Transition-metal luminescent polynuclear assemblies have seen significant research in the last 25 years owing to their potential application as molecular sensors, probes, and in other optoelectronic devices. Among the most studied metals are Re(I), Ru(II), Os(II), Pt(II), Pd(II) assemblies. Iridium, despite robust photoactive properties with vast applications in optoelectronics as molecular phosphors in organic light emitting diodes (OLEDs) and in light emitting electrochemical cells (LEECs), has seen comparatively few results in the areas of supramolecular photochemistry. Iridium has undergone little development in the field of supramolecular complexes owing to its substitutional inertness, making rapid and facile synthesis of such architectures difficult. To overcome substitutional barriers, a coordination-driven self-assembly approach using isocyanides was developed. A range of 2D and 3D cyclometalated iridium architectures were produced via the use of a new class of flexible or geometrically constrained σ-donating polydentate isocyanide bridging ligands. The synthetic chemistry and photophysical properties of the supramolecular structures are described, with the phosphorescence originating either from an excited state localized on the cyclometalated iridium nodes or on the conjugated isocyanide bridging ligand. These constructs should provide new avenues to facile synthesis of iridium-based supramolecular architectures which can be studied for a more holistic understanding of electronic communication in photoactive supramolecular compounds.

Coordination driven self-assembly of Ir (III) coordination cages using π-conjugated polydentate isocyanides

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ACS Fall 2022

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