時間的進化を伴う光再構成型自己集合による統合型フルオロクロミックセルロースエミッター

Light-driven dissipative self-assembly has garnered substantial attention due to its precise spatiotemporal controllability. However, achieving synergistic integration of spatial manipulation fidelity, architectural programmability, and dynamic reconfigurability within a free-standing platform remains a formidable challenge. Herein, we report a light-driven hierarchical dissipative self-assembly paradigm with temporally programmable fluorochromism, achieved through molecular-engineered coordination of dynamic macrocyclic host-guest interactions within sustainable cellulose matrices. Protonated vinylpyridium-derived merocyanine is designed and synthesized to construct light-controlled differential binding architectures with cucurbiturils. This system demonstrates quantitatively reversible interconversion between spiropyran and merocyanine states through alternating photoactivation (475 nm) and thermal relaxation. Structural modulation of host-guest stoichiometry between 1:2 and 1:1 induces nanoscale morphological switching between spherical and cuboid assemblies, accompanied by time-resolved fluorescence chromism. Leveraging the inherent affinity between cucurbiturils and cellulose nanofibrils, we engineered light-fueled hierarchical architectures into freestanding cellulosic papers, exhibiting self-erasing transient photowriting and multilevel anti-counterfeiting functions. The non-covalent host-guest architecture and reprocessable cellulose matrix synergistically enable material recyclability. This spatiotemporally programmed dissipative self-assembly system pioneers sustainable cellulose platforms for adaptive optoelectronics and smart sensing.