Non-equilibrium hydrogel with time-dependent ultrabright fluorescence fabricated by CB-mediated thermodynamic equilibrium host-guest complexes

While biomaterials are endowed with sophisticated functions by the temporal dynamics and autonomy derived from non-equilibrium assemblies in biological systems, fabricating advanced materials counterparts with these features through kinetic control remains rare. Herein, we report a non-equilibrium hydrogel that exhibits autonomous time-dependent ultrabright fluorescence (quantum yield 0.90), achieved through the kinetically controlled incorporation of thermodynamic equilibrium host-guest complexes into a poly(2-hydroxyethyl methacrylate) (PHEMA) network. Transient complexes are programmed by coupling rapid assembly kinetics with the slow competitive binding of the polymer matrix. This kinetic mismatch converts a thermodynamic equilibrium supramolecular system into a non-equilibrium state, generating temporally dynamic fluorescence that cyclically shifts from yellow to green and self-reverts. The programmed temporal dynamics endow the hydrogel with high potential for information encryption applications.