Dynamic Chiral Folding for Arene–Perfluoroarene Force Driven Clamping

Peptide folding provides a feasible protocol to design intelligent chiral supramolecular systems toward sensing, recognition, and many other advanced functions. Here we conjugated dual short peptide arms on the aromatic core in a spatially close manner, allowing for intramolecular folding. Through controlling the aromatic core skeleton and appended luminophores, efficient chirality transfer to terminal pyrenes was realized. The through-space transferred chirality exhibited ultrahigh sensitivity toward solvent environments. Micropockets within dipeptides would accommodate the solvents specifically to initiate the chiroptical inversion expressed in the ground-state circular dichroism and the circularly polarized luminescence at photoexcited states. The dynamics also were depicted on the selective binding of guests through arene-perfluoroarene interactions. We successfully constructed a dynamic peptide-based clamp that could control the <i>endo</i>- and <i>exo</i>-type arene-perfluoroarene complexation. This work inspires the design and fabrication of peptide-based chiroptical materials with adaptability to external fields.