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<p>Controllable molecular motion in chiral folded structures could realize switchable properties that facilitate the rational fabrication of smart chiroptical devices. In this work, we illustrate the crucial role of engineered chiral side arms of the rotatable axial skeletons in tuning the bulky properties as well as the fabrication of chiroptical molecular motors. Biaxial aryl skeletons implemented with pyridine are conjugated with dual chiral arms, where the <i>o, m</i> and <i>p</i>-locations affect the conformational locking by hydrogen bonds, leading to the great differences of crystallinity, color, luminescence and other physical properties in the solid and self-assembly states. In addition, <i>o</i>-chiral substitution allows for efficient folding with full chirality expression in the aryl skeleton, whereby the protonation and deprotonation caused the conformation conversion between open and closed state with chiroptical inversion. The chiral motion shows high repeatability, fidelity and reliability, with significant solvation effects ascribed to the dynamic nature of hydrogen bonds. Molecular aspects towards the chiral motion were delicately probed and depicted by a variety of spectroscopic techniques and density functional theory-based computations. This work by rational engineering the side arms, sheds lights on the explicit structure-property correlations of folded monomers and incorporates controllable motion to the responsive folding compounds with switchable chiral optics.</p>

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Engineering chiral arms in folded molecular motors

  • 期刊论文

  • 发表日期：

    2025年1月8日

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  • Yiran Xia,
  • Aiyou Hao,
  • Pengyao Xing

摘要

Controllable molecular motion in chiral folded structures could realize switchable properties that facilitate the rational fabrication of smart chiroptical devices. In this work, we illustrate the crucial role of engineered chiral side arms of the rotatable axial skeletons in tuning the bulky properties as well as the fabrication of chiroptical molecular motors. Biaxial aryl skeletons implemented with pyridine are conjugated with dual chiral arms, where the o, m and p-locations affect the conformational locking by hydrogen bonds, leading to the great differences of crystallinity, color, luminescence and other physical properties in the solid and self-assembly states. In addition, o-chiral substitution allows for efficient folding with full chirality expression in the aryl skeleton, whereby the protonation and deprotonation caused the conformation conversion between open and closed state with chiroptical inversion. The chiral motion shows high repeatability, fidelity and reliability, with significant solvation effects ascribed to the dynamic nature of hydrogen bonds. Molecular aspects towards the chiral motion were delicately probed and depicted by a variety of spectroscopic techniques and density functional theory-based computations. This work by rational engineering the side arms, sheds lights on the explicit structure-property correlations of folded monomers and incorporates controllable motion to the responsive folding compounds with switchable chiral optics.