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<p>The exceptional efficiency of natural light-harvesting systems arises from their precisely organized supramolecular architectures. Reproducing such structural control in synthetic aqueous assemblies, particularly over size and dimensionality, remains a formidable challenge. Here, we report a general seeded-growth strategy that enables precise, hierarchical assembly of two-dimensional (2D) porphyrin heterostructures in water. Integrating π–π stacking, hydrogen bonding, and hydrophobic interactions, the porphyrin amphiphiles follow a metastable assembly pathway that yields kinetically controlled nanosheets or heterostructures. This approach provides unprecedented control over the nanostructure area across two orders of magnitude, establishing a versatile platform for complex functional architectures. By integrating a cobalt–porphyrin acceptor via block co-assembly, we construct 2D donor–acceptor heterostructures that achieve a directed energy funneling. Ultrafast spectroscopic analysis combined with global fitting reveals the mechanism: the controlled 2D heterostructures promote exciton migration at rates 2.5-fold greater than in homostructures and drive the formation of a fully charge-separated state on a sub-nanosecond timescale, with dynamics that scale with platelet dimensions. This work establishes a synthetic route to biomimetic 2D heterostructures and elucidates the structural determinants of directed exciton and charge flow, offering key design principles for advanced biomimetic systems.</p>

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Controlled assembly of two-dimensional porphyrin heterostructures toward directed energy transfer and charge separation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年6月19日

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  • Yifei Lei,
  • Jiangshan Zhang,
  • Yifei Han,
  • Shixing Lei,
  • Song-Hai Xie,
  • Shu Wang,
  • Zhiyuan Huang,
  • Dan-Wei Zhang,
  • Zhan-Ting Li,
  • Li-Zhu Wu,
  • Chen-Ho Tung,
  • Jia Tian

摘要

The exceptional efficiency of natural light-harvesting systems arises from their precisely organized supramolecular architectures. Reproducing such structural control in synthetic aqueous assemblies, particularly over size and dimensionality, remains a formidable challenge. Here, we report a general seeded-growth strategy that enables precise, hierarchical assembly of two-dimensional (2D) porphyrin heterostructures in water. Integrating π–π stacking, hydrogen bonding, and hydrophobic interactions, the porphyrin amphiphiles follow a metastable assembly pathway that yields kinetically controlled nanosheets or heterostructures. This approach provides unprecedented control over the nanostructure area across two orders of magnitude, establishing a versatile platform for complex functional architectures. By integrating a cobalt–porphyrin acceptor via block co-assembly, we construct 2D donor–acceptor heterostructures that achieve a directed energy funneling. Ultrafast spectroscopic analysis combined with global fitting reveals the mechanism: the controlled 2D heterostructures promote exciton migration at rates 2.5-fold greater than in homostructures and drive the formation of a fully charge-separated state on a sub-nanosecond timescale, with dynamics that scale with platelet dimensions. This work establishes a synthetic route to biomimetic 2D heterostructures and elucidates the structural determinants of directed exciton and charge flow, offering key design principles for advanced biomimetic systems.