Multiscale Molecular Modelling of ATP-fueled Supramolecular Polymerisation and Depolymerisation

Fuel-regulated self-assembly is a key principle by which Nature creates spatiotemporally controlled materials and dynamic molecular systems that are in continuous communication (molecular exchange) with the external environment. Designing artificial materials that self-assemble and disassemble via conversion/consumption of a chemical fuel is a grand challenge in supramolecular chemistry, which requires a profound knowledge of the factors governing these complex systems. Here we focus on recently reported metal-coordinated monomers that polymerise in the presence of ATP and depolymerise upon ATP hydrolysis, exploring their fuel-regulated self-assembly/disassembly via multiscale molecular modelling. We use all-atom simulations to assess the role of ATP in stabilising these monomers in assemblies, and we then build on a minimalistic model to investigate their fuel-driven polymerization and depolymerization on a higher scale. In this way, we elucidate general aspects of fuel-regulated self-assembly that are important toward the rational design of new types of bioinspired materials.