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The idea of using individual molecules as conducting wires, regulators, and interconnects for charges in electronic circuitry has catalyzed the vibrant development of the field of single-molecule electronics. The ability to reliably and repeatedly construct single-molecule junctions (SMJs) has enabled the study of charge transport through a broad spectrum of individual molecules. Over the past decade, the capability of the SMJ platform has been greatly expanded thanks to the development of new experimental techniques and the integration of knowledge and methodologies from other disciplines. New opportunities beyond electrical conductance have emerged at the atomic and molecular scale. It has been demonstrated in many recent studies that the SMJ can now serve as a powerful and versatile tool to address critical physical and chemical questions that are otherwise inaccessible. This perspective focuses on the new capabilities and functionalities of the SMJ beyond conductance measurements and how they have enabled the investigation of crucial single-molecule processes and advanced our understanding beyond molecular electronics. 

Supramolecular nanocages with inner cavities have attracted increasing attention due to their fascinating molecular aesthetics and vast number of potential applications. Even though a wide array of discrete supramolecular cages with precisely designed sizes and shapes have been established, the controlled assembly of higher-order supramolecular frameworks from discrete molecular entities still represents a formidable challenge. In this work, a novel metallo-organic cage [Zn12L4] was assembled based on a triphenylene-cored hexapod terpyridine ligand. Synchotron X-ray analysis revealed a pair of enantiomeric cages in the crystal with flexible ligands twisted clockwise or anticlockwise due to steric hindrance in the structure. Interestingly, due to the strong π–π intermolecular interaction between triphenylene units, a controlled hierarchical packing of sphere-like cages in the crystal was established having a sparse packing mode with huge channels of around 3.6 nm diameter. This research sheds light on the design of strong π–π interactions in supramolecular hierarchical packing and materials science.