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The synthesis and structure of atomically precise Au130−xAgx (average x=98) alloy nanoclusters protected by 55 ligands of 4‐tert‐butylbenzenethiolate are reported. This large alloy structure has a decahedral M54 (M=Au/Ag) core. The Au atoms are localized in the truncated Marks decahedron. In the core, a drum of Ag‐rich sites is found, which is enclosed by a Marks decahedral cage of Au‐rich sites....
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