A homoleptic zinc(II) helicate organized by a pair of achiral dipyrromethene ligands through zinc(II) coordination was synthesized to evaluate the chiroptical properties. This zinc complex showed strong exciton-coupled chiroptical responses from the helical configuration with a large absorption dissymmetry factor |gabs| (up to 0.20). More importantly, intense polarized luminescence in the far-red region (700–850 nm) with a fluorescence quantum yield ΦFL of 0.23 was observed for this helicate with a dissymmetry factor |glum| of 0.022, the largest value among rare-earth- and precious-metal-free small molecules. These unprecedentedly large g values were supported by theoretical calculations.
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