Fig. 4.

Ab initio non-adiabatic molecular dynamics simulations. a Time evolution of electronic populations starting from the initially excited S_b state, where the charge carriers are localized in the PDI moieties. b Time evolution of electronic populations starting from the hole-transferred state (S_d), describing the dynamics of charge carriers after PDI-to-porphyrin hole transfer. c Evolution of electron-hole distribution starting from the initially excited S_b state, visualized with the Kohn–Sham (KS) orbitals of COFs. In each of HOMO and LUMO, the densities of holes (orange) and electrons (blue) are depicted. All possible electron-hole pairs in the active space are listed in Supplementary Table 2. d Evolution of electron-hole distribution starting from the hole-transferred state S_d. In each of HOMO and LUMO, the densities of holes (orange) and electrons (blue) are depicted