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Disentangling the isomeric structure of C 7 H 7  +  is a longstanding experimental issue. We report here the full mid‐infrared vibrational spectrum of C 7 H 7  +  tagged with Ne obtained with infrared‐predissociation spectroscopy at 10 K. Saturation depletion measurements were used to assign the contribution of benzylium and tropylium isomers and demonstrate that no other isomer is involved. Recorded spectral features compare well with density functional theory calculations. This opens perspectives for a better understanding and control of the formation paths leading to either tropylium or benzylium ions.

Direct Evidence of the Benzylium and Tropylium Cations as the Two Long‐Lived Isomers of C 7 H 7 +