Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 142, Issue 32, Pages 13709-13717Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c02635
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Funding
- MSCA Individual fellowship [INTERACT 751404]
- NWO Vidi grant
- STW Perspectief grant Cancer-ID [14192]
- ERC
- Netherlands Organization for Scientific Research (Veni) [722.015.005]
- Dutch Ministry of Education, Culture and Science [024.001.035]
- NWA StartImpuls
- Center for Information Technology of the University of Groningen
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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.
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