ABSTRACT
Supramolecular structures constructed by the non-covalent assembly of monomers have emerged over the last three decades as important nanostructured materials with promising applications in optoelectronics, light-harvesting, catalysis, and biology. In addition, the dynamic, transient, and adaptive nature of supramolecular nanoarchitectures showed great promise for use as a soft materials interface for creating biomimetic systems, catering to a variety of innovative and futuristic functions. Most notably, the function of these self-assembled supramolecular materials is highly dependent on their structure and dynamics. Therefore, to rationally design and develop supramolecular nanostructures with desired complexity and functional output, it is crucial to have an in-depth understanding of their structural characteristics and dynamic properties. Moreover, combining such knowledge with the mechanistic understanding of the self-assembly process can ultimately allow researchers to control molecular self-assembly at various length scales and hierarchical levels for designing next-generation functional supramolecular materials with advanced functionality. With the increasing push to understand supramolecular structures in greater detail, often, the use of conventionally employed microscopy techniques such as transmission electron microscopy (TEM), atomic force microscopy (AFM), and scanning electron microscopy (SEM) proved challenging to shed light on many vital aspects of these nanostructures [1–4]. These include deconvoluting the organization complexity of multi-component systems, elucidating hierarchical structures and 3-dimensional (3D) networks, and probing real-time spatiotemporal growth, dynamics, and exchange kinetics of these supramolecular systems. In addition, lower sampling capability, invasive sample preparation procedures (e.g., drying or freezing), and the use of ionizing radiation that can damage or alter the sample itself, further limit the application of these imaging techniques for large-scale artifact-free investigation of the supramolecular structures under native conditions.
