A central paradigm of self-assembly is to create ordered structures starting from molecular<br>monomers that spontaneously recognize and interact with each other via noncovalent interactions.<br>In the recent years, great efforts have been directed toward reaching the perfection in the<br>design of a variety of supramolecular polymers and materials with different architectures. The<br>resulting structures are often thought of as ideally perfect, defect-free supramolecular fibers,<br>micelles, vesicles, etc., having an intrinsic dynamic character, which are typically studied at the<br>level of statistical ensembles to assess their average properties. However, molecular simulations<br>recently demonstrated that local defects that may be present or may form in these assemblies, and which are poorly captured by conventional approaches, are key to controlling their dynamic<br>behavior and properties. The study of these defects poses considerable challenges, as the<br>flexible/dynamic nature of these soft systems makes it difficult to identify what effectively constitutes<br>a defect, and to characterize its stability and evolution. Here, we demonstrate the power<br>of unsupervised machine learning techniques to systematically identify and compare defects in<br>supramolecular polymer variants in different conditions, using as a benchmark 5°A-resolution<br>coarse-grained molecular simulations of a family of supramolecular polymers. We shot that this<br>approach allows a complete data-driven characterization of the internal structure and dynamics<br>of these complex assemblies and of the dynamic pathways for defects formation and resorption.<br>This provides a useful, generally applicable approach to unambiguously identify defects in<br>these dynamic self-assembled materials and to classify them based on their structure, stability<br>and dynamics.<br>
Identifying and Tracking Defects in Dynamic Supramolecular Polymers
