The univalent salt Ga(PhF) [Al(OR ) ] (R =OC(CF ) ) forms the strongly metal-metal bonded cluster tetracations [Ga (L) ] and [Ga (L') ] , when it reacts with innocent ligands like phenanthroline (L=phen) or t-butylisonitrile (L'= Bu-NC). Their structures and energetics are discussed as a function of the employed ligands, supported by DFT calculations and Born-Fajans-Haber cycles.

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The univalent salt Ga(PhF)2+[Al(ORF)4]− (RF=OC(CF3)3) forms the strongly metal–metal bonded cluster tetracations [GaII2(L)4]4+ and [GaI4(L′)8]4+, when it reacts with innocent ligands like phenanthroline (L=phen) or t‐butylisonitrile (L′=tBu‐NC). Their structures and energetics are discussed as a function of the employed ligands, supported by DFT calculations and Born–Fajans–Haber cycles.