Photo‐Controllable Förster Resonance Energy Transfer Based on Dynamic Chiral Self‐Assembly of Sequence‐Defined Amphiphilic Alternating Azopeptoids

Abstract Endowing biomimetic sequence–controlled polymers with chiral functionality to construct stimuli‐responsive chiral materials offers a promising approach for innovative chiroptical switch, but it remains challenging. Herein, it is reported that the self‐assembly of sequence‐defined chiral amphiphilic alternating azopeptoids to generate photo‐responsive and ultrathin bilayer peptoidosomes with a vesicular thickness of ≈1.50 nm and a diameter of around ≈290 nm. The photoisomerization of azobenzene moiety facilitates a reversible structural transformation from isotropic peptoidosomes to anisotropic 1D helical nanoribbons (≈80 nm width) under the alternating irradiation with UV and visible lights, consequently leading to the chirality expression and transfer from chiral asymmetric center to achiral azobenzene units. As a biomimetic model with deformation‐induced energy transfer, a non‐invasive azobenzene‐based Förster resonance energy transfer system is unprecedentedly constructed via the introduction of a fluorescent donor of pyrene derivatives and sequentially photo‐regulated the donor/acceptor ratio, displaying a reversible gradient fluorescent color variation from blue to yellow (a broad Stokes shift of ≈200 nm) and a high‐efficient energy transfer efficiency of 97.2%. The photo‐controllable photoluminescence phenomenon endows these chiral aggregates with a proof‐of‐concept application on multi‐colored information encryption. This work provides a prospective strategy to fabricate stimuli‐responsive chiral biomimetic materials with a potential on the light‐controllable switches.