到生物物理化学的领域中占有突出地位。组装途径通常通过瞬态中间体，可以控制组装过程的结果。然而，由于缺乏在分子水平上探索这些途径的实验工具，自组装的机制在很大程度上仍然模糊不清。在这里，通过高速原子力显微镜 (HS-AFM) 实时可视化自复制器到纤维中的自组装。纤维生长需要将前体分子转化为构成纤维的六元大环。由分子动力学模拟支持的 HS-AFM 实验表明，前体分子的聚集体聚集在纤维的侧面，然后扩散到发生生长的纤维末端。
更新日期：2020-07-31
中文翻译：
陷入困境：从实时可视化中深入了解超分子聚合驱动的自我复制
自组装在从材料科学到生物物理化学的领域中占有突出地位。组装途径通常通过瞬态中间体，可以控制组装过程的结果。然而，由于缺乏在分子水平上探索这些途径的实验工具，自组装的机制在很大程度上仍然模糊不清。在这里，通过高速原子力显微镜 (HS-AFM) 实时可视化自复制器到纤维中的自组装。纤维生长需要将前体分子转化为构成纤维的六元大环。由分子动力学模拟支持的 HS-AFM 实验表明，前体分子的聚集体聚集在纤维的侧面，然后扩散到发生生长的纤维末端。
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