Unlike S 0 →S 1 and S 0 →T 1 excitations, more pairs of MO transitions got involved in T 2 and T 3 states. For S 0 →T 2 excitation, HOMO-3→LUMO and HOMO-4→LUMO+1 contribute 74.0% and 11.3%, respectively. Consequently, T 2 state has the partial character of (n, π * ) referring the MO plots in Fig. of SI. Two pairs of NTOs contribute near equally to T 2 excitation, depicted in Fig. as panels (c) and (d). For S 0 →T 3 , on the other hand, HOMO→LUMO+1 makes a major contribution, accounted for 55.1%, followed by HOMO-4→LUMO of 14.8%. As shown in panels (c) and (d) of Fig. in SI, the relaxed density difference plots of T 2 -S 0 and T 3 -S 0 have local excitation character, which are different from those of S 1 -S 0 and T 1 -S 0 . As a result, the SOCMEs between S 1 and T 2 and between S 1 and T 3 should be larger than that between S 1 and T 1 , verified by the calculated values shown in Table .