Robust Delocalized Frenkel Excitons in Two-Dimensional Supramolecular Assemblies

Efficient energy transport in nanoscale photonic and optoelectronic systems requires excitons to remain delocalized in the presence of structural and environmental disorder, a central challenge for real-world applications ranging from artificial light harvesting to quantum information processing. Here we show that Frenkel excitons in two-dimensional supramolecular nanomaterials preserve extensive delocalization even in the presence of intentionally embedded deep-energy traps. Using fluorescent trap molecules introduced during the self-assembly of double-walled molecular nanotubes, we created a model system in which traps are incorporated without compromising the host lattice’s structural integrity. Polarization-resolved microscopy of individual nanotubes reveals that exciton delocalization is remarkably robust against trap incorporation. Complementary theoretical simulations based on realistic molecular geometries reproduce the experimental behaviour and further demonstrate that excitons adaptively redistribute to avoid trap sites. These results establish that higher-dimensional supramolecular architectures can sustain efficient exciton transport under fabrication-relevant levels of disorder, highlighting a key advantage of multidimensional excitonic materials and pointing toward the similar behaviour expected in fully three-dimensional systems.