A Quadri‐Dimensional Manipulable Laser with an Intrinsic Chiral Photoswitch

Abstract Dynamic and multi‐dimensional manipulation of laser emission with light allows for optical coding, computing, and imaging photonic chips. However, the coupling balance between photonic resonance and transmission is a formidable challenge due to the uncontrollable chiral microcavity with photo‐reversibility, which is limited to the multi‐freedom of the laser with sustainable and repeatable output beams. Herein, a helical superstructure system with a unique intrinsic chiral photoswitch is developed for resolving the always pendent problems on organized defects in the microcavity. The unique intrinsic chirality based on the photoswitchable system allows laser emission with a sharp and narrow band‐width, with both remarkable thermodynamic stability and robust fatigue‐resistance. A quadri‐dimensional manipulable laser, featuring wavelength‐tunability, wavefront‐shaping, spin angular momentum (SAM), and orbital angular momentum (OAM), is successfully established with the assistance of the photoresponsive intrinsic chiral superstructure with photoreversibility. This technology marks an important milestone, and sketches a future framework for the realms of nanophotonic information encoding, security imprinting, and integrated photonics.