The nonadiabatic dynamics simulations were performed using Tully's surface hopping (SH) approach with energy-based decoherence correction as implemented in the MNDO program. The electronic structure of the cations was described with the ROOM3/CISD(x × y) method. For Ada-CN + , two sets of SH simulations were considered, corresponding to excitation of two lowest energy bands recently observed experimentally by Crandall et al. . For Ama + , for which no experimental optical spectrum is available (to the best of our knowledge), excitation to the lowest energy band was considered. Each set of SH simulations includes 1000 trajectories. The initial geometries and nuclear velocities for the SH trajectories were sampled using the Wigner function at T = 0 K. The Wigner function was obtained under harmonic approximation following optimization and normal mode analysis (for the D 0 state) at the ROOM3/CISD(x × y) level. The initial electronic state for a given trajectory was chosen as the brightest state (i.e., the state with the largest oscillator strength) in a given excitation energy window. For Ama + , the energy window eV was considered; and for Ada-CN + , energy windows eV and eV were investigated. These choices are based on absorption spectra calculated at the initial geometries selected by Wigner sampling, as an alternative approach to the (harmonic) quantum approach using the VG approximation. These spectra were calculated as