Scalable Approach to Molecular Motor-Polymer Conjugates for Light-Driven Artificial Muscles

The integration of molecular machines and motors into materials represents a promising avenue for creating dynamic and functional molecular systems, with potential applications in soft robotics or reconfigurable biomaterials. However, the development of truly scalable and controllable approaches for incorporating molecular motors into polymeric matrices has remained a challenge. Here, we show that light-driven molecular motors with sensitive photo-isomerizable double bonds can be converted into initiators for Cu-mediated controlled/living radical polymerization enabling the synthesis of star-shaped motor-polymer conjugates. This approach enables scalability, precise control over molecular structure, block copolymer structures, and high end group fidelity. Moreover, we demonstrate that these materials can be crosslinked to form gels with quasi-ideal network topology, exhibiting light-triggered contraction. We investigate the influence of arm length and polymer structure, and develop the first molecular dynamics simulation framework to gain deeper insights into the contraction processes. Leveraging this scalable methodology, we showcase the creation of bilayer soft robotic devices and cargo-lifting artificial muscles, highlighting the versatility and potential applications of this advanced polymer chemistry approach. We anticipate that our integrated experimental and simulation framework will accelerate scalable approaches for active polymer materials based on molecular machines, opening up new horizons in materials science and bioscience.