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<p>The two-dimensional (2D) materials exhibit excellent electrical, optical, and mechanical properties. However, achieving precise control over chiral 2D materials remains a significant challenge. The present work introduces asymmetric side chain engineering to prepare the helically grooved poly(3,5-disubstituted phenylacetylene)s (PPAs), and investigates the effect of their asymmetric contour on tailoring 2D nanostructures. The post-polymerization modification of the same platform polymer was used to efficiently prepare a series of rigid helical PPAs with various lengths of alkyl side chains and the identical degrees of polymerization and distribution. Increasing asymmetry of side chains produces anisotropic hexagonal platelets with progressively high aspect ratios, while PPAs with symmetric side chains form regular 2D hexagonal sheets. Notably, the largest side chain asymmetry generates supramolecular structures with distinct chiral vortices. The computational simulations have also been performed to further elucidate the different self-assembly mechanisms of polymers. All 2D assemblies exhibit significantly enhanced circularly polarized luminescence compared to discrete polymer solutions. This work establishes side chain asymmetry as a crucial factor for programming supramolecular chirality and opens new avenues for developing advanced chiroptical materials.</p>

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Tailoring 2D assemblies from anisotropic hexagons to chiral vortices by modulating asymmetric side chains in helical poly(phenylacetylene) derivatives

  • 期刊论文

  • 发表日期：

    2026年3月24日

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  • Xin Zhou,
  • Shuming Kang,
  • Yihan Huang,
  • Xinhua Wan,
  • Jie Zhang

摘要

The two-dimensional (2D) materials exhibit excellent electrical, optical, and mechanical properties. However, achieving precise control over chiral 2D materials remains a significant challenge. The present work introduces asymmetric side chain engineering to prepare the helically grooved poly(3,5-disubstituted phenylacetylene)s (PPAs), and investigates the effect of their asymmetric contour on tailoring 2D nanostructures. The post-polymerization modification of the same platform polymer was used to efficiently prepare a series of rigid helical PPAs with various lengths of alkyl side chains and the identical degrees of polymerization and distribution. Increasing asymmetry of side chains produces anisotropic hexagonal platelets with progressively high aspect ratios, while PPAs with symmetric side chains form regular 2D hexagonal sheets. Notably, the largest side chain asymmetry generates supramolecular structures with distinct chiral vortices. The computational simulations have also been performed to further elucidate the different self-assembly mechanisms of polymers. All 2D assemblies exhibit significantly enhanced circularly polarized luminescence compared to discrete polymer solutions. This work establishes side chain asymmetry as a crucial factor for programming supramolecular chirality and opens new avenues for developing advanced chiroptical materials.