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Nature’s photosynthetic machinery uses precisely arranged pigment-protein complexes, often representing superstructures, for efficient light-harvesting and transport of excitation energy (excitons) during the initial steps of photosynthesis. This function is achieved by defined electronic Coulomb interactions between the conjugated molecules resulting in tailored excited-state energy landscapes. While such complex natural structures are synthetically difficult to achieve, supramolecular chemistry is now on its advent to realize defined artificial supramolecular nanostructures with tailored functionalities via controlled self-assembly processes of small molecules. In this review, we focus on recent work reporting photophysical studies on self-assembled and hierarchical nanostructures as well as complex superstructures. We discuss how the resulting excited-state energy landscapes influence energy transport. Progress in the field of supramolecular chemistry allows for the realization of distinct kinds of H- or J-aggregates with well-defined morphologies on the mesoscale. Advances in the field of optical spectroscopy and microscopy have permitted to resolve the incoherent/coherent dynamics of exciton transport in such systems down to the level of single nanostructures. Although outstanding diffusion lengths of up to several  μ m were found in selected nanostructures, a full understanding of the underlying principles is still missing. In particular, the unavoidable structural and electronic disorder in these systems influences the excited-state energy landscapes and thus the transport characteristics, which can be exploited to refine the molecular design criteria of supramolecular nanostructures and complex superstructures. Despite the rapid progress in the field of functional supramolecular nanostructures, we believe that revealing the full potential of such systems is far from complete. In particular, criteria for tailored and optimized (hierarchical) supramolecular nanostructures in view of applications are not yet established. Finally, we outline current challenges and future perspectives for optical and optoelectronic applications of supramolecular nanostructures.

Tailoring the excited-state energy landscape in supramolecular nanostructures