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<p>The complex dynamics of synthetic supramolecular systems in living cellular environments impede the correlation between the transient hierarchical species and their biological functions. Achieving this correlation demands a breakthrough that combines the precise control of supramolecular events at discrete time points via synthetic chemistry with their real-time visualization in native cells. In the present study, we reported two peptide sequences that undergo visible light-induced molecular and supramolecular transformations to form various assembly species in cells. In contrast to endogenous stimulus-responsive assembly, the proposed photochemistry enables full control over the photolysis reaction where the monomer generation and local concentration regulate the subsequent assembly kinetics. Phasor-fluorescence lifetime imaging traced the formation of various assembly states in cells associated with monomer activation and consumption, whereas correlative light-electron microscopy revealed the intracellular nanofibres formed. The temporally resolved assembly process shows that the emergence of cytotoxicity correlates with the accumulation of oligomers beyond the cellular efflux threshold.</p><p></p>

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Intracellular assembly of supramolecular peptide nanostructures controlled by visible light

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年3月12日

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  • Yong Ren,
  • Zhixuan Zhou,
  • Iain Harley,
  • Özlem Aydin,
  • Leon Driehaus-Ortiz,
  • Anke Kaltbeitzel,
  • Jiaqi Xing,
  • Konrad Maxeiner,
  • Ingo Lieberwirth,
  • Katharina Landfester,
  • David Y. W. Ng,
  • Tanja Weil

摘要

The complex dynamics of synthetic supramolecular systems in living cellular environments impede the correlation between the transient hierarchical species and their biological functions. Achieving this correlation demands a breakthrough that combines the precise control of supramolecular events at discrete time points via synthetic chemistry with their real-time visualization in native cells. In the present study, we reported two peptide sequences that undergo visible light-induced molecular and supramolecular transformations to form various assembly species in cells. In contrast to endogenous stimulus-responsive assembly, the proposed photochemistry enables full control over the photolysis reaction where the monomer generation and local concentration regulate the subsequent assembly kinetics. Phasor-fluorescence lifetime imaging traced the formation of various assembly states in cells associated with monomer activation and consumption, whereas correlative light-electron microscopy revealed the intracellular nanofibres formed. The temporally resolved assembly process shows that the emergence of cytotoxicity correlates with the accumulation of oligomers beyond the cellular efflux threshold.