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The reaction of the Ga+ source [Ga(PhF)2]+[Al(ORF)4]− with the neutral σ‐donor ligand dmap (4‐Me2N‐C6H4N) produces the unexpectedly large and fivefold positively charged cluster cation salt [Ga5(dmap)10]5+([Al(ORF)4]−)5. It includes a regular and planar Ga5 pentagon with strong metal–metal bonding. Additionally, the compound represents the first salt in which an ionic 1:5 packing is realized. We discuss...
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