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Abstract Helicenes represent a class of fascinating π compounds with fused yet folded backbones. Despite their broad structural diversity, harnessing helicenes to develop well‐defined materials is still a formidable challenge. Here we report the synthesis of crystalline porous helicene materials by exploring helicenes to synthesize covalent 2D lattices and layered π frameworks. Topology‐directed polymerization of 6helicenes and porphyrin creates 2D covalent networks with alternate helicene‐porphyrin alignment along the x and y directions at a 1.5‐nm interval and develops 6helicene frameworks through reversed anti‐AA stack along the z direction to form segregated 6helicene and porphyrin columnar π arrays. Notably, this π configuration enables the frameworks to be highly red luminescent with benchmark quantum yields. The 6helicene frameworks trigger effieicnt intra‐framework singlet‐to‐singlet state energy transfer from 6helicene to porphyrin and facilitate intermolecular triplet‐to‐triplet state energy transfer from frameworks to molecular oxygen to produce reactive oxygen species, harvesting a wide range of photons from ultraviolet to near‐infrared regions for light emitting and photo‐to‐chemical conversion. This study introduces a new family of extended frameworks, laying the groundwork for exploring well‐defined helicene materials with unprecedented structures and functions.
Yin et al. (Thu,) studied this question.