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<p>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.</p>

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Time-evolving photoreconfigurable self-assembly for integrated fluorochromic cellulosic emitter

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月29日

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  • Fengfan Zhu,
  • Xiao-Fang Hou,
  • Hongyang Zhang,
  • Juping Wang,
  • Naixu Li,
  • Bo Fu,
  • Jiancheng Zhou,
  • Xu-Man Chen

摘要

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.