Supramolecular rosette intermediated homochiral double helix

Tiejun Li, Dian Niu, Lukang Ji, Qian Li, Bo Guan, Hanxiao Wang, Guanghui Ouyang () and Minghua Liu ()
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Tiejun Li: Chinese Academy of Sciences
Dian Niu: Chinese Academy of Sciences
Lukang Ji: Chinese Academy of Sciences
Qian Li: Chinese Academy of Sciences
Bo Guan: Chinese Academy of Sciences
Hanxiao Wang: Chinese Academy of Sciences
Guanghui Ouyang: Chinese Academy of Sciences
Minghua Liu: Chinese Academy of Sciences

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract Precise organization of organic molecules into homochiral double-helix remains a challenge due to the difficulty in controlling both self-assembly process and chirality transfer across length scales. Here, we report that a type of bisnaphthalene bisurea molecule could assemble into chirality-controlled nanoscale double-helices by a supramolecular rosette-intermediated hierarchical self-assembly mechanism. A solvent-mixing self-assembly protocol is adopted to direct bisnaphthalene bisurea cyclization into chiral discrete rosettes through cooperative intramolecular and intermolecular hydrogen bonds. Controlled hexagonal packing of rosettes at higher concentrations gives one-dimensional single-stranded nanofibers, which intertwine into well-defined double-helix nanostructures with preferred chirality that depends on the absolute configurations of bisnaphthalene bisurea. The hierarchical organization of bisnaphthalene bisurea molecules enables effective excitation energy delocalization within the double-helix, which contributes to near-unity energy transfer from double-helix to adsorbed acceptor dyes even in donor/acceptor ratios over 1000, leading to bright circularly polarized luminescence from the originally achiral acceptor. The experimental and theoretical simulation results not only provide a hierarchical strategy to fabricate homochiral double-helix but also bring insights in understanding the high-efficiency light-harvesting process in photosystem II.

Date: 2025
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DOI: 10.1038/s41467-025-57059-3

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