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<p>Precisely constructing homochiral helical nanostructures from achiral molecules by non-covalent interactions remains challenging owing to the untraceable handedness control at different hierarchical levels. Here, we present an aurophilicity-assisted orthogonal assembly strategy, enabling not only the homochiral assembly of an achiral carbene-anchored trinuclear gold cluster with chiral amines but also the inversion of circularly polarized luminescence (CPL). This gold cluster could spontaneously form random right- or left-handed helices, while introduction of chiral amines effectively drives the formation of hierarchically homochiral twists with |<i>g</i><sub>lum</sub>| of 10<sup>−2</sup>, directed by inherent aurophilicity of gold cluster and orthogonal intermolecular C-H⋅⋅⋅O/N interactions. Furthermore, by fine-tuning the assembly conditions from DMF to DMF/H<sub>2</sub>O solvent, the morphology of assemblies can be specifically controlled, resulting in inversion of CPL signals. This study highlights the potential of aurophilicity-driven orthogonal assembly strategy in effectively controlling hierarchical chirality and paves the way for advancing chiral metallo-superstructures.</p>

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Solvent-mediated chirality inversion in orthogonal hierarchical assembly of achiral carbene-anchored gold cluster

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年11月26日

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  • Ying-Jie Liu,
  • Wen-Qiu Yu,
  • Yu Liu,
  • Xiao-Wen Qi,
  • Shuang-Quan Zang

摘要

Precisely constructing homochiral helical nanostructures from achiral molecules by non-covalent interactions remains challenging owing to the untraceable handedness control at different hierarchical levels. Here, we present an aurophilicity-assisted orthogonal assembly strategy, enabling not only the homochiral assembly of an achiral carbene-anchored trinuclear gold cluster with chiral amines but also the inversion of circularly polarized luminescence (CPL). This gold cluster could spontaneously form random right- or left-handed helices, while introduction of chiral amines effectively drives the formation of hierarchically homochiral twists with |glum| of 10−2, directed by inherent aurophilicity of gold cluster and orthogonal intermolecular C-H⋅⋅⋅O/N interactions. Furthermore, by fine-tuning the assembly conditions from DMF to DMF/H2O solvent, the morphology of assemblies can be specifically controlled, resulting in inversion of CPL signals. This study highlights the potential of aurophilicity-driven orthogonal assembly strategy in effectively controlling hierarchical chirality and paves the way for advancing chiral metallo-superstructures.