For our single LSC trajectory depicted in Figure , we found the charge transfer to occur from the S 4 state to the S 1 state within 25 fs. Figure shows the excited state and ground state density difference plots at different times during the trajectory, where we weight the density difference according to the occupation of the excited state, shown in Figure . For example, at t=1.5 fs where a crossing between the S 4 and S 3 surfaces occurred, the population is predominantly on the S 3 surface and so the density difference shown is primarily between S 3 and S 0 . Similarly, at the end of the trajectory, the population is mostly in the S 1 state, and the density difference shown is mostly that for S 1 and S 0 . At t=16 fs shortly after the S 4 and S 3 avoided surface crossing, this state has mixed locally excited and charge transfer character, and the occupation is shared between S 4 and S 3 . Figure shows the TDDFT energies of the four lowest lying excited states, colored according to the occupation during the trajectory. Surface crossings and avoided surface crossings occur throughout the trajectory, with state mixings often leading to population transfer between states, notably at t ≈ 14 fs, t ≈ 17 fs, and t ≈ 21 fs. Note that these LSC NAMD dynamics are for a single trajectory, and an ensemble of LSC NAMD trajectories would be required to compute the LSC correlation function.