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Watching Molecular Nanotubes Self-Assemble in Real Time
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-10-06 , DOI: 10.1021/jacs.3c07103
Marìck Manrho 1 , Sundar Raj Krishnaswamy 1 , Björn Kriete 1 , Ilias Patmanidis 2, 3 , Alex H de Vries 2 , Siewert J Marrink 2 , Thomas L C Jansen 1 , Jasper Knoester 1, 4 , Maxim S Pshenichnikov 1
Affiliation  

Molecular self-assembly is a fundamental process in nature that can be used to develop novel functional materials for medical and engineering applications. However, their complex mechanisms make the short-lived stages of self-assembly processes extremely hard to reveal. In this article, we track the self-assembly process of a benchmark system, double-walled molecular nanotubes, whose structure is similar to that found in biological and synthetic systems. We selectively dissolved the outer wall of the double-walled system and used the inner wall as a template for the self-reassembly of the outer wall. The reassembly kinetics were followed in real time using a combination of microfluidics, spectroscopy, cryogenic transmission electron microscopy, molecular dynamics simulations, and exciton modeling. We found that the outer wall self-assembles through a transient disordered patchwork structure: first, several patches of different orientations are formed, and only on a longer time scale will the patches interact with each other and assume their final preferred global orientation. The understanding of patch formation and patch reorientation marks a crucial step toward steering self-assembly processes and subsequent material engineering.

中文翻译:


实时观察分子纳米管自组装



分子自组装是自然界的一个基本过程,可用于开发用于医学和工程应用的新型功能材料。然而,它们的复杂机制使得自组装过程的短暂阶段极难揭示。在本文中,我们跟踪了基准系统双壁分子纳米管的自组装过程,其结构与生物和合成系统中的结构相似。我们选择性地溶解了双壁系统的外壁,并使用内壁作为外壁自重组的模板。结合微流体、光谱学、低温透射电子显微镜、分子动力学模拟和激子建模,实时跟踪重组动力学。我们发现外壁通过瞬态无序拼凑结构进行自组装:首先,形成多个不同方向的斑块,只有在较长的时间尺度上,这些斑块才会相互作用并呈现其最终首选的全局方向。对补片形成和补片重新定向的理解标志着朝着引导自组装过程和后续材料工程迈出的关键一步。
更新日期:2023-10-06
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