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Ligand‐induced surface restructuring with heteroatomic doping is used to precisely modify the surface of a prototypical [Au25(SR1)18]− cluster (1) while maintaining its icosahedral Au13 core for the synthesis of a new bimetallic [Au19Cd3(SR2)18]− cluster (2). Single‐crystal X‐ray diffraction studies reveal that six bidentate Au2(SR1)3 motifs (L2) attached to the Au13 core of 1 were replaced by three...
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