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Light‐responsive materials enable the development of soft robots that are controlled remotely in 3D space and time without the need for cumbersome wires, onboard batteries, or altering the local environment. Azobenzene liquid crystal polymer networks are one such material that can move and deform in response to light actuation. Previous works have demonstrated azo‐based soft robotic grippers and transporters that are remotely powered by light. However, highly adaptive, automated spatiotemporal optical control over these materials has not yet been realized. Herein, a system for an azobenzene liquid crystal elastomer soft robotic arm is created by dynamically patterning light for independently maneuverable joints. The nonlinear material response to optical actuation is characterized, and the broad actuation space is explored with diverse arm configurations. A neural network is trained on the arm configurations and corresponding laser pattern to automate the pattern generation for a desired configuration. Finally, the azobenzene liquid crystal elastomer arm demonstrates complex targeted motion, marking an important step toward optically actuated soft robotics with applications ranging from optomechanics to biomedical tools. 

Time-reversal symmetry (TRS) is pivotal for materials’ optical, magnetic, topological, and transport properties. Chiral phonons, characterized by atoms rotating unidirectionally around their equilibrium positions, generate dynamic lattice structures that break TRS. Here, we report that coherent chiral phonons, driven by circularly polarized terahertz light pulses, polarize the paramagnetic spins in cerium fluoride in a manner similar to that of a quasi-static magnetic field on the order of 1 tesla. Through time-resolved Faraday rotation and Kerr ellipticity, we found that the transient magnetization is only excited by pulses resonant with phonons, proportional to the angular momentum of the phonons, and growing with magnetic susceptibility at cryogenic temperatures. The observation quantitatively agrees with our spin-phonon coupling model and may enable new routes to investigating ultrafast magnetism, energy-efficient spintronics, and nonequilibrium phases of matter with broken TRS.