Here, the diagonal elements of ρ (i.e., ρ ii (t)) are chosen based on the active state |Φ α (r, R(t)) . Along a specific trajectory, R(t), the instantaneous population at time t is considered as 1 for the active state |Φ α (r, R(t)) , and 0 for all other states. The off-diagonal elements are computed based on the wavefunction expansion coefficients, a j (t). Apart from the above adiabatic populations, we also need the timedependent diabatic/charge populations, on each moiety of the entire system, to characterize the photo-induced charge transfer dynamics. The charge population on a specific fragment is obtained by projecting the adiabatic reduced density matrix onto the AO basis associated with that molecular fragment, N , as: