Watching Molecular Nanotubes Self-Assemble in Real Time

Citation (APA 7)

Manrho, M., Krishnaswamy, S. R., Kriete, B., Patmanidis, I., de Vries, A. H., Marrink, S. J., … & Pshenichnikov, M. S. (2023). Watching molecular nanotubes self-assemble in real time. Journal of the American Chemical Society, 145(41), 22494-22503.

Abstract

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.