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One‐ and two‐electron oxidation of a digallene stabilized by an N‐heterocyclic carbene afforded the first stable gallium‐based radical cation and dication salts, respectively. Structural analysis and theoretical calculations reveal that the oxidation occurs at the Ga=Ga double bond, leading to removal of π electrons of the double bond and a decrease of the bond order. The spin density of the radical...
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