Phosphorescence-Plastic Hydrogel Driven by Frustrated Phase Separation

Achieving dynamic control of phosphorescence in polymer materials remains challenging due to the inherent conflict between the rigid matrix required to stabilize long-lived triplet excitons and the network plasticity necessary for dynamic editing. Herein, we report a neuromorphic phosphorescence-plastic hydrogel based on a poly(acrylamide-co-acrylonitrile) network whose luminescence can be spatially and temporally reconfigured through a frustrated phase separation mechanism. Under mild thermal training, the system undergoes a reversible phase transition, forming cyano-rich clusters in polymer-dense regions as intrinsic phosphorescent centers. The phase-separated structure expels water from between chains, promoting aggregation and suppressing nonradiative transitions, thereby promoting phosphorescence emission. This process enables the creation of fully rewritable phosphorescent patterns featuring a tunable afterglow duration of up to 5.0 s, repeatable erasure, and excellent water stability. The emission intensity and duration can be precisely regulated by varying the thermal input time, emulating memory consolidation and loss behaviors observed in neural systems. We further demonstrate applications in multilevel information encryption and dynamic displays. This work provides a polymer physics strategy for designing editable phosphorescent materials via controlled nonequilibrium network states, offering a pathway to bridge neuromorphic functions with soft matter photonics.