In this and the next section we analyze the behavior of TDHF electron dynamics when the electron occupation is close to that expected for the S 1 state. In order to drive the system away from the initial S 0 reference state the molecules considered were again perturbed with fields using the linear response resonant frequencies. Field-strengths and durations were chosen by picking trajectories from the set used to plot Fig. that, when the field was removed, had average HOMO and LUMO occupations close to one for a "clean" S 0 → S 1 transition (HOMO→LUMO transition being the major contributor to the S 1 state, cf. Table ). Then the field-parameters corresponding to the most stationary evolution (constant MO occupation(s) with time) were chosen to induce the transition. In Fig. we show the TDHF MO occupations with the chosen field parameters. For the three molecules, the final occupation is close to one electron in the HOMO and one electron in the LUMO, as expected for the S 1 state (see figure for the corresponding TD-CIS MO occupation and S 1 state population plot). We next analyze the degree of charge transfer during this population change by monitoring the timedependent dipole moment for each molecule. Based on the stationary state characterization in Table , we expect the dipole moment to increase as the population is driven from S 0 to S 1 , with the change in dipole moment increasing with increasing system size. This is indeed what we see with both TDCIS and TDHF methods, as shown in Fig. . For all systems, the initial dipole moment is identical for both methods as both TDCIS and RT-TDHF have the same initial HF ground state. The stationary state S 1 dipoles are shown with dashed lines, and we see that the TDCIS time-dependent dipole moment approaches this value and remains centered around the S 1 dipole moment. There is very little oscillation for System 1 and System 2, and a small amount of oscillation for System 3.