Programmable reconfiguration of one-dimensional supramolecular polymers into multidimensional topological nanostructures

Supramolecular polymers (SPs) formed by strong directional noncovalent interactions among molecular subunits possess high degrees of internal order, making them promising candidates for the construction of one-dimensional (1D) sophisticated architectures. However, the directional packing of subunits, in turn, may limit the processability of their overall shape and dimensionality, which play significant roles in determining the properties of nanomaterials. How to realize the topological engineering of SPs beyond their shape and dimensionality remains a challenging task. Here, we demonstrate that 1D crystalline SPs of positively charged organometallic complexes can be tailored into multidimensional topological loops by adding oppositely charged block copolymers (BCPs), thereby triggering dynamic structural reconfiguration of the preformed SPs. The kinetics of structural reconfiguration can be finely modulated, enabling one to rationally fabricate multidimensional heterostructures containing both rigid and flexible constituent parts with unprecedented topologies (i.e., tri-block, penta-block, hepta-block, multi-segment, rod-loop, etc.), as well as spatially distinct features.