Ultrafast capture of electrons ejected by photoionization leading to the formation of a charge-separated state at a high energy level

state of pyrene by 0.53 eV. In addition, the subsequent ionic dissociation without a remarkable geminate recombination in the sub-nanosecond to nanosecond time region effectively avoids the quantity loss of the CS state. By applying the two-photon excitation method, we experimentally achieved ultrafast formation of the long-lived CS state at a high energy beyond the traditional framework of electron transfer reactions.