Abstract

AbstractDNA G‐quadruplex structures were recently discovered to provide reliable scaffolding for two‐dimensional organic frameworks due to the strong hydrogen‐bonding ability of guanine. Herein, 2,7‐diaryl pyrene building blocks with high HOMO energies and large optical gaps are incorporated into G‐quadruplex organic frameworks. The adjustable substitution on the aryl groups provides an opportunity to elucidate the framework formation mechanism; molecular non‐planarity is found to be beneficial for restricting interlayer slippage, and the framework crystallinity is highest when intermolecular interaction and non‐planarity strike a fine balance. When guanine‐functionalized pyrenes are co‐crystallized with naphthalene diimide, charge‐transfer (CT) complexes are obtained. The photophysical properties of the pyrene‐only and CT frameworks are characterized by UV/Vis and steady‐state and time‐resolved photoluminescence spectroscopies, and by EPR spectroscopy for the CT complex frameworks.

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