Fully Room-Temperature Reprogrammable, Reprocessable, and Photomobile Soft Actuators from a High-Molecular-Weight Main-Chain Azobenzene Crystalline Poly(ester-amide)

Azobenzene (azo) polymer photoactuators with full room-temperature reprogrammability, reprocessability, and photo-mobility are highly desirable for large-scale applications, but their development remains a daunting challenge. Herein, a strategy is first presented for fabricating such advanced photoactuators from a high-molecular-weight main-chain azo crystalline poly(ester-amide) (PEA) prepared via Michael addition polymerization. This azo PEA can be readily processed into both physically cross-linked, uniaxially oriented fibers and films with high mechanical robustness and reversible photoinduced bending/unbending at room temperature. Importantly, the presence of both amide unit-induced hydrogen bonding and crystalline domains in such films and fibers endows them with dynamic, yet stable cross-linking points, which enable their easy reprogrammability under strain at room temperature into various three-dimensional (3D) shapes (e.g., film helicoid and spiral ribbon, fiber spring) capable of showing completely different shapedependent photomobile modes. In particular, these reshaped photoactuators can maintain their accurate 3D shapes and highly reversible photoinduced motions even after being kept at 80 degrees C for 20 days or at 100 degrees C for 2 days. They can also be reprocessed and recycled from solution at room temperature. Such a multifunctional main-chain azo crystalline PEA can serve as a versatile platform for fabricating various photoactuators with desired 3D shapes and motion modes under mild ambient conditions.