biostudies-literatureLiu YJNatural Science Foundation of Henan Province (Henan Province Natural Science Foundation)China Postdoctoral Science FoundationNational Natural Science Foundation of China (National Science Foundation of China)10586https://www.ebi.ac.uk/biostudies/studies/S-EPMC12657935biostudies-literatureUnknown16(1)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 |g_lum| of 10^-2, directed by inherent aurophilicity of gold cluster and orthogonal intermolecular C-H⋅⋅⋅O/N interactions. FurNature communicationsSolvent-mediated chirality inversion in orthogonal hierarchical assembly of achiral carbene-anchored gold cluster.PMC126579352523004211742210517792461304923563042021TQ0294Liu YQi XWLiu YJYu WQZang SQfalseSolvent-mediated chirality inversion in orthogonal hierarchical assembly of achiral carbene-anchored gold cluster.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 |g_lum| of 10^-2, directed by inherent aurophilicity of gold cluster and orthogonal intermolecular C-H⋅⋅⋅O/N interactions. Fur2025-01-01T00:00:00Z2025 Nov2026-06-05T21:22:23.358Z2026-05-22T03:09:02.356ZS-EPMC126579354129844110.1038/s41467-025-65637-8