Before comparing the S3 lifetimes of the two molecules, we should consider the short time constant (11 fs; Table ) we observed in 7-AIH + simulations. As explained, this time constant is associated with dissociative trajectories. This dissociation process results from the initial conditions sampling, which contains energy excess well above the 0-0 excitation (see SI-1). Thus, when comparing theory to the experiments, we should only consider the long S3 lifetime predicted for 7-AIH + . If we bear these considerations in mind, the dynamics simulations predict a shorter S3 lifetime for 6-AIH + (156 fs) than for 7-AIH + (278 fs). The value for 7-AIH + agrees well with the experimental measurement (~230 fs). The one for 6-AIH + , however, is considerably longer than the experimental S3 lifetime, ~25 fs.