Abstract
AbstractThe energetics, structures, stabilities and reactivities of[CnH2]2+ ions have been investigated using computational methods and experimental mass spectrometric techniques. Spontaneous decompositions of [CnH2]2+ into [CnH]+ + H+ products, observed for ions with odd‐n values, have been explained by invoking the formation of excited triplet states. Even‐n [CnH]+ ions possess triplet ground states with low‐lying excited states, whereas odd‐n ions have triplet states with energies several eV above ground singlet states. Radiationless transitions of vibrationally excited long‐lived triplet state ions into singlet state continua are suggested as possible mechanisms for spontaneous deprotonation processes of odd‐n [CnH2]2+ ions. Evidence for these long‐lived excited states has been obtained in bimolecular single electron transfer reactions.
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