Dynamic pathways in energy landscapes guiding supramolecular Janus dendrimer self-assemblies between lamellar and cubic architectures

Elaborate kinetic control enables supramolecular self-assemblies to deviate from equilibrium, depicting profound energy landscapes with remarkable structural and functional diversity. Despite this potential, achieving an energy landscape that encompasses lamellar and inverse cubic structures remains a significant challenge, contrasting with the sophisticated structural transformations naturally orchestrated by cellular systems. Here, we present a dynamic and minimalistic Janus dendrimer self-assembly system capable of reversibly transitioning between lamellar vesicles and inverse cubic structures. By exploiting temperature-triggered non-covalent interactions, including OEG interdigitation and hydrogen bonding, conformational flexibility, and molecular packing, we reveal a rich energy landscape featuring diverse assembly pathways spanning lamellar vesicles and inverse cubosomes. Our study not only enriches the structural versatility of Janus dendrimer assemblies but also provides a foundation for advancing supramolecular systems toward applications in biomedicine, catalysis, and beyond.