Room Temperature Phosphorescence Polymer Ionogel with Nucleation‐Induced Dynamic Reversible Behavior

Abstract Room temperature phosphorescence (RTP) materials with mechanical and dynamic reversible properties are essential for intelligent flexible optoelectronic materials. However, development of these materials is often hampered by a trade‐off between the flexibility demanded by mechanical and dynamic properties, as well as the rigidity required by RTP. Herein, a strategy is developed to construct a series of RTP polymer ionogels (PIs) with dynamic reversible behavior by photo‐polymerizing rigid monomers and luminescent monomer in supercooled ionic liquid (IL). PIs exhibit exceptional mechanical duality, reflecting in the changeable stiffness, which facilitates achieving dynamic reversible RTP. Moreover, mechanical duality also enables PIs to reversibly transform between two states and accompany with tremendous variations in transparency, tensile property, adhesion, and conductivity, which can be visualized by RTP. The RTP‐indicated dynamic reversible behavior in PIs emerges from the flowing supercooled IL within the polymer network in gel‐state, and the ordered stacking crystal IL in crystal‐state. PIs are successfully implemented in crystallization area monitoring, tailored adhesion, circuit indication, information storage, and fingerprint acquisition. This work will provide a perspective for constructing RTP with dynamic reversible behavior and multifunctional luminescent materials.